MATERIAL CHARACTERIZATIONS OF MWCNT/NZF BASED

POLYMER NANOCOMPOSITES FOR RADAR ABSORBING

STRUCTURES

A thesis submitted in partial fulfilment of the requirement

for the award of the degree of

DOCTOR OF PHILOSOPHY
in
MECHANICAL ENGINEERING

By
PUPPALA SIVA NAGASREE

Under the guidance of

Dr. KOONA RAMJI
Professor, Dept. of Mechanical Engineering
A.U College of Engineering (A), Andhra University &
Former Vice-Chancellor, Dr. B.R. Ambedkar University, Srikakulam

DEPARTMENT OF MECHANICAL ENGINEERING

ANDHRA UNIVERSITY COLLEGE OF ENGINEERING (A)
ANDHRA UNIVERSITY, VISAKHAPATNAM – 530003,
ANDHRAPRADESH, INDIA
2022

i
 DEPARTMENT OF MECHANICAL ENGINEERING

AU COLLEGE OF ENGINEERING (Autonomous)

ANDHRA UNIVERSITY

CANDIDATE’S DECLARATION

I hereby declare that the work described in this thesis, entitled “MATERIAL

CHARACTERIZATIONS OF MWCNT/NZF BASED POLYMER

NANOCOMPOSITES FOR RADAR ABSORBING STRUCTURES ” which is

being submitted in partial fulfilment for the award of Doctor of Philosophy (Ph.D.) in

Dept. of Mechanical Engineering to the Andhra University College of Engineering, is

an authentic record of my own work carried out under the guidance of Dr.K.Ramji of

Department of Mechanical Engineering, AU College of Engineering (A), Andhra

University. The work is original and has not been submitted by me for any Degree to

this university or any other university.

(P. Siva Nagasree)

ii
 DEPARTMENT OF MECHANICAL ENGINEERING

AU COLLEGE OF ENGINEERING (Autonomous)

ANDHRA UNIVERSITY

CERTIFICATE

This is to certify that the thesis entitled “MATERIAL CHARACTERIZATIONS OF

MWCNT/NZF BASED POLYMER NANOCOMPOSITES FOR RADAR

ABSORBING STRUCTURES “that is being submitted by Smt. PUPPALA SIVA

NAGASREE in partial fulfilment for the award of Doctor of Philosophy (Ph.D.) in

Mechanical Engineering to the Andhra University, Visakhapatnam is a record of

bonafide work carried out by her under my guidance and supervision.

The results embodied in this thesis have not been submitted to any other

University or Institute for the award of any degree or diploma.

Signature of GUIDE

Dr.Koona Ramji
Professor
Department of Mechanical Engineering
AUCE (A)
VISHAKHAPATNAM

iii
 ABSTRACT

In the 21st century, microwave absorbers present a wide range of applications

such as anechoic chambers, electromagnetic interference (EMI) shielding materials in

radar and wireless communications. The development of novel microwave absorbing

materials is vital to avoid the harmful effects of electromagnetic (EM) radiation and for

stealth technology applications. Researchers worldwide have been devoting their best

efforts to synthesize materials that strongly absorb electromagnetic radiation in a wide

frequency range. In particular, many studies focus on the X-band region because most

radar and telecommunication applications are associated with this band. The main

objectives of the microwave absorbers are strong microwave absorption, broad

bandwidth, low weight and fine thickness. The load bearing capabilities establish the

service life of radar absorbing materials in any practical or real world application. So,

the present work aims to develop radar absorbing materials with adequate strength and

thermal stability using both material based and geometry based techniques to achieve

the above mentioned objectives.

In order to prepare the radar absorbing materials (RAMs), multiwalled carbon

nanotubes (MWCNT), nickel zinc ferrite (NZF) nano powder and the combination of

MWCNT and NZF with different aspect ratios of MWCNT are used as lossy fillers in

the E-glass fiber reinforced epoxy composites. The multi-layered and geometrically

arrayed structures are designed using these materials and analyzed to obtain their

microwave absorption properties. Initially, the nanocrystalline Ni0.5Zn0.5Fe2O4 was

synthesized by a facile and effective sol–gel auto combustion technique to prepare

magnetic RAMs. The microstructural and magnetic properties of synthesized ferrite

were determined by various characterization techniques like FESEM, TEM, XRD,

FTIR and VSM. The E-glass/epoxy-based nanocomposites with different weight

iv
percentages of MWCNT, nickel zinc ferrite and the combination of MWCNT and

nickel zinc ferrite were fabricated by in-situ polymerization. Further, electromagnetic

properties were investigated to elucidate the possible absorption mechanism of the

fabricated composites. The fabricated RAM’s thermal stability was determined using

TGA analysis.

The reflection loss of multi layered RAMs are determined according to the

transmission line theory using MATLAB for thirty six different cases. Multi Criteria

Decision Making (MCDM) methods TOPSIS, VIKOR and PROMETHEE-II, are

implemented to select one RAM from the five better performing alternative multi-

layered RAMs. The mechanical properties including tensile strength, flexural strength,

impact strength and hardness of the selected RAM were obtained according to the

ASTM standards. Microwave absorption of geometry based RAS composed of

MWCNT and NZF is analysed for different arrayed geometries using COMSOL

Multiphysics software.

The microwave absorbers are fabricated using successfully synthesized NZF by

the sol-gel method and MWCNT. The raw materials and RAMs purity, microstructure

analysis was done using different characterization techniques. The SEM results

revealed that the particle size of synthesized NZF is 26 nm, consistent with XRD and

TEM results. The TGA results indicated that, all the composites are thermally stable up

to 3000C. The electromagnetic properties of dielectric and hybrid RAM are increased

with an increase in weight percentage of fillers, whereas for magnetic RAM these

properties are increased up to 20 wt% of NZF and decreased further. From the results

of multilayer magnetic RAM, it is observed that double layered magnetic radar

absorbing material NRAS 5 exhibited reflection loss (RL) −10 dB for a bandwidth of

2.4 GHz and a maximum RL of −33 dB at 9.6 GHz. In dielectric RAMs composed of

v
MWCNT, MRAS 8 double layered structure exhibited an RL of -15 dB for 2 GHz

bandwidth and -10 dB for 4 GHz bandwidth with a thickness of 3 mm. The hybrid RAM

of double layered E-glass/epoxy/MWCNT/nickel zinc ferrite with high aspect ratio

MWCNT, named as NMRAS 10 has shown an RL of -16 dB for 2.6 GHz bandwidth

and -10 dB for 4 GHz bandwidth with 3 mm thickness which is better microwave

absorption performance than hybrid RAM prepared with low aspect ratio MWCNT

From the multilayer analysis of thirty six RAMs, it is observed that five RAMs,

namely MRAS 8, MRAS 6, MRAS 3, NRAS 5 and NMRAS 10, exhibited better

performances in terms of -15 dB, -10 dB bandwidths, maximum reflection loss and

thickness. In order to select RAM with strong microwave absorption with minimum

thickness, MCDM methods are used. From the results of the three MCDM methods, it

is observed that NMRAS 10 is assigned with rank 1 against the given performance

criteria. The similarity of the ranks by the three methods is determined by evaluating

Kendall’s coefficient of similarity index and good agreement is obtained among the

three methods. The hybrid radar absorbing material NMRAS10’s better performance is

due to the coupling of the lossy dielectric and magnetic materials and its double layered

design. This resulted in a thin and efficient microwave absorber by eliminating the

impedance mismatch and providing the required loss mechanism to improve the

microwave absorbing performance. The structural performance of NMRAS 10 is

investigated by tensile strength (216 N/mm2), flexural strength (318 N/mm2), impact

strength (101 J/m) and hardness (Barcol hardness 50). These mechanical properties

confirms its suitability as a load bearing radar absorbing material.

From the simulation results of EM analysis of RAS composed of MWCNT and

NZF, torus arrayed structure has better microwave absorption than cylinder and cone.

Moreover, even from the parametric analysis, maximum RL of -75 dB at 9.2 GHz and

vi
-30 dB in the entire x-band is observed for torus arrayed structure with 0.5 mm minor

radius and 1.75 mm major radius. Therefore, the proposed RAS can be utilized as band

stop filters in the X-band as they possess high microwave absorption, lightweight and

fine thickness.

Keywords: Microwave Absorption, Nanocomposites, Solgel Method, Reflection loss,

MCDM methods, Electromagnetic simulation.

vii
 ACKNOWLEDGMENTS

First and foremost, I would like to thank God Almighty and my spiritual guru

Sadguru Jaggi Vaasu Dev for giving me strength, knowledge, ability and opportunity

to undertake this research study and to persevere and complete it satisfactorily. Without

their blessings this achievement would not have been possible.

A major research project like this is never the work of anyone alone. The

contributions of many different people, in their different ways, have made this work

possible. First and foremost, I owe my deep sense of gratitude to my

research supervisor Prof. KOONA RAMJI for giving me an opportunity to work

under his continuous guidance, support and encouragement throughout this

study and also for his guidance for my personal development and maturity to evolve

as an independent, confident and strong researcher, something which

I could have never learned from a book. I am extremely lucky to work with

such a high profile personality. This work is a result of many long and constructive

discussions. His guidance was the next best thing to knowledge, which I will cherish

throughout my life. He is truly a source of inspiration to me to pursue a research

oriented career.

I place on record my sincere thanks to Prof. P.V.G.D. Prasad Reddy, Vice-

Chancellor, Prof. P. Srinivasa Rao, Principal, Andhra University College of

Engineering (Autonomous) and other authorities of Andhra University,

Visakhapatnam, for providing an opportunity to work for my Ph.D. degree under the

part-time, external registration scheme.

I thank Prof. K. Venkata Subbaiah, Head of the Department, P. Srinivasa

Rao, Chairman of Board of Studies and all the faculty of the Department of

viii
Mechanical Engineering, A.U. College of Engineering (A), for the suggestions given

by them while carrying out my research work.

I am really grateful to Governing body of D.M.S.S.V.H.C.E, Machilipatnam

for sanction of leave and encouragement for speedy completion of my research work.

My special thanks to Prof. T. Ravi Kumar, Head of the Department of D.M.S.V.H.C.E

for his constant encouragement and for providing me the required facilities at my work

place to complete this research work.

On a personal level, my husband P. S. Kameswara Rao, deserves my total

acknowledgement for his love, care, patience, encouragement, unending support and

sacrifices towards perusing my research work. Without his help I cannot imagine

fulfilling my goal of completing this research work. He deserves to share my success

equally. My loving children Jaanu and Pandu missed me a lot and sacrificed many of

their pleasant moments with me. I am greatly indebted to my beloved parents Sri. M.

Rambabu (Late), Smt. M. Jaya Lakshmi and my mother in law

Smt. P. Pitchamma for their blessings and unwavering support. I am grateful to my

sister M. Nagalakshmi and my friends, Dr. M. K. Naidu, Smt. T. Haritha,

Smt. B. V. S. R. N. Santoshi and Dr. K. S. R. Radhika, who supported me a lot in

every stage of this work. My special thanks to Dr. T. C. Shami,

Dr. Ch. Subramanyam, Dr. K. Krushna Murthy and Dr. V. V. S. S. Srikanth, for

access to their resources and cooperation. I gratefully acknowledge one and all who

helped me directly or indirectly in one way or the other for the successful completion

of this work.

P. Siva Nagasree

ix
 NOMENCLATURE

𝜀′ Real part of permittivity

𝜀 ′′ Imaginary part of permittivity

𝜖0 Permittivity of vacuum

𝜇′ Real part of permeability

𝜇′′ Imaginary part of permeability

𝜇0 Permeability of a vacuum

𝑓 Frequency

𝜖𝑝 " Polarization relaxation

𝜖𝑐 " Conduction loss

𝜏 Relaxation time

tan 𝛿𝑀, Magnetic loss tangent

𝑡𝑎𝑛 𝛿𝐸 Dielectric loss tangent

T5% Temperature required for 5% of weight loss

Zi Input impedance at the first air-absorbing interface

Za Free-space impedance

ki Propagation constant

α Attenuation constant value

C Velocity of light

𝐶𝑖+ Closeness coefficient

𝑄𝑖 Vikor Index

  a  Net outranking flow

𝑤
̃ Kendall’s coefficient

x
 ABBREVIATIONS

AFM Atomic force microscope

AHP Analytical hierarchy process
AMB Adjustable mean bar methods
ANP Analytic network process
ASTM American society for testing and materials
BWM Best worst method
CF Carbon fibre
CNF Carbon nano fibre
CNT Carbon nanotube
CPU Central processing unit
CRITIC Criteria importance through inter criteria correlation
DSC Differential scanning calorimetry
DTG Differential thermogravimetric
EDX Energy dispersive X-Ray analysis
EM Electromagnetic
EMI Electromagnetic Interference
EMW Electromagnetic Wave
FDTD Finite difference time domain method
FEM Finite element method
FESEM Field emission scanning electron microscope
FMR Ferromagnetic resonance
FTIR Fourier transform infrared spectroscopy
HDPE High density polyethylene
HFSS High frequency structural simulator
HRTEM High resolution transmission electron microscope
ICT Information communication Technology
LDPE Low density polyethylene
MADM Multi attribute decision making
MAUA Multi-attribute utility analysis
MAUT Multi attribute utility theory
MCDM Multicriteria decision making
MDL Modified digital logic

xi
MRI Magnetic resonance imaging
MODM Multiobjective decision making
MOM Method of moments method
MOORA Multiobjective optimization ratio analysis
MUT Material under test
MWCNT Multiwalled carbon nanotube
NL Numeric logic
NMR Nuclear magnetic resonance spectroscopy
NRW Nicholson ross weir
NZF Nickel zinc ferrite
PA Polyamide
PANI Polyaniline
PE Polyethylene
PEDOT Polyethylene dioxythiophene
PMC Polymer matrix composite
PMMA Polymethyl methacrylate
PP Polypropylene
PPY Polypyrrole
PROMETEE Preference ranking organization method for enrichment evaluations
PS Polystyrene
PSI Preference selection index
PVC Polyvinyl chloride
RAM Radar absorbing material
RAS Radar absorbing structure
RTM Resin transfer molding
SCF Silicon carbon fiber
SCL Short circuit line
SEM Scanning electron microscope
SiC Silicon Carbide
SMART Simple multi attribute ratio technique
STEM Scanning transmission electron microscope
SWCNT Single walled carbon nanotube
SQUID Super conducting quantum interference device

xii
TE Transverse electric
TGA Thermogravimetric analysis
TMM Transfer matrix method
TOPSIS Technique for Order Preference by Similarity to Ideal Solution
TPU Thermoplastic polyurethane
VARTM Vacuum assisted resin transfer molding
VIKOR Vlsekriterijumska optimizacija Ikompromisno Resenje
VNA Vector network analyzer
VSM Vibrating sample magnetometer
WSM Weighted sum model
XPS X-Ray photo electron spectroscopy
XRD X-Ray diffraction Analysis
Zno Zinc Oxide

xiii
 TABLE OF CONTENTS
CANDIDATE’S DECLARATION ii
CERTIFICATE iii
ABSTRACT iv
ACKNOWLEDGMENTS viii
NOMENCLATURE x
ABBREVIATIONS xi
LIST OF FIGURES xx
LIST OF TABLES xxiii
LIST OF PUBLICATIONS ON THE PRESENT WORK xxv

Chapter 1 INTRODUCTION ..................................................................................... 1

1.1 Introduction to Microwave absorption ................................................. 1
1.1.1 Introduction to Electromagnetic waves .......................................... 2
1.1.2 Microwave absorbers: Classifications ............................................ 3
1.2 Polymer composites for Microwave absorption................................... 8
1.2.1 Micro fillers in microwave absorption composites ........................ 9
1.2.2 Nano fillers in microwave absorption composites ....................... 10
1.3 Importance of MWCNT and NZF as radar absorbing materials ........ 11
1.3.1 MWCNT....................................................................................... 11
1.3.2 Nickel Zinc Ferrite ....................................................................... 12
1.4 Synthesis of Nano ferrites .................................................................. 14
1.4.1 High energy ball milling method ................................................. 15
1.4.2 Precipitation method .................................................................... 15
1.4.3 Microwave assisted and Sol-gel auto combustion methods ......... 16
1.5 Characterization of Nanomaterials ..................................................... 18
1.5.1 Microstructural characterization techniques ................................ 19
1.5.2 Chemical characterization techniques .......................................... 19
1.5.3 Magnetic and miscellaneous characterization techniques ............ 20
1.6 Fabrication of Radar absorbing materials .......................................... 21
1.6.1 RTM and VARTM ....................................................................... 21
1.6.2 Autoclave and compression moulding methods........................... 22
1.6.3 Hand layup method ...................................................................... 23
1.7 Theory of EMW absorbers and testing of EM properties .................. 24
1.7.1 Maxwell’s theory of electromagnetic waves ................................ 24

xiv
 1.7.2 Design of EMW absorbers ........................................................... 25
1.7.3 Single and multilayer absorbers ................................................... 27
1.7.4 Testing of EM properties.............................................................. 27
1.8 Thermal and Mechanical properties testing ....................................... 30
1.8.1 Thermal properties ....................................................................... 30
1.8.2 Mechanical properties .................................................................. 31
1.9 Multi Criteria Decision Making (MCDM) methods .......................... 32
1.9.1 Introduction .................................................................................. 32
1.9.2 Different MCDM techniques and Applications ........................... 34
1.10 Numerical simulation studies of RAMs ......................................... 34
1.10.1 Introduction ................................................................................ 34
1.10.2 Methodology .............................................................................. 35
1.11 Objectives of the current Research ................................................. 37
1.12 Hypothesis Statements .................................................................... 38
1.13 Significance of Present Research ................................................... 38
1.14 Motivation for Research and Problem Definition .......................... 41
1.15 Organization of the thesis ............................................................... 42
Chapter 2 LITERATURE REVIEW ....................................................................... 44
2.1 Introduction ........................................................................................ 44
2.2 Theoretical background and Applications of RAMs.......................... 46
2.3 Dielectric materials for Radar absorption .......................................... 50
2.3.1 Effect of weight percentage and thickness on absorption
properties ...................................................................................... 51
2.3.2 Effect of multilayer design on absorption properties ................... 52
2.3.3 Gaps identified in literature .......................................................... 53
2.4 Magnetic materials for Radar absorption ........................................... 54
2.4.1 Effect of weight percentage on absorption properties .................. 56
2.4.2 Effect of thickness on absorption properties ................................ 56
2.4.3 Effect of multilayer design on absorption properties ................... 57
2.4.4 Gaps identified in literature .......................................................... 58
2.5 Hybrid materials for Radar absorption ............................................... 59
2.5.1 Effect of weight percentages on absorption properties ................ 60
2.5.2 Effect of thickness on absorption properties ................................ 61
2.5.3 Effect of multi-layer design on absorption properties .................. 62
2.5.4 Gaps identified in literature .......................................................... 64
2.6 Synthesis of NZF by Sol-gel auto combustion method...................... 64

xv
 2.6.1 Effect of fuel agents and heat treatment on ferrites properties .... 65
2.6.2 Doping of elements in ferrites by sol-gel ..................................... 65
2.6.3 Microwave Absorption properties of ferrites prepared by sol-gel66
2.6.4 Gaps identified in literature .......................................................... 67
2.7 Fabrication of fibre reinforced Radar Absorbing materials ............... 67
2.7.1 Preparation of pre mixture in fibre reinforced RAMs fabrication 68
2.7.2 Temperatures and pressures in fabrication process ...................... 69
2.7.3 Gaps identified in the literature .................................................... 69
2.8 Evaluation of Thermal and Mechanical properties of RAMs ............ 70
2.8.1 Thermal properties of RAMs ....................................................... 71
2.8.2 Mechanical properties of RAMs .................................................. 72
2.8.3 Gaps identified in the literature .................................................... 74
2.9 Multi Criterion Decision Making (MCDM) Methods ....................... 74
2.9.1 Application of MCDM methods for material selection ............... 76
2.9.2 Gaps identified in the literature .................................................... 76
2.10 Numerical simulation of EM properties ......................................... 77
2.10.1 Modelling in EM simulation ...................................................... 77
2.10.2 Analysis in EM simulation ......................................................... 78
2.10.3 Gaps identified in the literature .................................................. 79
2.11 Shortcomings based on the Literature ............................................ 79
2.12 Objectives of the present work ....................................................... 81
2.13 Summary......................................................................................... 82
Chapter 3 EXPERIMENTAL METHODS FOR SYNTHESIS, FABRICATION
AND CHARACTERIZATION .............................................................. 83
3.1 Introduction: ....................................................................................... 83
3.2 Synthesis of NZF by Sol-gel auto combustion method...................... 84
3.3 Materials used in Fabrication ............................................................. 86
3.3.1 Epoxy resin and hardener ............................................................. 86
3.3.2 E-glass fibre.................................................................................. 87
3.3.3 MWCNT and NZF ....................................................................... 87
3.4 Fabrication Method of Radar Absorbing Materials ........................... 88
3.4.1 Fabrication of E-glass/epoxy /MWCNT composites ................... 89
3.4.2 Fabrication of E-glass/epoxy/NZF composites ............................ 90
3.4.3 Fabrication of E-glass/epoxy / MWCNT/Nickel Zinc Ferrite
composites for microwave absorption properties......................... 91

xvi
 3.4.4 Fabrication of E-glass/epoxy / MWCNT/Nickel Zinc Ferrite
composites for mechanical properties .......................................... 93
3.5 Characterization Techniques .............................................................. 93
3.5.1 X-ray diffraction analysis (XRD) ................................................. 94
3.5.2 Scanning electron microscope (SEM) .......................................... 95
3.5.3 Energy dispersive X-ray (EDX) analysis ..................................... 97
3.5.4 Transmission electron microscope (TEM) ................................... 98
3.5.5 Fourier transform infrared spectrometer (FTIR) ........................ 100
3.5.6 Vibrating sample magnetometer (VSM) .................................... 101
3.6 Testing of RAMs for EM, Thermal and Mechanical properties ...... 103
3.6.1 Vector network analyser (VNA) ................................................ 103
3.6.2 Thermogravimetric Analyzer (TGA) ......................................... 105
3.6.3 Universal testing machine (UTM).............................................. 106
3.6.4 Impact testing Machine .............................................................. 108
3.6.5 Barcol hardness tester................................................................. 109
3.7 Summary .......................................................................................... 111
Chapter 4 MICROSTRUCTURAL, CHEMICAL, MAGNETIC AND
THERMAL CHARACTERIZATIONS OF MICROWAVE
ABSORBING MATERIALS................................................................ 113
4.1 Introduction: ..................................................................................... 113
4.2 Characterization of Synthesized Nickel Zinc Ferrite ....................... 113
4.2.1 Morphological characterization of NZF ..................................... 113
4.2.2 Microstructural characterization of NZF.................................... 115
4.2.3 Magnetic characterization of NZF ............................................. 117
4.2.4 Chemical characterization of NZF ............................................. 118
4.3 Characterization of MWCNT ........................................................... 120
4.3.1 Morphological and chemical characterization of MWCNT ....... 120
4.4 Microstructural and chemical characterization of fabricated RAMs122
4.5 Thermogravimetric analysis of RAMs ............................................. 124
4.5.1 Thermogravimetric analysis of magnetic (NZF) RAMs ............ 124
4.5.2 Thermogravimetric analysis of hybrid (MWCNT+NZF) RAMs ....
.................................................................................................... 126
4.6 Summary .......................................................................................... 128
Chapter 5 EM CHARACTERIZATION AND MULTILAYER ANALYSIS
OF RAMs ............................................................................................... 129
5.1 Introduction: ..................................................................................... 129
5.2 Electromagnetic characterization of RAMs ..................................... 129

xvii
 5.2.1 EM characterization of dielectric (MWCNT) RAMs ................ 129
5.2.2 EM characterization of magnetic (NZF) RAMs ........................ 134
5.2.3 EM characterization of combined (MWCNT+NZF) RAMs ...... 140
5.3 Multilayer Analysis of RAMs .......................................................... 149
5.3.1 Multilayer analysis of dielectric (MWCNT) RAMs .................. 150
5.3.2 Multilayer analysis of magnetic (NZF) RAMs .......................... 152
5.3.3 Multilayer analysis of RAMs with low aspect ratio MWCNT and
NZF ............................................................................................ 154
5.3.4 Multilayer analysis of RAMs with high aspect ratio MWCNT and
NZF ............................................................................................ 157
5.3.5 Absorption mechanism in hybrid (MWCNT+NZF) RAM ........ 161
5.4 Summary .......................................................................................... 161
Chapter 6 SELECTION OF RAM USING MCDM METHODS AND IT’S
MECHANICAL PROPERTIES ....................................................... 162
6.1 Introduction ...................................................................................... 162
6.2 Subjective Weights by AHP ............................................................. 163
6.3 Objective Weights by ENTROPY method....................................... 168
6.4 Evaluation of compromised weights ................................................ 171
6.5 Determination of Ranks of RAMs ................................................... 172
6.5.1 TOPSIS method.......................................................................... 173
6.5.2 VIKOR method .......................................................................... 178
6.5.3 PROMETHEE-II method ........................................................... 181
6.6 Similarity of Ranks and Selection of RAM ..................................... 185
6.7 Comparison of M.A properties of NMRAS 10 with literature ........ 186
6.8 Mechanical Properties of MWCNT/NZF RAMs ............................. 186
6.8.1 Tensile and flexural strength ...................................................... 187
6.8.2 Impact strength and hardness ..................................................... 190
6.9 Summary .......................................................................................... 191
Chapter 7 SIMULATION STUDIES OF MWCNT/NZF RASs USING
COMSOL ............................................................................................... 193
7.1 Introduction ...................................................................................... 193
7.2 Procedure for Modelling and Analysis............................................. 194
7.2.1 Pre-processing ............................................................................ 194
7.2.2 Solution and Post processing ..................................................... 198
7.3 Validation of simulation and mesh convergence ............................. 198

xviii
 7.4 Microwave absorption of MWCNT/NZF nanocomposites with
geometric arrays ............................................................................... 200
7.4.1 Cylinder arrayed RASs............................................................... 200
7.4.2 Cone arrayed RASs .................................................................... 201
7.4.3 Torus arrayed RASs ................................................................... 202
7.5 Summary .......................................................................................... 203
Chapter 8 CONCLUSIONS AND FUTURE SCOPE .......................................... 204
8.1 Introduction ...................................................................................... 204
8.2 Conclusions ...................................................................................... 204
8.3 Recommendations for future studies ................................................ 207
REFERENCES ......................................................................................................... 209

xix
 LIST OF FIGURES

Figure No. Title of the Figure Page

No.
Figure 1.1: Electromagnetic spectrum and its applications 3
Figure 1.2: Types of microwave absorbers: a) Tapered loading absorber b) 5
Matching layer absorber c) Dallenbach absorber d) Salisburry
e) Jaumann abosrbers
Figure 1.3: Flow chart of Sol-gel auto combustion method 18
Figure 1.4: Hand layup Process a) Positioning of fabric b) Coating the 24
fabric with brush c) Squeezing with rollers d) Curing of samples
Figure 1.5: Measurement procedure using vector network analyser 29
Figure 3.1: Schematic representation of sol-gel auto combustion method 86
Figure 3.2: Raw materials used in synthesis process: a) Nickel Nitrate b) 87
Zinc nitrate c) Iron nitrate d) Urea
Figure 3.3: Sol-gel process a) Weighing of elements b)Sol-gel conversion 87
c) Auto combustion d) Before grinding e) After grinding f)
Calcination g) Ball milling h) Nickel zinc ferrite nano powder
Figure 3.4: Schematic representation of fabrication process 90
Figure 3.5: Fabrication process-Premixture preparation (a) Weighing of 92
components (b) After ball milling (c) During sonication
Figure 3.6: Fabrication process-Hand layup method (a) Cutting of E-glass 92
fabric (b) Coating on E-glass fabric (c) Before curing
Figure 3.7: Fabrication Process-Curing of samples (a) Hot air Oven (b) 92
Samples for curing (c) Prepared samples
Figure 3.8: XRD equipment at Dept. of chemistry, IIT Hyderabad, 96
Telangana
Figure 8.9: FESEM at AU Centre for Nanotechnology, Visakhapatnam, 98
Andhra Pradesh
Figure 1.10: Transmission Electron Microscope at SAIF lab, IIT Bombay, 100
Mumbai, Maharashtra
Figure 1.11: FT-IR at SAIF lab IIT Madras, Chennai, Tamilnadu 102
Figure 1.12: Vibrating Sample Magnetometer at SAIF lab, IIT Madras, 103
Chennai, Tamilnadu
Figure 3.13: VNA at Dept. of M.E, AUCE (A), Visakhapatnam, Andhra 105
Pradesh
Figure 3.14: TGA at Dept. of chemistry, IIT Madras, Chennai, Tamilnadu 107
Figure 3.15: Universal Testing Machine at CIPET, Vijayawada 109
Figure 3.16: Impact testing machine at CIPET, Vijayawada 110
Figure 3.17: Barcol hardness tester at CIPET, Vijayawada 111

xx
Figure 4.1: a) SEM image b) TEM image of NZF 115
Figure 4.2: Particle size distribution of NZF 116
Figure 4.3: XRD of synthesized NZF 117
Figure 4.4: SAED patterns of NZF 118
Figure 4.5: VSM of NZF 119
Figure 4.6: a) EDX and b) FTIR of synthesized NZF 120
Figure 4.7: SEM image of a) high and b) low aspect ratio MWCNT 122
Figure 4.8: a) TEM image and b) EDX of high aspect ratio MWCNT 123
Figure 4.9: a) FESEM and b) EDX of fabricated MWCNT RAM sample 124
Figure 4.10: a) FESEM and b) EDX of fabricated NZF RAM sample 124
Figure 4.11: a) FESEM and b) EDX of fabricated NZFM RAM sample 125
Figure 4.12: TGA curves of E-glass/epoxy/NZF composites 127
Figure 4.13: TGA curves of NZFM composites 128
Figure 5.1: Real values of complex permittivity of MWCNT samples 131
Figure 5.2: Imaginary values of complex permittivity of MWCNT samples 132
Figure 5.3: Real values of complex permeability of MWCNT samples 134
Figure 5.4: Imaginary values of complex permeability of MWCNT samples 134
Figure 5.5: Dielectric loss tangents of MWCNT samples 135
Figure 5.6: Magnetic loss tangents of MWCNT samples 135
Figure 5.7: a) Real values of Complex permittivity of NZF samples 137
Figure 5.7: b) Imaginary values of Complex permittivity of NZF samples 137
Figure 5.8: a) Real values of Complex permeability of NZF samples 138
Figure 5.8: b) Imaginary values of Complex permeability of NZF samples 138
Figure 5.9: Dependence of 𝝁′′ (𝝁′ )−𝟐 𝒇−𝟏 on frequency for NZF composites 139
Figure 5.10: Loss tangents of NZF samples 141
Figure 5.11: Real values of complex permittivity of NZFM samples 142
Figure 5.12: Imaginary values of complex permittivity of NZFM samples 142
Figure 5.13: Real values of complex permeability of NZFM samples 143
Figure 5.14: Imaginary values of complex permeability of NZFM samples 144
Figure 5.15: Dependence of 𝝁′′ (𝝁′ )−𝟐 𝒇−𝟏 on frequency for NZFM 145
composites
Figure 5.16: Dielectric loss tangents of NZFM samples 145
Figure 5.17: Magnetic loss tangents of NZFM samples 146
Figure 5.18: Complex permittivity of NMWCNT samples 147
Figure 5.19: Complex permeability of NMWCNT samples 148

xxi
Figure 5.20: Dielectric loss tangents of NMWCNT samples 149
Figure 5.21: Magnetic loss tangents of NMWCNT samples 150
Figure 5.22: Multi-layer Radar absorbing structure 151
Figure 5.23 Reflection loss of double layered MWCNT RAMs 153
Figure 5.24: Reflection loss of double layered NZF RAMs 155
Figure 5.25: Reflection loss of low aspect ratio E- 157
glass/epoxy/MWCNT/NZF RAMs
Figure 5.26: Reflection loss of high aspect ratio E- 160
glass/epoxy/MWCNT/NZF RAMs
Figure 5.27: Normalized characteristic impedance values of NZFM samples 160
Figure 5.28: Attenuation constant values of NZFM samples 161
Figure 5.29: Absorption mechanism in MWCNT/NZF composites 161
Figure 6.1: Methodology used in the determination of ranks 175
Figure 6.2: a) Tensile and b) Flexural and c) impact test samples 188
Figure 6.3: a) Tensile and b) flexural stress strain diagram of E-glass/epoxy/ 189
MWCNT/NZF composites
Figure 6.4: Flexural testing of E-glass/epoxy/MWCNT/NZF composites 190
Figure 7.1: Flow chart of modeling and analysis of RASs using COMSOL 196
Figure 7.2: Geometric modelling of cylinder arrayed RAS 197
Figure 7.3: Geometric modelling: a)cone arrayed RAS and b)torus arrayed 198
RAS
Figure 7.4: Generated mesh in COMSOL 198
Figure 7.5: Validation of simulation studies 199
Figure 7.6: Mesh convergence 201
Figure 7.7: RL of cylinder arrayed RASs 202
Figure 7.8: RL of cone arrayed RASs 203
Figure 7.9: RL of torus arrayed RASs 204

xxii
 LIST OF TABLES

Table No. Title of the Table Page

No.
Table 1.1 Microwave frequency bands and their applications 6
Table 2.1 Details of M.A properties of dielectric RAMs 54
Table 2.2 Details of M.A properties of magnetic RAMs 58
Table 2.3 Details of M.A properties of hybrid RAMs 63
Table 3.1 Weight percentages of high aspect ratio E-glass/epoxy/ 93
MWCNT/NZF samples
Table 3.2 Weight percentages of low aspect ratio E-glass/epoxy / 94
MWCNT/NZF samples
Table 4.1 TGA details of E-glass/epoxy/NZF composites 126
Table 4.2 TGA details of E-glass/epoxy/MWCNT/NZF composites 128
Table 5.1 Various double layered MWCNT Radar Absorbing Materials 152
Table 5.2 Details of the double layered NZF RAMs 154
Table 5.3 Details of the four layered low aspect ratio MWCNT and NZF 157
RAMs
Table 5.4 Details of the double layered high aspect ratio MWCNT and 159
NZF RAMs
Table 6.1 Performance details of the RAMs considered for MCDM 164
methods
Table 6.2 Saaty’s scale for comparison 166
Table 6.3 Pair wise comparison matrix 166
Table 6.4 Normalized pair wise matrix 167
Table 6.5 Weightages of performance criteria 167
Table 6.6 RCI average values by Saaty 169
Table 6.7 Decision matrix 170
Table 6.8 Entropy measure of performance characteristics of RAMs 171
Table 6.9 Degree of divergence and objective weights by Entropy method 172
Table 6.10 Subjective, objective and synthesis weights of criteria 173
Table 6.11 Form of generalized decision matrix 175
Table 6.12 Details of separation measures, closeness coefficient and ranks 179
from TOPSIS
Table 6.13 Utility measure and regret measure of alternatives in the VIKOR 181
method
Table 6.14 Details of VIKOR indices and ranks from VIKOR 181
Table 6.15 Performance difference of RAMs 183

xxiii
Table 6.16 Preference functions of alternatives 185
Table 6.17 Net out ranking of RAMs from PROMETHEE-II 185
Table 6.18 Scores & ranks provided by TOPSIS, VIKOR and 186
PROMETHEE-II
Table 6.19 Comparison of R.L values of NMRAS 10 with literature results 187
Table 6.20 Details of tensile and flexural properties 190

xxiv
 LIST OF PUBLICATIONS ON THE PRESENT WORK

Journal Publications:

 P. Siva Nagasree, K. Ramji, M. K. Naidu and T. C. Shami, “X-band radar-

absorbing structures based on MWCNTs/NiZn ferrite nanocomposites,

”Plastics rubber and composites, ISSN: 1465-8011 (Print), 1743-2898

(Online), Volume 50/Issue 2, pp. 71-82, 2021, SCIE, Impact factor-2.01,

DOI: https://doi.org/10.1080/14658011.2020.1836882

 P. Siva Nagasree, K. Ramji, C. Subramanyam, K. Krushnamurthy and T.

Haritha, “Synthesis of Ni0.5Zn0.5Fe2O4-reinforced E-glass/epoxy

nanocomposites for radar-absorbing structures” Plastics rubber and

composites, ISSN: 1465-8011 (Print), 1743-2898 (Online),Volume 49/Issue

10, pp. 434-442, 2020. SCIE, Impact factor-2.01, DOI:

https://doi.org/10.1080/14658011.2020.1793080

 P. S. Nagasree, K. Ramji, K. K. Murthy, M. Kannam Naidu and T. Haritha,

“Fibre Reinforced Polymer (FRP) Nanocomposites for Radar Absorption

Application in the X-Band”, Lecture notes in Mechanical Engineering, ISSN:

2195- 4356 (print) 2195-4364 (online),pp. 409-418, 2020, Scopus (Springer),

DOI: https://doi.org/10.1007/978-981-15-1124-0_35

 P. S. Nagasree, K. Ramji, T. Haritha and B. V. S. R. N. Santoshi, “Polymer

based MWCNT/Nickel Zinc Ferritenanocomposites for RAS application with

simulation,” Materials Today proceedings, ISSN:2214-7853, Volume 8/part-1,

pp. 406-412, 2019, Scopus (Elsevier), DOI:

https://doi.org/10.1016/j.matpr.2019.06.318

xxv
 International Conferences:

 P. S. Nagasree, K. Ramji, K. K. Murthy, M. Kannam Naidu and T. Haritha,

“Fibre Reinforced Polymer (FRP) Nanocomposites for Radar Absorption

Application in the X-Band”,The Second International Conference on

Innovations in Mechanical Engineering (ICIME 2019) by the Department of

Mechanical Engineering, Guru Nanak Institutions, Telangana, India, January

4 and 5, 2019

 P. S. Nagasree, K. Ramji, T. Haritha and B. V. S. R. N. Santoshi, “Polymer

based MWCNT/Nickel Zinc Ferritenanocomposites for RAS application with

simulation, ” The international conference on Advances in Materials and

Manufacturing Engineering (ICAMME-2018) by the Department of

Mechanical Engineering, University college of engineering and Technology,

Acharya Nagarjuna University, Guntur, A.P, India, 24th to 25th January 2018.

xxvi
Chapter 1 INTRODUCTION
1.1 Introduction to Microwave absorption

The information age, current era we are living in has turned the entire world into

a global village. This transformation happened due to the unprecedented growth of

advancements in wireless communications and electronics systems. These systems

operate in the Giga frequency range due to high data transfer rates [1-2]. This

information communication technology (ICT) has had a significant economic impact

around the globe and made personal lives more digital, connected and automated.

However, the radiation emissions and unwanted electromagnetic waves of ICT devices

cause the malfunctioning of electronically controlled systems like aeroplanes control

panels, computer LANs, mobile phones and personal computers. This phenomenon is

known as noise or electromagnetic interference (EMI). Another serious issue to be

considered here is the effect of radiation on human health. It causes diseases like

leukaemia, cancer, sleep disorder, headache, higher stress and fatigue when humans are

longer exposed to radiation.

It is necessary to absorb the microwaves to eliminate the EMI and to protect

human health [3-4]. To reduce the detectability of aeroplanes and ships in stealth

technology, lightweight, strong microwave or radar absorbing materials (RAMs) with

multifunctionality are needed to be developed. When the microwave absorbers with

load bearing capabilities are used to prepare the components like wing airfoils,

dielectric resonator absorbers, band stop filters, doors of microwave ovens and bricks

for EMI shielding rooms they are named as radar absorbing structures (RASs). These

RAMs and RASs found wide applications in civil and military fields, in particular

stealth technology, TV image interference in high rise buildings and EMI coatings,

EMC and anechoic chambers, microwave dark rooms, EMI shielding rooms, gaskets,

1
tapes, for protection of medical and laboratory equipment [5-7]. It is necessary to

understand the nature of electromagnetic waves, their interaction with the matter and

microwave absorption methods to design and develop microwave absorbers.

1.1.1 Introduction to Electromagnetic waves

The electromagnetic waves permeate the earth and whole cosmos from all

directions and are formed with the periodic change of electric field and magnetic fields

perpendicular to each other. The electromagnetic spectrum of different wavelengths is

produced depending on the periodic change and the generated power. The main source

of EM waves is the sun on the earth and several other sources depend on technology.

Their frequency, wavelength and energy express the EM waves. The EM waves may

be reflected, diffracted or refracted when striking the matter or they are also absorbed

by matter and converted to heat energy depending on the EM properties of the matter.

The EM spectrum includes radio waves to gamma rays with wavelength and

frequency ranging from (108 m, 3 Hz) to (10-12 m, 300X1018 Hz). They are of

enormous scientific interest and imperative in modern communications, medical,

military, scientific instruments, radars, satellites and spaceships. The EM waves are

familiar in computer processing, memory, data, microwave instrumentation and

automobiles. The spectrum of electromagnetic radiation and applications are shown in

Figure 1.1. The X-band (8.2-12.4 GHz) in microwave frequency is significant as it is

employed in electronics applications including wireless computer networks, amateur

radio and satellite communications as well as mechanical applications like motion

detectors in traffic control, airborne, land and naval radars of military agencies and

lighting strike structures.

2
 Figure 1.1: Electromagnetic spectrum and its applications

1.1.2 Microwave absorbers: Classifications

The German Inventor Cristian Hulsmeyer in 1904 was the first who used radio

waves to detect the presence of metallic objects. The electromagnetic interference

(EMI) is recognized in the year 1933 by the international Electrotechnical commission

(IEC) committee located at Paris. It is aimed initially to realize the complications in

long term applications in radio frequency range. Later in 1960s and 1980s the

researchers became fascinated in developing new regulations for EM emissions and the

preparation of materials to suppress the EM radiation. During the early stages,

microwave absorbers are mostly used to eliminate the EMI problem. Because of the

critical requirement of low observability in the aerospace sector, the need for absorbers

got enhanced. This need fostered the development of different types of radar absorbing

3
materials, which are thin, lightweight and reliable whilst having strong absorption, a

wide bandwidth and tunable electromagnetic properties [8-9]. Particularly the

development of radar absorbing materials in the X-band is needed because most radar

applications are involved in this region. The designation of microwave frequency bands

and their applications are shown in Table 1.1.

The major classification of RAMs is impedance matching absorbers, resonant

absorbers, circuit analogue RAMs and magnetic RAMs. Different types of available

impedance matching absorbers are pyramidal, tapered loading and matching layer

absorbers. The zero reflections from the absorber layer are provided by reducing the

impedance step between the absorbing material and incident media. The resonant

absorbers are also known as quarter wavelength or tuned absorbers, including

Salisbury, Jaumann and Dallenbach absorbers [10-15]. They are dependent on the

destructive interference of electromagnetic waves. When the difference in the distance

travelled by the equal intensity reflected EM waves is equal to the even multiples of

λ/2, then the intensity of reflection will be equal to zero. The impedance matching and

resonance absorbers are shown in Figure 1.2.

The Salisbury screens are the long back developed simple structured RAMs in

which the homogeneous resistive sheets are placed at a distance of λ /4 distance from

the ground plane. The limited bandwidth provided by single layered screens can be

eliminated using the multi-layered designs known as Jaumann absorbers, but they are

also limited by high thickness

4
Figure 1.2: Types of microwave absorbers: a) Tapered loading absorber b)
Matching layer absorber c) Dallenbach absorber d) Salisburry e) Jaumann
abosrbers

5
 Table 1.1 Microwave frequency bands and their applications
S. No. Designation Frequency Wavelength Applications
range range
(GHz)
1 L band 1-2 15-30 cm Mobile phones, GPS, military
telemetry, amateur radio
2 S band 2-4 7.5-15 cm Radar for weather and surface
ships, some communication
satellites, microwave ovens, radio
astronomy, mobile phones,
wireless LAN, GPS, blue tooth
zigbee, amateur radio
3 C-band 4-8 3.75-7.5 cm Long distance radio tele
communications
4 X-band 8-12 25-37.5 mm Satellite communications, radar,
terrestrial, broad band, space
communications, amateur radio,
mobile applications, LANs
5 Ku band 12-18 16.7-25 mm Satellite communications, vehicle
speed detection, television
network’s studio
6 K band 18-26.5 11.3-16.7 Radar, Satellite communications,
mm astronomical observations and
automotive radar
7 Ka band 26.5-40 5.0-11.3 Satellite communications,
mm emergency communications, rural
broad band, distance education and
telemedicine
8 Q band 33-50 6.0-9.0 mm Satellite communications,
terrestrial communications,
automotive radar, radio astronomy
9 U band 40-60 5.0-7.5 mm Satellite communications,
10 V band 50-75 4.0-6.0 mm Millimeter wave radar research
and other kinds of scientific
research
11 W band 75-110 2.7-4.0 mm Satellite communications, military
radar targeting and tracking,
millimeter wave radar research and
automotive radar
12 F band 90-140 2.1-3.3 mm Radio astronomy, microwave
devices/communications, wireless
LAN, most modern radars, satellite
television broadcasting,
communication satellites, amateur
radio
13 D-band 110-170 1.8-2.7 mm High frequency microwave radio
relay, radio astronomy, microwave
remote sensing, directed energy
weapon, amateur radio and
millimeter wave scanner

6
 In the Dallenbach absorber, a homogeneous layer is placed on a conducting

plane. For a particular wavelength, the permittivity, permeability and layer thickness

can be altered to minimize the reflectivity. However, several homogeneous layers piled

together can produce increased bandwidth as it is impossible to obtain a broad

bandwidth with a single layer.

Another way of improving the performance of resonant absorbers in terms of

minimum reflectivity, less thickness and wider bandwidths is to replace the resistive

sheets with geometric patterns of materials containing capacitance and inductance. This

type of absorbers are known as circuit analogue RAMs and the examples are conducting

polymer coated fibres and dielectric layer coated helical metal coils etc. [16-17]. The

frequency selective surface (FSS) is also one type of circuit analogue RAMs. It consists

of two-dimensional array of elements on metallic structure with frequency filtering

properties [18-20]. FSSs are frequently used as band pass filters in radomes. Magnetic

RAMs are based on hexaferrite and carbonyl iron as lossy materials. By varying the

sintering temperature and particle size [21-22], these materials can be used as absorbers

in the high frequency range (5-20 GHz).

Other noted categories of RAMs are based on the loss mechanisms exhibited

and the strength of the absorbers. The dielectric, magnetic and hybrid absorbers are

characterized based on the loss mechanisms they displayed. The hybrid absorbers with

the combination of both types of losses result in lower thickness, larger bandwidths [23-

24]. Depending upon the strength of the radar absorbing materials, they are classified

as absorber coatings and structural absorbers. These are the two popular absorbers used

to reduce the radar cross section of aeroplanes and ships used in stealth technology. The

third method to reduce the RCS is shaping the targets to reduce the EM waves

backscattered to a radar source direction.

7
 Generally, absorbing coatings are used where the space is a premium

consideration and they can be applied on any existing target surface with any shape.

But they increase the weight of the target structure and lack environmental resistance

and mechanical properties and also they need constant repairs and maintenance. The

idea of a structural absorber is to propose an absorber that has a load withstanding,

environmental resistance and EM energy absorbing capabilities [20 and 25-26]. The

properties like high stiffness and strength of RAS, in addition to strong microwave

absorption, make them significant in aeronautical/ aerospace, EMI shielding and EM

lightning protection applications.

1.2 Polymer composites for Microwave absorption

The composite materials are multi phased materials with a continuous phase

known as matrix and scattered phase known as reinforcement. They can sustain the

benefits and overcome some deficiencies of initial components and exhibit certain new

novel properties. The evolution and advancements of these composites is form typical

example of material designing. In 1970’s, only 7% of the Concorde airplanes were

fabricated using fibre reinforced polymer (FRP) composites. Today 85% of Boing

Dreamliner is made of FRP composites. They are widely used due to their ability to

merge easily with other materials needed to cater to different applications, including

aircrafts and automobiles. In particular, polymer based composites are widely used as

microwave absorbers and shielding materials because of their high specific strength,

low weight, low cost, corrosion resistance, good damping characteristics, flexibility and

ease of processibility compared to metal matrix and ceramic matrix composites [27-

28]. The structural integrity and microwave absorption properties required for aircrafts,

wind turbine blades are also ensured by the polymer based fiber reinforced composites.

8
 All three types of polymer matrices namely thermoplastic (PVC, polyethylene,

polypropylene, TPU, LDPE, HDPE, polystyrene, polyamide), thermosetting (epoxy,

polyester, polyurethane, urea formaldehyde) and elastomers (natural rubber, silicone

rubber) are used in the fabrication of radar absorbing materials [29-32]. In

thermosetting polymer matrices, epoxies are good candidates for microwave absorption

(MA) applications due to their ease of mixing with various fillers, low cost and

chemical resistance. Along with the above-mentioned insulating polymers, conducting

polymers including polyaniline (PANI), polypyrrole (PPY), polyacetylene and

polyethylene dioxythiophene (PEDOT) are also used in radar absorption.

1.2.1 Micro fillers in microwave absorption composites

The recent advances in polymer composites are accommodating various types

of fillers to make them suitable for numerous fields such as microelectronics,

automobiles and structural applications. Filler is a substance that is incorporated in a

matrix to enhance the processing characteristics and adjust composite properties. The

interface and compatibility of the polymer matrix and the filler have a significant role

in the ultimate properties of the composites. Particularly the microwave absorbers are

designed to suppress the incident EM radiation consisting of electrical and magnetic

energies by dissipating them into heat. Various dielectric and magnetic materials with

microns size (ranging from 1μm to 30 μm) acting as lossy fillers/absorbents are

combined with polymers to reduce electromagnetic radiation. The carbon black in

epoxy polymers are widely used microfillers in microwave absorbing materials along

with CNT, CNF, SrFe12O9, NiFe [108, 109 and 166]. The multiple reflections exists

in polymer microfiller composites, where an EM wave reflects on the interfaces

between the composite components which leads to increase in total absorption loss.

9
Further decrease in size of fillers from microns to nano size offers additional advantages

in microwave absorption as described in next section.

1.2.2 Nano fillers in microwave absorption composites

The polymer composites filled with nanomaterials are the best choice for RAM

due to their larger interfacial area per unit volume. At the nanometre length scales, more

number of atoms are present at or near the surface yields high surface energy, more

reactive nature and unique properties of lossy materials compared to their micro or bulk

counterparts [23 and 33]. When they are uniformly distributed in the polymer matrices,

they cause the dissipation of EMW energy by their different loss mechanisms. Several

research works were conducted to enhance the dispersion of nano fillers in the polymer

matrices, including shear mixing, ultra-sonication, chemical modification as they are

prone to form agglomerations.

Depending upon the major loss exhibited by the fillers, they are known as

dielectric, magnetic and hybrid absorbing materials. Dielectric absorbers exhibit the

maximum dielectric loss possessed by the conductive fillers e.g MWCNT, CF, carbon

black, graphite, silicon carbide. They have high permittivity values, low density and are

used in small weight percentages compared to magnetic absorbers [34-37].

Nevertheless, they suffer from narrow bandwidths and high matching thickness.

Various metals and ceramics having high permeability and magnetic loss are commonly

used magnetic absorbers. Their permittivity and permeability can be controlled by

varying their weight percentages. Examples of magnetic absorbing materials are spinel

ferrites, hexa ferrites, NiFe, Co, Fe, Ni, carbonyl iron [38-41]. The high density, high

weight percentage and resonance frequency in the MHz range are the demerits of

magnetic RAMs. The combination of dielectric and magnetic materials overcome many

10
of the disadvantages of single lossy filler absorbers due to the synergetic effect of both

materials

1.3 Importance of MWCNT and NZF as radar absorbing materials

An electromagnetic (EM) wave consists of both electric energy and magnetic

energy. The dielectric and magnetic absorbers that can absorb the corresponding energy

component. The absorption mechanism responsible for microwave absorption is largely

influenced by the geometry and EM properties of lossy fillers. Therefore various

dielectric and magnetic fillers for example SWCNT, MWCNT, graphene, RGO, CB,

SiC, FeNi, CoNi and various ferrites are used to prepare radar absorbing materials as

they possess various geometries and electromagnetic properties. Particularly

MWCNT and NZF are promising materials to be considered in the design of material

based RAM because of their attractive properties.

1.3.1 MWCNT

The carbon nanotubes, since discovered by Sumio Iijima in 1991, have been

captivating scientists and researchers of science and engineering to explore their unique

and unusual properties. The high-resolution TEM and electron diffraction helped

Iijjima reveal the structure and morphology of CNTs [42-43]. Depending on the

number of graphene layers rolled in the seamless cylindrical form, they are either

SWCNT or MWCNT. Carbon nanotubes are formed by the strong molecular

interactions provided by sp2 bonded carbon atoms. Combining this feature with the

natural tendency of CNT to bind together through Vanderwaal’s forces results in

exceptional properties for example high aspect ratio, electrical conductivity, elasticity,

strength to weight ratio, thermal conductivity and expansion [44-45]. Their potential

11
applications include composites, hydrogen storage, batteries, drug delivery, electronics,

sensors, electric conducting devices, space applications.

The multiwall carbon nanotubes is the most widely used dielectric microwave

absorbing and shielding material in the carbonaceous materials due to their ability to

enhance the host matrix dielectric loss even at low weight percentages [46-47].

According to the theory of electromagnetic percolation, the absorbent material in

polymer matrix should have high aspect ratio and high conductivity to set up a

conductive network. Due to these properties, the usage of MWCNT with various

polymer matrices like epoxy, polystyrene, polyaniline, polypropylene and PMMA led

to lightweight and low thickness RAMs [44 and 48]. The increase in the MWCNT

content in polymer matrices increases the conductive paths and the regions of

intercepting EM radiation. The combination of high aspect ratio MWCNT and

insulating matrices epoxy, polypropylene contribute to the absorption of

electromagnetic energy by the interfacial polarization and scattering due to differences

in permittivity values [30 and 47]. The incorporation of MWCNT greatly enhances the

mechanical strength and thermal stability of the RAMs. The combination of MWCNT

with Fe, Ni, FeNi, FeCo, CoNi and various ferrites compensated the low reflection loss

and bandwidths of MWCNT based RAMs [17 and 49-51]. The complementarity

between the complex permittivity and permeability supports the impedance matching

condition provided by combining the materials.

1.3.2 Nickel Zinc Ferrite

The interference and absorption of electromagnetic radiation are becoming vital

due to increased communication devices working in the GHz frequency range. The

polymer composites with magnetic materials are popular suppressors of EM radiation

12
due to their notable flexibility in regulating the magnetic properties and facileness of

preparation. The metallic/ alloy magnetic materials and ferrites are also majorly used

for this purpose. Ferrites in nano size exhibit complex permeability and permittivity,

which are essential for high frequency applications [52-53]. In the three types of

ferrites, spinel, garnets and hexa ferrites, spinel ferrites are used in the 3-30 GHz

frequency range for microwave absorption [54-55]. The spinel nickel zinc ferrite (Ni1-

xZnxFe2O4), a special member of the ferrites group, is a ceramic ferromagnetic material

that crystallizes into a face-centered cubic lattice structure. It is a magnetic oxide system

with divalent (Ni+2, Zn+2) and trivalent (Fe+3) ions occupying the tetrahedral and

octahedral sites. The allocation of ions in the respective sites can be altered by changing

the synthesis temperature and particle size in the nano region. These changes

significantly influence the magnetic properties of the nickel zinc ferrites and make them

suitable for different applications. Apart from microwave absorption, nickel zinc ferrite

has applications in antennas, recording heads, gas sensors, power transformer’s core

materials, electron beam reflectors, radiofrequency coils, rod antennas and many

branches of electronics and telecommunication engineering [56-57].

The facile synthesis methods can produce NZF with required particle size and

morphology, chemical homogeneity and crystal structure [58-59]. These inexpensive

synthesis methods, excellent chemical and thermal stability and the high magnetic loss

of nickel zinc ferrites are favourable for the preparation of cost-effective RAMs.

However, the application of NZF as radar absorbing material has limitations like high

filler loading, high density, low bandwidths and reflection loss [41 and 60]. These

drawbacks are surpassed by utilizing the NZF with low density and high dielectric loss

materials like MWCNT, graphene, carbon black [61-63].

13
1.4 Synthesis of Nano ferrites

Nanoscale materials largely promise the development of diverse applications in

current and future times. Nanostructured materials are needed for applications like

microwave absorption devices, wastewater treatment, biomedical imaging, recording

media, chemistry, medical diagnostics and genetic engineering [60 and 64]. The unique

electrical, optical, catalytic, magnetic and multi-functional properties of nanomaterials

are superior to their bulk counter parts due to the quantum size effect and larger surface

to volume ratio. The presence of many atoms at the surface causes interfacial

polarization, which leads to high dielectric loss and microwave absorption. Considering

the influence of nanoscale on magnetic material properties, it is always a real challenge

for scientists and researchers to synthesize materials with required stoichiometry,

structure and properties.

Many researchers developed several physical and chemical methods to produce

nanostructured magnetic materials. These methods include high energy ball milling,

chemical precipitation, auto combustion, sol-gel, hydrothermal, microwave sintering,

spray spin heating coating, refluxing, pulsed wire discharge, ultrasonic cavitation,

solvothermal, pulsed laser deposition, citrate precursor method, reverse micelle

method. Ferrites are the most versatile soft magnetic materials that attracted significant

research because of their low cost and interesting magnetic and electromagnetic

properties [56 and 65]. In preparing nano ferrites, high energy ball milling,

hydrothermal, solvothermal, precipitation, microwave-assisted auto combustion and

sol-gel auto combustion methods are the most widely used methods.

14
1.4.1 High energy ball milling method

The synthesis methods of nanomaterials are classified as top-down approaches

and bottom-up approaches. Mechanical milling or high energy ball milling is a top-

down approach employed to prepare various nanomaterials and nanocomposites.

During this process, different elemental powders are mixed in an inert gas atmosphere

subjected to plastic deformation and cold welding due to ball-ball and ball-vial

collisions [57 and 66]. This method is accompanied by post thermal treatment to

produce the sample with strain free grain formation. Even though it is a simple

technique operating at relatively low temperature for the production of nanocrystalline

or amorphous materials, it has some disadvantages like long milling hours (40 h, 60 h),

need of post processes like annealing and very controlled experimentation without any

contamination which is needed to avoid unstable phase formation [57 and 67-69].

1.4.2 Precipitation method

This method is a convenient and facile bottom-up approach for the synthesis of

magnetic nanoparticles. In this process, reduction of metallic ions is accomplished by

utilizing a basic solution (usually NH3OH NaOH, N(CH3)4OH) below 1000C

temperature [70-72]. As this method involves atomic scale mixing, the required

temperatures needed for calcination is low. The properties of the final product

synthesized by the co-precipitation method depend on the concentration of reagents,

pH, stirring speed and temperature of the mixture. The high yield, low cost and low

temperatures make this co-precipitation a more chosen method for the synthesis of

ferrites. It has the disadvantages like agglomerations, random particle sizes, not

applicable for high pure, accurate stoichiometric phase and batch to batch

reproducibility problems [73-74].

15
1.4.3 Microwave assisted and Sol-gel auto combustion methods

In auto combustion methods, ferrites are prepared using metal nitrates as

oxidant and cation sources, whereas the organic compound (urea, glycine, citric acid,

carbohydrazide and alanine) is used as a fuel. Once the reaction has started by the heat

supply, the auto combustion method is self-propagating and attains high temperatures.

Following powders rapid formation and crystallization, a large quantity of gas is

released, leading to minimum particle agglomerations. The advantages of this method

are fast preparation of reagents, simple reaction and controllability of the characteristics

of the final products.

For heating the reaction mixtures, two approaches are used. They are

microwave irradiation and conventional heating techniques (ex., Furnace or hot plate)

[75-78]. If the microwave irradiation is used, it is known as the microwave-assisted

auto combustion method and if the second method is used, it is the sol-gel auto

combustion method. The main advantage of the microwave auto combustion method is

that by utilizing the domestic microwave oven and in less than 10 min of reaction time,

the nanomaterials are synthesized. On the other hand, the sol-gel method was one of

the simplest and effective one step methods. In this process, sol is transformed into gel

to form voluminous, fluffy nano powders and it has many advantages. The flow chart

of sol-gel auto combustion method to prepare nickel zinc ferrite is shown in Figure 1.3.

The disadvantages associated with this method are long process durations, large volume

shrinkage and cracking during drying, difficulty in the synthesis of monolithics and use

of organics that can be toxic.

1.4.3.1 Advantages and applications of Sol-gel auto combustion method

This method has following advantages

16
  Flexibility and capability to prepare a wide range of materials

 The low temperature synthesis process

 Ease of controlling the stoichiometry

 Simple equipment and preparation process

 Low processing time and cost-effective process

 Vacuum free environment

 Good chemical homogeneity (mixing cations of required composition at the

molecular level)

 High product purity and crystallinity, fine particle size and narrow particle size

distribution

This method is used to prepare various types of ferrites used in the following

applications: Magnetic information storage media, Magnetic resonance imaging and

sensing, Magneto – optical devices, gas sensors and actuators, cell labelling and sorting,

therapeutic applications, catalytic applications, drug delivery, antenna rods, microwave

device applications, telecommunication equipment and microwave absorbers.

17
 Figure 1.3: Flow chart of Sol-gel auto combustion method

1.5 Characterization of Nanomaterials

The nanomaterial’s inherent small size (<100 nm), large surface area to volume

ratio and the number of shapes make them suitable in various fields e,g medical,

defence, security, agriculture, consumer goods, industry, energy and information

technology. Moreover, they are often the most engineered materials due to their

structure-property relationship. Therefore, before utilizing any material in a specific

application, the first step is to characterize or measure its physical and chemical

properties. Due to the extensive applications of nanomaterials, a wide range of

instrumentation consisting of microscopy, spectroscopy, diffraction, magnetization,

nanoindentation methods are developed largely a decade ago by many organizations.

The microscopy techniques of scanning probe microscopy and electron microscopy are

used to form the images of nanoparticles to measure the morphological details. The

spectroscopy measures the interaction of light with nanoparticles as a function of

18
wavelength or energy. The characterization methods are used to accurately measure the

size, shape, dispersion, solubility, chemical composition, surface area, crystal structure,

optical, magnetic and mechanical properties of nanomaterials.

1.5.1 Microstructural characterization techniques

The initial characterization performed after the nanomaterials synthesis reveals

the main parameters of nanoparticles, i.e., shape, size and their distributions, crystal

structure, chemical composition and surface area. To determine each of the above

properties, number of techniques are available. For example, to explore the size and

shape of the particles, SEM, TEM, AFM, 3D tomography, UV-vis, NMR, FMR are

available. Generally, the microwave absorption materials nanomaterials like carbon

nanotubes, ferrites, graphene, carbonyl iron are composed of different shapes

(spherical, cylindrical, platelets, flower) and sizes. The difference in particle size and

their distribution, the surface area of the materials influence the reflection and scattering

of EM waves. To achieve excellent microwave absorption properties of composites,

uniform dispersion of nanomaterials will be an advantage. Therefore, SEM and TEM

are majorly used to determine the shape, size, dispersion state of fillers and internal

porosity in the matrix material. The crystal structure can be obtained from XRD,

HRTEM, electron diffraction and STEM equipment. The XRD analysis obtains the

average crystal diameter and lattice constants using the Debye Scherrer formula and

Bragg’s law of diffraction [79-81].

1.5.2 Chemical characterization techniques

The XRD, FTIR, XPS, SEM-EDX, NMR techniques are devised for finding

elemental chemical composition. The analysis of chemical compositions of

nanoparticles near and at the surface can be obtained using the EDX attached to the

19
SEM. The major peaks in the EDX spectrum confirm the presence of main constituents

in the material and the minor peaks might be due to impurities present in the starting

materials used for the synthesis process [80 and 82].As researchers are developing

various microwave absorbers with a combination of different dielectric and magnetic

materials, EDX analysis is greatly assisting in the determination of different elements

present in the composites [83-85].FTIR is used to determine the molecule’s structure

with their characteristic absorption of infrared radiation. The data obtained from

microstructural and chemical characterization are used to check the formation of the

nanomaterials with the required nature (amorphous/crystalline), size, compositions or

presence of any impurities. All of these have a significant effect on microwave

absorbing properties.

1.5.3 Magnetic and miscellaneous characterization techniques

Nanoparticles with magnetic nature exhibit distinctive properties compared to

their bulk material. Magnetic materials are the first and most important materials to

absorb electromagnetic radiation. The SQUID, VSM, Mossbauer, MFM, FMR,

XMCD, MBS are the techniques utilized to determine magnetic properties. These

properties include magnetization saturation, remanence, curie temperature, magnetic

anisotropy energy, demagnetization field, magnetic moments and magnetic

susceptibility [86-87]. The hysteresis loops can obtain the magnetic nature of the

materials from the VSM result. In addition to the above characterization techniques,

thermo analysis techniques TGA and DSC are used to determine the percentage

composition of elements in a compound and heat capacity and reaction kinetics of

nanomaterials used for microwave absorption [88-89].

20
1.6 Fabrication of Radar absorbing materials

The polymer matrix composites for microwave absorption applications attracted

many researchers because of their simple processing techniques, ease of manufacturing,

low density, low cost and corrosion resistance. Moreover, by adding nanofillers like

MWCNT, carbon black, graphene, ferrites, nickel iron, the PMC's electromagnetic

properties can be tailored effectively. But the difficulty in achieving uniform dispersion

of these materials is a challenging task due to the agglomerated and entangled nature of

nanofillers in the polymer matrix. Therefore, many studies were conducted by

researchers on introducing different methods like mechanical agitation, shear mixing,

ultra-sonication, calendaring technique, solution evaporation processing, electroless

plating, sputtering and functionalization etc., to achieve the required uniform dispersion

of nanofiller [9 and 90-94].

The methods developed for the manufacturing of polymer matrix composites

are resin transfer moulding, compression moulding, injection moulding, filament

winding, pultrusion process, autoclave moulding, spray up method, resin film infusion,

hand layup and prepreg method. In all these methods, resin transfer moulding,

autoclave moulding, compression moulding and hand layup methods are more popular

to prepare radar absorbing materials [90 and 95-97]. During the curing of polymer-

based radar absorbing materials, the required temperatures and pressures have to be

provided as per the guidelines of the polymer suppliers. Equipment including

autoclaves, hot air ovens, hydraulic press and heavyweights are used for this purpose.

1.6.1 RTM and VARTM

In resin transfer moulding (RTM), preforms (pre-shaped fabric reinforcements)

are placed in the mould cavity and pressurized liquid resin with low viscosity is injected

21
via a central channel. It flows through the preform, which consisting of several layers

of continuous fibres. This method has the advantages like a short moulding cycle, low

volatile emissions, better reproducibility and the need for simple equipment [98-

99].Vacuum assisted resin transfer moulding (VARTM) process is the variation of

RTM process, in which vacuum is used to fill the preform in addition to resin injection

system [100-105]. Here thorough impregnation of the fiber reinforcement with liquid

resin was accomplished in a vacuum bag. The advantages of this method are lower

tooling costs, large components production and cored structures in one operation. Even

though resin transfer moulding processes (RTM and VARTM) has many advantages;

they have limitations like critical mould design, difficulty in uniform resin flow causing

resin rich edges and radii, movement of reinforcement during resin injection and very

expensive scrap parts with incomplete impregnation of preform. Apart from these, due

to the incorporation of nano constituents, an increase in viscosity restricts the resin's

flow and alters the curing process. Therefore, the application of these techniques in

nanoscience and nanoengineering has limited scope [106-107].

1.6.2 Autoclave and compression moulding methods

The autoclave moulding involves stacking nano-reinforced prepregs or fibers

coated with nanofillers, followed by a vacuum bagging method to remove all air

entrapped between the layers. Afterward, for curing in required pressure and

temperature, the whole assembly is moved to an autoclave machine. The composites

are removed from the mould after cooling the assembly [25, 97and 108-111]. The

advantages of this technique are high fiber volume fraction, versatile fiber orientation

and quality of products. In the compression moulding method, the prepregs are placed

between male and female metal dies and compressed with a hydraulic press or

heavyweights [6, 26, 92, 94 and 112]. This compression ensures the densification of

22
the composites. Then composites can be cured at room temperature or elevated

temperature depending on the strength requirements. Compression moulding is a low-

cost process and suitable for large volume production but curing cycle times are long.

1.6.3 Hand layup method

It is the oldest and most commonly used simple open moulding technique for

the manufacturing of composites. The manually positioned reinforcing fabric in an open

mould is poured, brushed, or sprayed over, by resin, layer by layer, so the required

thickness is obtained. The rollers or squeegees are used to remove any entrapped air in

the laminates structure as shown in Figure 1.4. The catalyst in the matrix resin system

initiates the curing process and hardens the fibre reinforced resin with or without

external heat. Most commonly, epoxies and polyster matrix resins which are cured at

room temperature, are used. This method makes it easy to align the fibers at the desired

orientation as hand assembly is used.

This process is labor intensive and the product quality depends on the skill of

the operator. But it has many advantages like low capital investment, the possibility of

onsite production, no limit on the size of the part, ease in changing the mould/design

etc. Several research works have been published on the fabrication of polymer based

radar absorbing structures using a hand layup method with autoclave and compression

moulding methods [26, 90, 92, 95-96, 108 and 112-114]. This method can produce

RAMs with excellent performances with lossy fillers like carbonyl iron, MWCNT,

NiFe, carbon black, graphene, carbon nanofibers etc.

23
 Figure 1.4: Hand layup Process a) Positioning of fabric b) Coating the fabric with brush
c) Squeezing with rollers d) Curing of samples

1.7 Theory of EMW absorbers and testing of EM properties

1.7.1 Maxwell’s theory of electromagnetic waves

The electromagnetic waves were first described by the equations given by James

Clerk Maxwell in 1864, one of the greatest achievements of physics and verified

experimentally by Heinrich Hertz in 1888. These equations showcase how the varying

electric and magnetic fields of EMW travel in vacuum at a constant speed. Along with

the EM properties of the matter through which they are travelling, these equations

determine the interaction of the matter with microwaves. The response of the matter

when microwaves strike completely depends on these EM properties only. Maxwell’s

equations are given by [12 and 115]

⃗⃗⃗⃗⃗
𝛁 ⃗ = − 𝛛𝐁 = −𝛍. ⃗⃗⃗⃗⃗
⃗ ×𝐄 𝛛𝐇/𝛛𝐭 1.1
𝛛𝐭

⃗⃗⃗⃗⃗⃗
⃗⃗ = 𝑱 + 𝝏𝑫 = 𝝈𝒄 ⃗𝑬 + 𝝐𝟎 (𝝐′ + 𝒋𝝐" ). 𝝏𝑬
⃗𝛁 × ⃗𝑯 ⃗ /𝝏𝒕 1.2
𝝏𝒕

⃗𝛁. ⃗𝑫
⃗ = ⃗𝛁. 𝝐. ⃗𝑬 = 𝝆𝒄 1.3

24
 ⃗ .𝑩
𝛁 ⃗⃗ = 𝛁
⃗ . 𝝁𝑯
⃗⃗⃗ = 𝟎 1.4

1.7.2 Design of EMW absorbers

The essential aspect of the microwave absorber is to soak up the incident EM

energy, thereby reducing the reflection of the waves from the surface. It has to exhibit

required loss and wide absorption bandwidth within the allowed thickness. The loss

characteristics of absorbers are dependent on the complex permittivity, complex

permeability and conductivity of the material. The complex permittivity and

permeability of the material indicate its polarization and magnetization capabilities.

The real and imaginary parts of them give the storage and dissipating capacity of

microwave energy. Single and double primes indicate them in the following equations

𝝐 = 𝝐′ + 𝒋𝝐" = 𝝐𝟎 (𝝐′𝒓 + 𝒋𝝐"𝒓 ) 1.5

𝝁 = 𝝁′ + 𝒋𝝁" = 𝝁𝟎 (𝝁′𝒓 + 𝒋𝝁"𝒓 ) 1.6

Where 𝝐𝟎 = 𝟖. 𝟖𝟓 × 𝟏𝟎−𝟏𝟐 F/m and 𝝁𝟎 = 𝟒𝝅 × 𝟏𝟎−𝟕 H/m

The conduction loss is predominant in electrical conductors, dependent on the

value of the conductivity. The value of conductivity can be calculated by the following

eq.

𝝈
𝝐"𝒓 = 𝝎.𝝐 1.7
𝟎

To have greater absorption of EM waves, the loss tangents (the ratios of

imaginary to the real parts of permittivity and permeability) should be high. They are

also known as the dielectric and magnetic loss capabilities of the material and given by

the following equations

𝝐"𝒓
𝒕𝒂𝒏𝜹𝒆 =
𝝐′𝒓
1.8

25
 𝝁"𝒓
𝒕𝒂𝒏𝜹𝒎 =
𝝁′𝒓
1.9

Generally, the EM wave consists of both electrical energy and magnetic energy.

Depending on the dominant loss exhibited by the microwave absorbing materials, they

are identified as dielectric, magnetic or hybrid microwave absorbers. The absorbed

energy is converted into heat.

From the definition, the reflection coefficient of lossy material at the interface

with the free space is given by,

𝒁−𝒁𝟎
𝚪=
𝒁+𝒁𝟎
1.10

Where 𝒛𝟎 is the free space impedance 𝒁 is the intrinsic impedance of the

material given by

𝝁𝒓
𝒛 = 𝒛𝟎 √
𝝐𝒓
1.11

The reflection coefficient values in decibels or reflection loss is given by

𝒛−𝒛𝟎
𝑹𝒅𝑩 = 𝟐𝟎 𝐥𝐨𝐠 (
𝒛+𝒛𝟎
) 1.12

Depending upon the number of layers of absorbent materials, they are classified

as single layer absorbers or multilayer absorbers. From the above equation, to have

greater reflation loss, the intrinsic impedance value of the material should be equal to

the impedance of the free space, known as the impedance matching condition. In

addition, another condition that needs to be satisfied by the absorbent material is the

greater attenuation constant. These two conditions are satisfied in a single layer and

multilayer absorbers by different design approaches.

26
1.7.3 Single and multilayer absorbers

The Dallenbach layer and Salisbury screens are the simple single layer resonant

radar absorbers. In Dallenbach layers, homogeneous lossy materials are coated on the

top of the metal backing. Salisbury screens consist of thin resistive material and foam

backed by PEC. These screens are narrow band absorbers, but their reflection loss can

be enhanced by utilizing a multilayer design. In multilayer design, the RAM is

composed of two or more layers of absorbing materials. The first layer is designed as

impedance matching layer and the subsequent layers as absorbing layers with high

attenuation constant. Due to this flexibility offered by multi-layered RAM, it provides

smaller thickness, wide bandwidth and maximum RL compared to single-layer

absorbers.

1.7.4 Testing of EM properties

The complex permittivity and permeability needed to determine the reflection

loss and transmission loss are obtained from various non-destructive experimental

methods like transmission/ reflection line method, open ended coaxial probe method,

free space method and resonant method. Each technique is restricted to specific

materials, frequencies and applications by its constraint. These methods utilize the

vector network analyzer and different conversion techniques to calculate the

permittivity and permeability from scattering parameters (S11 and S21). These

conversion techniques include NRW (Nicholson ross weir), NIST iterative, new non

iterative and SCL (short circuit line) approaches.

1.7.4.1 Transmission/Reflection line method

This technique involves placing a tight fitted machined sample in a wave guide

or coaxial line section and measuring the S-parameters. The TEM mode in the coaxial

27
line and TE 10 mode in rectangular wave guides are assumed to propagate. Computer

programs are developed to solve the equations for the conversion of S-parameters (S11

and S21). The samples with medium to high loss are measured using this technique

from which both permittivity and permeability of material under test can be obtained

[4 and 116]. But using this technique due to the air gap effects, accuracy is limited and

gives low accurate results when the length of the sample is the multiple of half the

wavelength of the EMW. The procedure of measurement of EM properties using VNA

is shown in Figure 1.5.

1.7.4.2 Open ended coaxial probe method

This method is particularly used when it is not possible to cut the samples for

measurement, for example biological specimens, liquids or semi solid samples [117-

118]. The reflection coefficient measured is used to calculate the permittivity of the

sample in the open-ended coaxial probe method. Here the probe is either immersed in

liquid samples or pressed against the specimen without causing any changes in the

material characteristics. The advantages of this method are easy to sample preparation

without any machining, short time measurement and temperature-controlled

environment for measurement. Disadvantages include the availability of only reflection

measurement, inability to determine permeability and measurement affected by air gaps

on the specimen.

28
 Figure 1.5: Measurement procedure using vector network analyser

1.7.4.3 Free space method

The large and flat material under test (MUT), under high temperatures or hostile

environments is measured in wide band frequencies through the free space method.

After calibration, the MUT is placed in the sample holder between the two antennas

facing each other and connected to VNA. The transmission and reflection coefficients

obtained from this method are post processed using a computer program to determine

the EM properties. This method gives both magnetic and dielectric properties. The

limitations of this method are the large size of the sample, diffraction of the sample

edges, multiple reflections between the sample surface and antenna [119-120].

1.7.4.4 Resonant Method

29
 The most accurate methods of obtaining permittivity and permeability are the

resonant methods. The perturbation method and low loss measurement are the two types

of resonant measurements generally used. In the more popular perturbation method, the

dielectric properties are obtained first by determining the quality factor and resonant

frequency of a blank cavity. After that filling the cavity with MUT and repeating the

measurement gives the permeability and permittivity by calculation [21 and 121]. Small

MUT and no need for calibration are the merits and requirements of VNA with high

frequency resolution; limited to narrow band frequencies are the drawbacks of this

method.

1.8 Thermal and Mechanical properties testing

Polymer matrix composites are well known for superior high strength and

stiffness to weight ratio, corrosion & fatigue damage resistance and high service

temperature. These composites attracted many industries like aerospace, automobile,

sport, rocket and military industry. In stealth technology and EMI shielding

applications, the PMC with absorbents/lossy fillers are widely used. Research on the

development of new and improved RAM needs its thermal and mechanical properties

to be tested. The thermal properties of any RAM is important as it decides how it reacts

when subjected to thermal fluctuations. The structural properties like tensile strength,

flexural strength, impact strength and hardness etc. determines the radar absorbing

materials ability to with stand loads applied in practical applications.

1.8.1 Thermal properties

The sufficient thermal stability of RAM is needed for maintaining stable

operation under high temperature operating conditions. The heat generated through the

dielectric and magnetic loss mechanism of absorbing materials has to be dissipated fast

30
for the stable and long-term performance of microwave absorbing materials. Hence the

temperature resistance and thermal conductivity are the required thermal properties to

be investigated for RAM [9, 31 and 122-123].

The thermogravimetric analyzer is used to determine the thermal properties in

the form of TGA and DTG curves. They give the changes that occurred in the weight

due to temperature changes. These changes are used to determine thermal stability,

moisture/volatile contents and the sample's composition, especially of multi-component

systems with different thermal degradation behaviours. The TGA curves have

temperature (00C-12000C) on X-axis and weight retention (0-100 wt%) on the Y-axis.

At the same time, the DTG curves indicate the temperatures of the most apparent weight

loss points. The TGA analysis of RAM indicates the weight percentages of different

fillers such as MWCNT, cobalt, graphite, ferrite, SiC etc. [123-124]. The effect of

weight percentages of fillers on thermal stability, relative amounts and purity of the

fillers are effectively confirmed by TGA curves [89 and 125-126].

1.8.2 Mechanical properties

Nowadays, the two stringent requirements of microwave absorbers are high

structural strength and low weight. Sandwich structures and fiber reinforced radar

absorbing materials satisfy these conditions adequately due to reinforcing elements.

The mechanical characterization of the composite materials is complex due to their

anisotropic and inhomogeneous behaviour. It brings about a range of test types and a

plethora of test standards. The radar absorbing materials are tested for different

strengths e.g tensile, flexural, impact, interlaminar shear, compressive and peel

strengths.

31
 RAM’s tensile and flexural strengths are determined using a universal testing

machine largely according to ASTM standards D3039 and D790-03. The obtained

stress strain curves are used to determine the various properties like young’s modulus,

flexural stiffness, maximum stress, maximum strain, elastic deformation and elongation

at break [95-96 and 127-128]. The inter laminar shear strength test, also known as the

short beam shear test used to determine the interplay strength of all parallel fiber

reinforced composites. A similar test for adhesively bonded layers is the peel strength

test [90 and 129]. To determine the suitability of materials for impact environments,

the total energy absorbed during impact events are measured by impact testing

machines. A dynamic mechanical analyzer determines the thermomechanical

properties of PMCs with frequency, load amplitude and temperature as input for the

test. The elastic modulus, viscous modulus and glass transition temperatures are the

outputs used to reveal the transition behavior from the glassy to the rubbery state of the

PMCs [128 and 130]. The high aspect ratio and interfacial bonding with matrix due to

homogeneous dispersion of absorbents in RAM favors the significant enhancement of

mechanical properties [47 and 131]

1.9 Multi Criteria Decision Making (MCDM) methods

1.9.1 Introduction

The MCDM problems of finding prioritization are prevalent in real-world

decision-making situations and the solution techniques were not newly developed.

These powerful and popular techniques evaluate the alternatives based on the decision

maker’s choice for a set of conflicting and non-commensurate criteria. The procedural

steps in the general MCDM method are: 1) Generation of alternatives, 2) Identification

of criteria, 3) Determination of criteria weights, 4) Assessment of alternatives 5)

32
Allocation of ranks. The MCDM techniques are of two kinds: the multi objective

decision making (MODM) and Multi attribute decision making (MADM). The MODM

consists of process designing and planning, whereas MADM in decision-making

considers assessing and selecting processes [132-133].

In 1970, Saaty proposed a 1-9 numerical scale to compare each criteria

preference level and used in AHP, ANP, BWM and MDL methods. The TOPSIS

method developed by Hwang and Yoon in 1981 determines the best alternative by

calculating the positive and negative ideal solutions [134-136]. The criteria or attribute

weights specified by the decision makers (DMs) are pivotal and control the decision-

making process’s result. In TOPSIS methods also the unreasonable allocation of criteria

weights leads to the wrong selection of the alternatives. The methods to determine

criteria weights are of three kinds, subjective methods (AHP, ANP, BWM, Delphi,

DLM, SMART), objective methods (AMB, CRITIC, entropy, MDL, NL) and

combinative weighing methods. The subjective methods consider the DMs preferences

by a ratio scale and are used for qualitative data. The objective methods are data based

and do not rely on DMs tendencies. It is always advantageous to use combinative

weighing methods as they take care of both qualitative and quantitative data [137-141].

The integration of MCDM methods compared to single ones resulted in better

alternatives as the limitations of one method can be overcome by the other. The

combination of AHP-PSI, AHP-PROMETHEE, AHP-VIKOR, TOPSIS-PSI, AHP-GC

TOPSIS, entropy-GRA and entropy-VIKOR explores the interrelations among the

various criteria. Currently, Fuzzy versions of MCDM methods are implemented in the

selection process to benefit from several experts’ linguistic assessments [132 and 142-

144].

33
1.9.2 Different MCDM techniques and Applications

The major application of MCDM in engineering design is in the material

selection process. This is due to the complex relationship between mutually exclusive

decision criteria for selecting numerous available material alternatives [3, 136 and 145].

The AHP, DEMATEL ELECTRE, TOPSIS, VIKOR, PROMETHEE II, MAUT,

MAUA, MOORA, PSI and WSM are popular methods used for this purpose. The

selection of inappropriate material may lead to many adverse effects like the

component’s failure, customer dissatisfaction, less profitability and damage to the

organization’s reputation. Moreover, if the sophisticated tools like MCDM techniques

are not implemented in the management of various field for example marketing and

business, environment, health, safety, logistics, human resources, water resources may

result in similar consequences and even more damage like fatality, environmental

degradation etc. also can happen.

1.10 Numerical simulation studies of RAMs

1.10.1 Introduction

Electromagnetic modeling or computational electromagnetics is the modeling

of the interaction between electromagnetic fields and physical objects. These

simulation studies allow researchers and engineers to effectively explore the EM

properties of various components or total systems [6, 16 and 146-147]. They are

applicable in every step of the design process of electromagnetic components, from the

beginning of conceptualization to the fabrication of the components to fulfil the

specifications related to the electromagnetic behaviour under working conditions. The

EM simulation software will be a game changer as it reduces the cost and time of a

product to appear in the market. These products range from sensors, chips, band filters

34
and antennas to whole devices, including smart phones, MRIs and aircraft. The various

possible designs of these products with enhanced performance can be tested. For

example, band pass/stop filters with dielectric resonators with arrays of different

geometries.

The Maxwell’s EMW theory equations of radar absorbing materials were

numerically solved using versatile and well established methods like finite element

method (FEM), method of moment method (MOM), transfer matrix method (TMM),

finite difference time domain method (FDTD) [6 and 148]. The microwave absorbing

properties are determined by 2D and 3D modeling of the electromagnetic structures

with different commercial softwares like COMSOL (FEM based), HFSS (FEM based)

and CST studio (FDTD based) FEKO (MOM based) [146]. The dedicated software

solvers acquire fast and accurate solutions with the help of specified numerical

technologies.

1.10.2 Methodology

The RF module is used for the simulation of EM absorption properties. In that

module, using Maxwell’s equations, frequency domain analysis, steady state and

transient analysis and eigen value analysis can be done. In the EM simulation, the

frequency domain interface is more appropriate whenever the properties of the

materials are linear with reference to the strength of the EM field and, the fields have

to vary as sinusoidal at a given time. In modeling rectangular waveguides WR90,

WR62, WR-28, WR-22 (corresponding to X, Ku, Kα, Q bands) and the RAMs or RASs,

inbuilt geometry tools are used. Otherwise, they can be imported from other modeling

softwares. The geometric model consists of domains and the boundary conditions

(BCs). The materials have to be specified for all the domains and depending on the type

35
of analysis, BCs are imposed [4 and 149]. The measured complex permittivity,

permeability and conductivity values obtained from VNA were specified as the input

parameters.

During the discretization process of FEM, the geometry is divided into number

of domains and consequently to number of elements, number of edges and number of

nodal points. In any finite element analysis, the accurate solution of the problem can be

achieved by meshing the spatial domain or the geometry more finely. But the finer

meshing consumes more CPU’s process time and memory. So, studies have to be

conducted on element sizes to balance the run time of CPU and accuracy of the solution

which is known as convergence in simulation analysis. One of the major issues faced

by electromagnetic simulation users is the validation of the results. i.e., how accurate

they are? The validation can be done in three ways of comparison 1) with the analytical

solution, 2) with experimentation and 3) with different softwares based on different

codes. The RAM simulations were validated majorly by using analytical analysis and

experimental verification [18, 23, 90, 96, 129 and 148].

The scattering S-parameters are selected as the output of the RAM/RAS

electromagnetic simulation analysis. The scattered electric field, power loss densities

by RAM/RAS is also calculated and visualized clearly. The mesh convergence tests are

also have to be performed to determine the suitable mesh density of given simulation

problem. These numerical methods were mainly utilized to replace expensive

prototyping. The safe virtual testing of dangerous operating environments in less time

can be accomplished [16, 148 and 150].

36
1.11 Objectives of the current Research

The ever increasing demand for microwave absorbers brings the need for their

design considering the most significant factors influencing their performance

characteristics. Therefore the present work’s objectives are to determine the influence

of the aspect ratio of multiwalled carbon nanotubes on the reflection loss of radar

absorbing materials. The larger length to diameter ratio of MWCNT results in fine

thickness RAMs even at low weight percentages. The exploration of microwave

absorbing properties of double layered MWCNT RAMs is to be attained by varying the

weight ratios of filler MWCNT in single layers since multi-layered RAMs absorption

properties can be tailored by changing the individual layer properties. The flexibility of

controlling EM properties by changing the dopants and their composition makes

magnetic materials a good choice for RAMs. For the preparation of magnetic RAM,

Nickel Zinc Ferrite is to be synthesized using the sol gel method by employing urea as

a fuel agent. The raw materials used in the preparation of RAMs are to be characterized

for their morphological, structural, chemical properties and the fabrication of RAMs

samples is to be done using Insitu polymerization process. The EM characterization has

to be done by VNA in the X-band by varying the weight ratios of filler materials.

The design of double layered NZF RAMs and prediction of their reflection

losses are to be accomplished to develop magnetic RAMs with strong absorption and

fine thickness. The microwave absorbing properties of hybrid multi-layered RAMs

with the combination of MWCNT and NZF are to be investigated as they provide

impedance matching condition, attenuation constants and dielectric & magnetic losses,

required to develop a good microwave absorber. Further, to ensure the applicability of

RAMs in real world applications like air foil wings, composite walls for EMI shielding,

stealth air crafts, their thermal stability in terms of decomposition temparatures,

37
mechanical properties like flexural strength, impact strength and hardness are to be

examined. The MCDM methods like TOPSIS, VIKOR and PROMETHEE-II are

needed to be executed for the selection the preferred hybrid RAM. These three methods

are going to offer systematic approach in the ranking of multi-layered RAMs

alternatives with conflicting and non-commensurable attributes of wider bandwidths,

maximum reflection loss and minimum thickness. These attribute are having substantial

importance in the design of an efficient RAM. Finally, the simulation studies of

geometrically arrayed RAS with different elements will be done to simulate the

application of the proposed hybrid RAS as a band stop filter in the X-band.

1.12 Hypothesis Statements

 Radar absorbing materials with larger aspect ratio fillers might enhance the

absorption and reduce the thickness compared to low aspect ratio fillers.

 E-glass fiber reinforced dielectric RAMs with fine thickness may exhibit good

microwave absorption properties than high thickness sandwich structures.

 Preparation of multilayered RAM with less than 30 wt% of NZF nanopowder

from the solgel auto combustion method would result in lightweight and high

absorption magnetic RAMs.

 Combination of MWCNT & NZF in multilayered RAMs could result in greater

absorption characteristics like maximum RL, larger bandwidths, and minimum

thickness in the frequency range of 8.4 to 12.4 GHz.

 Presence of NZF and MWCNT in E-glass/epoxy composites might ensure the

thermal stability of neat E-glass/epoxy composites. It may also promise load

bearing capabilities in terms of tensile strength, flexural strength, impact

strength and hardness.

38
  Selection of hybrid RAM by the several MCDM methods with combinative

weights may confirm the synergetic effects of dielectric and magnetic materials

in microwave absorption.

 Simulation of various geometric arrayed structures might guide the design of

efficient RASs, which can be further used for practical applications of RAMs.

Ultimately, the arrayed and optimized RASs from parametric studies may

provide 100 % absorption in the X-band as band stop filters in communication

devices.

 Implementing techniques like electroless plating, sputtering, surface

modification of nanofillers and the variation of the composite’s curing pressure

in the fabrication could raise the microwave absorbing properties of RAMs.

 Modelling the geometry of various lossy fillers like spheres and tubes and

simulation of their mechanical and microwave absorption properties would

result in efficient load bearing RAMs

1.13 Significance of Present Research

Nowadays, the microwave absorbers are gaining substantial importance due to

their involvement in the proper functioning of electronically controlled systems,

avoidance of the health hazards and enhancing the capabilities of stealth technology.

Particularly, X-band absorbers are most vital due to large number of applications like

detection of military targets, terrestrial communications, mobile applications, amateur

radio, LANs are associated with this band. The current research explores the details of

effect of weight percentages, thickness on the performance of dielectric, magnetic and

hybrid RAMs, fabrication methods and geometric designs such as multi-layered and

arrayed structures. These studies are crucial in the design of any microwave absorbing

material. It describes the preparation of magnetic RAM from the nanonickel zinc ferrite

39
synthesized using solgel auto combustion method which was not attempted by many

researchers earlier even though it is beneficial in the preparation of RAM. The

characterization of nanomaterials used in the fabrication of RAMs and samples of

RAMs for morphological, structural, and chemical and EM properties by XRD, SEM,

EDX, TEM, VSM and VNA are discussed in detail. These results helps to understand

the relation between these properties and nanomaterials absorption characteristics.

The fabrication of RAMs using insitu polymerization process along with

sonication and ball milling dispersion methods is explained. This RAM preparation

method will result in microwave absorbing materials with better reflection loss, thermal

and mechanical properties. The present work measures the changes in the EM

properties of RAMs by varying the magnetic (NZF), dielectric (MWCNT) and hybrid

nanofillers (MWCNT and NZF) weight percentages in the range of 8.2 to 12.4 GHz

and these properties are the important input parameters for the multilayered design of

RAMs. The reflection loss of multilayered E-glass/Epoxy/MCNT and magnetic E-

glass/Epoxy/NZF and hybrid E-glass/Epoxy/MCNT RAMs are predicted in this

research work, according to the transmission line theory. These reflection losses

demonstrates the multilayered structure’s influential microwave absorption properties

than single layered ones. The multi criteria decision making methods TOPSIS, VIKOR

and PROMETHEE-II are implemented to select the preferred RAM with better

microwave absorption properties using both subjective and objective weights by AHP

and Entropy methods. This implementation establishes the usage of MCDM methods

in the selection of microwave absorbing materials using combinative weights helps to

get an accurate decision. The investigation of decomposition temperatures, tensile

strength, flexural strength, impact strength and hardness of E-

Glass/epoxy/MWCNT/NZF composites which promotes the notable load bearing

40
characteristics of E-Glass fibre reinforced hybrid RAMs is also presented in this work.

The utilization of the COMSOL multiphysics software to design and optimize the

cylinder, cone and torus arrayed radar absorbing structures is reported in this current

research. It proposes the development of low weight and thin radar absorbing structures

to be implemented as bandstop filters in the X-band.

1.14 Motivation for Research and Problem Definition

In the twenty-first century, microwave absorbers are gaining vital importance

due to their vast applications in wireless & telecommunication devices and stealth

technology [20, 48, 151, 198 and 205]. The preparation of microwave absorbing

composites is not a simple process. It involves the careful study of various aspects like

type, size, geometry and weight percentage of lossy fillers to be used, selection of

appropriate synthesis method of the fillers, type of the polymer and the fabrication

method, structure design and thickness of radar absorbing materials. The systematic

approach used in the design of RAM can result in lightweight and thin microwave

absorbers with wider bandwidths. Even though many researchers proposed RAMs with

several lossy dielectric and magnetic fillers and multi-layered designs, very few of them

[148 and 344] utilized a combination of material and geometry based designs to prepare

RAMs with fine thickness. The evaluation of RAM's thermal stability and mechanical

properties are also not appropriately addressed despite their importance in practical

usage. The implementation of hybrid fillers, multilayer design approaches bring us one

step closer to solving the problems of conventional RAMs, such as high filler weight

percentage, larger thickness, low reflection loss, narrow bandwidths. Instead of fewer

attempts using MCDM methods for the selection of EMW absorber, still, the effect of

utilizing combinative weights needed to be focussed in implementation of these

methods. The attention paid to the simulation studies of radar absorbing materials

41
visualizes their applicability in real-world applications; still, there is a great deal of

work to be done in this area. [16, 129, 148 and 150].

The problem definition in the present work is to design the radar absorbing

materials with lower thickness, filler weight percentage, and intense absorption in the

X-band using multi-layered and arrayed structures of hybrid materials. Investigation of

decomposition temperatures, tensile, flexural, impact and hardness properties of RAMs

according to ASTM standards for real world applications. Subsequently, to implement

the multicriteria decision making methods using combinative weights in the selection

of RAMs from several alternatives available. Lastly, by adopting simulation studies to

design radar absorbing structures using geometric arrayed designs that can be further

employed in real-world applications.

1.15 Organization of the thesis

Chapter 1 details the microwave absorption materials, synthesis methods of

nano ferrites, characterization techniques and fabrication methods of RAMs. It also

presents the EM and mechanical testing of RAMs and outlines the application of

MCDM methods and simulation studies of RAMs.

Chapter 2 reports the earlier research conducted on radar absorbing materials,

the sol-gel method for synthesis of nano ferrites, fibre reinforced RAMs fabrication

techniques, evaluation of thermal and mechanical properties, multi criteria decision

making methods and numerical analysis of microwave absorbing materials.

Chapter 3 discusses the procedure used to synthesize NZF using the sol-gel

method and the equipment used to characterize the nickel zinc ferrite and MWCNT

used to prepare the radar absorbing materials. It demonstrates the fabrication of

different types of RAMs and also describes the experimental methods utilized to test

electromagnetic (VNA) and thermal properties (TGA) of radar absorbing materials.

42
 Chapter 4 shows the microstructural, chemical, magnetic properties of

synthesized NZF and MWCNT used to fabricate the RAMs. It also reflects the thermal

stability of fabricated RAMs.

Chapter 5 presents EM characterization results and the multilayer analysis of

fabricated RAMs using transmission line theory. The various multilayered RAMs

composed of MWCNT, NZF and combination of MWCNT and NZF were analyzed to

determine their microwave absorption properties.

Chapter 6 depicts the usage of TOPSIS, VIKOR and PROMETHEE II to

identify one RAM from five alternative RAMs with maximim reflection loss, wider

bandwidth and less thickness. It also gives the mechanical properties of the selected

double layered RAM composed of MWCNT and NZF with 3 mm thickness.

Chapter 7 demonstrates the modeling of RASs with three types of geometries

entities of a cylinder, cone and torus. It also describes the parametric analysis conducted

to determine the dimensions of geometric entities for optimum performance of RASs

in terms of reflection loss.

Chapter 8 shows the conclusions and future scope of the work. The outcomes

derived from EM and thermal characterization, analysis of multilayered RAMs,

MCDM analysis, mechanical characterization of selected RAM and simulation of

reflection loss of geometric elements arrayed RASs composed of MWCNT and NZF

were presented.

43
Chapter 2 LITERATURE REVIEW

2.1 Introduction

This chapter furnishes an outline of the earlier research conducted on radar

absorbing materials. The extensive applications of RAMs in both defence and civil

fields focus on reducing the EMI and avoiding detection of the target from radar [8-9].

The research on the development of lightweight microwave absorbers is essential to

reduce the risk of human health, protect electronic equipment and enhance the

capabilities of stealth technology [5-7]. To develop a radar absorbing material with

required performance characteristics like broad bandwidth, min RL, thickness, thermal

stability and mechanical strength, it is necessary to conduct a systematic literature

review on various aspects of RAMs and RASs. The literature review conducted on the

present work is divided into nine categories.

The attenuation of EMW mainly depends on the dielectric loss and magnetic

loss provided by the absorbing materials. Therefore, to select the best material for the

microwave absorption, the review of materials with predominant dielectric loss,

magnetic loss and combination of both losses was conducted [23-24 and 151-152]. The

theoretical background and applications of RAMs, effect of filler weight percentage,

thickness of the composites and multilayer design on EM absorption properties was

studied in 2.2, 2.3, 2.4 and 2.5 sections of this chapter. The review was confined to

polymer-based RAMs due to its low density, inherent flexibility and ease of preparation

[20 and 153-154]. The metal matrix absorbers only are referred to whenever it is

appropriate.

44
 The synthesis of nanomaterials with desired characteristics like size,

microstructure, composition and electrical and magnetic properties is always

challenging. The choice of synthesis method and its process parameters largely

influence the electromagnetic properties of RAM [155-156]. So, the literature on

synthesis of magnetic nano ferrites by sol-gel auto combustion method and the effect

of doping of various elements, influence of calcination temperatures on ferrites

properties discussed in section 2.6. The RAM electromagnetic properties and

mechanical properties depended on the fillers' homogeneity in the matrix, achieved

during the fabrication process [92, 111, 113 and 157]. Hence, in sections 2.7 and 2.8,

the past research works on the fabrication methods implemented to obtain efficient

RAMs and evaluation of mechanical and thermal properties of RAMs to determine their

suitability in practical applications were studied in detail.

Later, in section 2.9, the research works on the MCDM methods to select the

one RAM with wider bandwidth, maximum RL and lesser thickness were explored [3,

132, 145 and 158]. The last section 2.10 deals with the literature on simulation studies

of electromagnetic properties, which greatly assists the researchers in the EM

evaluation of new materials and designs. EM simulation studies facilitate the prototype

testing of electromagnetic components by avoiding fabrication and testing in the real

world [1 and 159-160]. Following is the list of literature review sections

2.2 Theoretical background and Applications of RAMs

2.3 Dielectric materials for radar absorption

2.4 Magnetic materials for radar absorption

2.5 Hybrid materials for radar absorption

2.6 Synthesis of NZF by sol-gel auto combustion method

45
 2.7 Fabrication of radar absorbing materials

2.8 Evaluation of thermal and mechanical properties of RAMs

2.9 Multi criteria decision making (MCDM) methods

2.10 Numerical simulation of EM properties

2.2 Theoretical background and Applications of RAMs

Microwave absorption theories play a significant role in the design of radar

absorbing materials. Major theories include Maxwell's theory of electromagnetic

waves, pointing theorem, transmission line theory, percolation theory, Maxell-Garnet

theory, and quarter wavelength matching theory. Maxwell's theory describes the

electromagnetic wave as coupled electric and magnetic fields travelling at speed equal

to the speed of light [12 and 115]. It gives the response of matter to electromagnetic

waves. The equations are given in detail in Section 1.7. The microwave energy, when

incident on a lossy dispersive material, creates heating within the material through the

interactions of the electromagnetic field with the material's molecular and electronic

structure. Poynting theorem governs the understanding of the conservation of power in

dispersive media. It states that the total power entering a through surface increases the

field energy stored inside the volume and is partially lost into heat [32 and 186].

The electromagnetic properties of complex permittivity and complex

permeability are the deciding factors of RAM's absorption properties. The EM

properties' real and imaginary parts represent the storage and dissipating capabilities of

electric and magnetic energies of incident electromagnetic waves [26, 54, 224, and

324]. The energy loss in a material illuminated by EM waves comes about through

damping forces acting on polarized atoms and molecules and through the finite

conductivity of a material. The loss tangents, which are the imaginary to the real part

46
of the EM properties, are directly proportional to the absorption properties exhibited by

the microwave absorbing materials [20, 23, 202, 234, and 246].

In order to enhance absorption, various types of fillers are added to RAMs. The

change in the EM properties due to adding fillers can be calculated using Maxwell–

Garnet theory. According to this theory, RAMs' effective permittivity and permeability

increase with the filler's volume fraction and it is expressed in equation 2.1 [32, 237,

319, 353 and 354]. The importance of high aspect ratio fillers in microwave absorption

is given by the electromagnetic percolation theory. This theory states that the filler

material in the polymer should possess high conductivity and aspect ratio to form a

conductive network easily and reach the percolation threshold at a low concentration of

conductive filler. The equation 2.2 expresses this percolation theory. [47, 213 and 321].
3𝜀𝑚
𝜀𝑒𝑓𝑓 = 𝜀 −𝜀𝑚 − 2𝜀𝑚 2.1
1−𝑓𝑖 [ 𝑖 ]
𝜀𝑖 +2𝜀𝑚

𝜎 = 𝜎0 (𝑉𝑓 − 𝑉𝐶 )𝛼 2.2

𝜎, 𝜎0 are the electrical conductivities of composite and filler respectively, 𝑉𝑓 , 𝑉𝐶

are the filler volume fraction and critical volume fraction at the electrical percolation

and α is the critical exponent.

The transmission line theory, the basis for the design of single or multilayered

RAMs, expresses the reflection loss in terms of the impedance of the absorber and free

space [26, 38, 112, 175 and 249]. The impedance of absorbers depends on EM

properties and their thickness. The corresponding equations are discussed in Section

5.3. Another important theory used in the design of RAM is quarter wave length

matching theory. This theory says, at a particular thickness, the incident and reflected

waves in the materials are out of phase by 1800 resulting in total cancellation of

reflected waves at air- material interface. The relation between the thickness of RAM

and the frequency to get maximum reflection loss is also given by this theory and

47
expressed in equation 2.3 [81, 87, 94, 192 and 199]. According to this theory, by

increasing the thickness of the composite, the reflection peak has to move toward the

lower frequency range.

𝑛 𝑛𝐶
𝑡𝑚 = 4 𝜆𝑚 = 4𝑓 2.3
𝑚√|𝜖𝑟 𝜇𝑟 |

Where fm is the peak frequency of R.L, tm is the thickness of the sample, 𝜖𝑟 & 𝜇𝑟

are the complex permittivity and permeability at fm and c is the velocity of the light.

Besides the quarter wavelength matching theory, two conditions must be

ensured in the design of RAM. One is impedance matching condition, and the other is

a high attenuation constant value [26, 61 and 222]. These two conditions were evaluated

for the magnetic MWCNT RAMs of N doped Co-C/MWCNT, zinc ferrite/MWCNT,

COZnF/N doped MWCNT composites for the maximum reflection loss [82, 214 and

216]. Implementing the impedance matching condition and high attenuation constant

can be done effectively using a multilayer design in the hybrid absorbing materials

[51,149, 151 and 242-248]. Either by the combination of the dielectric and magnetic

materials in each layer [243 and 247] or by using the dielectric or magnetic materials

separately in different layers of multilayered absorbers, the required reflection loss and

bandwidths are gained with lower thickness values [51, 149, 242, 244-246 and 248].

Comparison studies were conducted in the past literature to demonstrate the superiority

of the double absorber over the single layers absorbers [149, 244-245 and 247].

The microwave absorbers have wide applications in civil, medical, nuclear

physics and military fields. These applications include EM shielding for electronic

equipment, wireless mobile communications, EM resistant buildings, EMI shielding

gaskets and tapes, in the medical industry to isolate critical patient chambers from EM

exposure, shielding of human eyes, optical sensors from severe laser pulses, electronic

pacemakers, defensive shielding of computers and consumer electronics, RCS

48
reduction in stealth air crafts, helicopters, missiles, warships and camouflage

technology [15, 16, 20, 129, 148, 150, 198, 345, 346 and 347]. In nuclear physics, for

nuclear EM pulses, protection and shields used in particle accelerators are made of

RAMs.

An RCS reduction technology plays a very vital role in the survivability and

mission capability of an aircraft and weapon system [15, 16, 20, 129, 198, 345, 346 and

347]. The RAS, a representative application of multifunctional composite structure,

provides the simultaneous functions of load bearing electromagnetic absorption. The

RASs made of nickel coated glass fibre epoxy composites are used to prepare wing

shaped air foils to reduce the RCS of stealth air crafts [15, 16,129 and 198]. Studies

were conducted to prepare the potential applications of microwave absorbing materials,

including composite walls, wind turbine blades made of lossy fillers to avoid EM

waves, and structures resistant to natural lightning strikes [6, 136,148 and 150].

Several methods are used to measure the frequency and time domain

electromagnetic properties using one or two ports. Each method has its restrictions and

is applicable to specific frequencies, materials and applications. Majorly four methods

are widely used and they are 1. Transmission/ Reflection line method 2.Open ended

coaxial probe technique 3. Free Space technique 4. Resonant Method. In order to

perform the EM measurements in all the above methods, microwave dark rooms,

anechoic chambers for realizations of wedges and pyramidal arrays, radar dome

(radome) are required. Modern microwave communication especially mobile

communication and satellites, require high performance band stop filters having high

frequency selectivity, smaller size, and high stopband attenuation.

49
2.3 Dielectric materials for Radar absorption

The polymer matrices with dielectric materials have gained considerable

attention in microwave absorption due to their ability to produce lightweight,

structurally sound, corrosion-resistant and flexible RAMs [29-31 and 161-162]. The

major dielectric materials include conductive fillers like SWCNT, MWCNT, CB,

graphene, reduced graphene oxide, CF, SCF, CNF etc. as they possess lightweight, high

complex permittivity and dielectric loss [29, 34-37, 44, 47-48, 130,151, 163 and 164-

166].

The unique structured MWCNT is popular carbon based EM absorbing material

due to its excellent electrical, mechanical and thermal properties even, at 0.1 wt% [44

and 47]. Graphene & reduced graphene oxide are the important allotropes of the carbon

that attracted researchers due to their distinct high surface area, lightweight, porous and

layered morphology [48 and 151]. The CNF has advantages like higher aspect ratio,

electrical conductivity and less expensive mass production [163-164]. The microwave

absorption properties of dielectric materials dependent on the method of dispersion,

filler loading, the thickness of the composite, frequency and angle of incidence of EM

wave. By varying the EM wave’s angle of incidence on microwave absorbers from 00-

800,the RL of -10 dB was obtained, only in the angular range of 300-450 [34-37 and

167].

At microwave frequencies, carbon nanomaterials geometry and size can greatly

modify the EM properties [5, 34 and 165]. Previous studies [29, 35, 130 and 166] shown

that the high aspect ratio of MWCNT enhances the microwave absorbing and shielding

performances. Further to strengthen the dielectric properties, different dielectric

50
materials like SiC, ZnO, TiO2, BaTiO3 , La(NO3)3, Al2O3, BaCa(TiSn)O3 ,SrTiO3, are

mixed with carbon materials [24 and 168-170].

In dielectric radar absorbing structures, E-glass fibres, carbon fibres, aramid

fibres, honeycomb structures, foams are used to ensure required mechanical strength to

polymer matrices (epoxy, polyester, PU, PF) with MWCNT, CB, graphene, RGO etc.

acting as absorbing materials [6, 17-18, 26, 90-92, 95-97, 108-114, 123 and 171-175].

2.3.1 Effect of weight percentage and thickness on absorption properties

In MWCNT based RAMs, the electrical conductivity, complex permittivity and

dielectric loss tangents values were directly proportional to the MWCNT weight

percentage with fixed thickness, whereas complex permeability was not varied much

[30-31, 162 and 176]. Similar trend was observed in RGO (2,4,10 wt%), CB(5-50 wt%)

and CNF(1-6 wt%) polymer composites and their reflection loss values increased with

increase in filler loading [151 and 163-166]. The frequency of maximum RL depends

both on the weight percentage and thickness of the sample. Better reflection loss values

of dielectric RAM can be obtained by tuning the thickness at a given weight percentage

of the filler [36 and 163]. The relation between the thickness and the frequency to get

maximum reflection loss is given by the quarter wavelength matching theory.

According to this theory, by increasing the thickness of the composite, the reflection

peak has to move toward the lower frequency range. The absorption peaks of

MWCNT/epoxy (1-5 mm), CNF/epoxy (1-3 mm), CB/PU (2-4 mm) composites shifts

to lower frequency by increasing the thickness values [36, 126, 161 and 163].

The maximum filler loadings of 2.5 wt% of graphene/E-glass/PU and 4.1 wt%

of RGO/silica textile/PF radar absorbing materials resulted in maximim RL of -35 dB

and -36 dB at 12.1 GHz frequency [92 and 123]. The optimum RL of E-glass /epoxy

51
composites with CB, CNF and MWCNT were obtained by varying their weight

percentages [91 and 109-111]. The studies conducted on epoxy composites with

graphene (0.5-2.5 wt%), MWCNT grown CF(0.5-3 wt%) resulted in structurally strong

EMI shielding materials at 2.5 and 3 wt%, respectively [6 and 171]. The research works

[96, 123 and 172] studied, the effect of thickness of MWCNT/E-glass, graphene/silica

textile polymer composites to get maximum RL in the X-band.

2.3.2 Effect of multilayer design on absorption properties

The multilayer designs were succeeded in the enhancement of absorption value

and broadening of the frequency range due to the possibility of tailoring the properties

of layers [2, 34, 37 and 177-180]. The seven-layered MWCNT-PMMA, four-layered

graphite+MWCNT, three-layered graphene epoxy composites were reported as better

EMI absorbing materials due to the multiple internal reflections and the absorptions in

their stacked layers [35, 165, 177 and 179]. The double-layered coatings of SiC/Cu,

graphene/epoxy, CNT+graphite/epoxy composites shown maximum reflection loss and

wider bandwidths due to the design based on impedance matching condition compared

to their single layered absorbers [2, 178 and 180].

In fibre reinforced RAM also double layer composites were better compared to

their single layer structures [110-111 and 172-173]. Honeycomb cores with MWCNT

prepregs were designed to achieve -10 dB broad bandwidth in the frequency range of

0-20 GHz [95 and 174]. In the foam (PMI, PVC, PU) based RAS, face sheets composed

of nanofillers (MWCNT, CB, graphene) are utilized to prepare efficient absorber of

sand witch structure [18, 90, 96-97 and 114]. Compared to honeycomb and sandwich

structures, E-glass or CF reinforced multi layered structures are beneficial for the fine

thickness design of microwave absorbers. The fibre reinforced multi layered RAM

52
performance was influenced by the individual layer arrangement, thickness and the

amount of filler content. These effects were studied in epoxy-based graphene, CB,

MWCNT composites [26, 108, 112-113 and 175]. Table 2.1 gives the results extracted

from some published papers in literature. From the above table, it is summarized that

dielectric materials are mostly used in weight percentages from 0.1 to 25 to get the 90%

absorption for 2 – 5 GHz bandwidths. These materials can be used to prepare the light

weight microwave absorbers due to their lesser densities.

2.3.3 Gaps identified in literature

 Very few research works focused on the effect of angle of incidence on dielectric

RAMs absorption properties.

 Limited reports are available on the influence of size and geometry of dielectric

materials on the microwave absorption properties.

 Few research works are focused on effect of weight percentages and thickness on

Dielectric RAMs having thickness less than 1mm.

 Most of the works on dielectric RAMs shown bandwidths from 2-5 GHz only.

Very few researchers achieved -10 dB for more than 5 GHz frequency bandwidths.

 Limited research is available on microwave absorbing properties of double

layered E-glass /epoxy/MWCNT nanocomposites.

53
 Table 2.1 Details of M.A properties of dielectric RAMs
Thickness
Filler (mm) & Maximum
S. No. Ref. Filler/Matrix loading Bandwidth RL (dB) Application
(wt%) (GHz) for @ GHz
10 dB RL
RCS
reduction of
1 [151] RGO/NBR 10 3 4.5 -57 @9.6
airborne
systems
Microwave
2 [48] Graphene/TPU 10 2 0.5 -13 @10.5 absorbing
material
microwave
3 [163] CNF/epoxy 4 4 1.8 -25 @18.8 absorbing
material
Structural
material for
MWCNT- -47.2
4 [168] 25 2.2 2 aeroplanes
SiC/paraffin @10.5
and
spacecrafts
In the field
La (NO3)3- -27 @ of
5 [24] 6 2 5
MWCNT/PVC 13.5 microwave
absorption
Microwave
6 [30] MWCNT/epoxy 8 3 5 -18 @ 17 technology
applications
practical
RGO/silica -36 @ microwave
7 [123] 4.1 4 4.2
textile/PF 12.1 absorption
applications
CB, MWCNT, CB-8, RAS
8 [97] PU foam, MWCNT- 9.9 3 -20@ 9.7 sandwich
CF/epoxy 5 structures
CB/rubber +
CB-30, Stealth
9 [175] CF/epoxy 3 6 -30 @10
CF-60 technology
light-weight
MWCNT/E- -44 @
10 [112] 0,1,1.5,2.5 8 4.2 microwave
glass/epoxy, 11.5
absorber

2.4 Magnetic materials for Radar absorption

In magnetic radar absorbing materials, due to the controllability of EM

properties, ferrites, magnetic metallic materials and alloys are widely used.Ferrites are

54
suitable for microwave absorbing materials due to their high permeability, resistivity,

flexibility in the modification of magnetic properties and ease of preparation [40-41,

60, 88, 156 and 181-190]. For tuning of the microwave absorption properties of ferrites,

in the previous studies, the addition of dopants and change in their composition,

changes in the loading of the filler, variation in the thickness of the composites and

multilayer design usage were the methods utilized. The matching between permittivity

and permeability can improve the attenuation characteristics and achieved by the

doping of zinc, titanium, zirconium, manganese, copper and cobalt in different ferrites

[40-41, 88, 156 and 181-185].

In the magnetic transition alloys, properties like ferromagnetic loss, eddy

current loss and dielectric loss are favourable to microwave absorption properties and

they dependent on particle size, microstructure and morphology. The advantage of

magnetic alloys (NiCo, FeNi, FeCoNi) compared to single element metals (Fe, Co, Ni)

is the possibility of balancing of the EM properties by adjusting the components of

alloys and their microstructure [38-39 and 191-194]. The carbonyl iron is one of the

important magnetic material used in RAMs due to its high saturation magnetization,

permeability, low conductivity and high stability in air compared to other magnetic

materials [195-197].

In magnetic RASs, e-glass fibres and honeycomb structures were magnetically

coated without using any carbon materials to act as multi-functional composite

structures with simultaneous functions of microwave absorption and load bearing [15-

16, 23, 129, 157 and 198]. Nickel coated glass fabric epoxy composites are used to

fabricate the wing air foil models [16 and 129]. The radar absorbing structures with

magnetic and conductive materials coated on glass fabric have significant potential

55
applications in lightning strike applications and low observable technology [15, 23, 157

and 198].

2.4.1 Effect of weight percentage on absorption properties

The influence of filler content of the magnetic RAMs on the complex

permittivity and complex permeability was studied as it brings significant changes in

the microwave absorption properties [153, 186-187, 196, 199 and 200-204]. An

increase in volume fraction of carbonyl iron, MZF, NZF, LiZF in polymer composites

shifted the reflection loss peak towards the lower frequency [153, 196, 199 and 200-

201]. The maximum loading of 120 phr of nickel ferrite and 45 phr of cobalt ferrite in

rubber matrices has shown remarkable enhancements in the absorption properties due

to a raise in the complex permittivity and permeability values [186-187]. The studies

on the variation of weight percentages for investigating M.A properties of cobalt (5-30

wt%), carbonyl iron (50-75 wt%), BaHF (50-80 wt%) composites resulted in the

maximum reflection loss values at 30 wt%, 55 wt%, 80 wt% of the fillers respectively

[202-204].

2.4.2 Effect of thickness on absorption properties

Microwave absorber has to satisfy the impedance matching condition to get the

maximum reflection loss i.e., the impedance at the air absorber interface must be equal

to the impedance of the free space. This condition will be satisfied at a particular

thickness and frequency [186, 199, 200, 202 and 204]. To determine this matching

thickness and matching frequency, change in the reflection loss values w.r.t frequency

have to be evaluated by varying the thickness of the composites [39, 191-192 and 205-

206]. The thickness of Ni ferrite (1-14 mm), MZF (1-8 mm), CI (2-8mm) and cobalt

(1-11 mm) composites varied to find the maximum reflection loss and obtained at 12

mm, 3 mm, 2 mm and 10 mm thickness of the composites respectively [186, 199, 200

56
and 202]. The changes in the thickness of magnetic RAMs of many studies were in

accordance with the quarter wavelength matching theory [39, 60, 188-189, 191-192 and

204-206].

2.4.3 Effect of multilayer design on absorption properties

Without increasing the filler content, another method to achieve the broadband

and maximum reflection loss at a smaller thickness of the absorber was to use double

layered design [60, 188-190 and 207-211]. The first layer was designed to match the

impedance condition and the second layer was the absorbing layer. The NF/ NZF,

NiO/CONiZnF, CoTi doped BaF, ZnCo doped BaF double layered coating has shown

a remarkable increase in the reflection loss and bandwidths at a lower thickness than

their single layer absorbers [60 and 188-190]. In the multilayer design also the

maximum reflection loss occurs at a particular thickness of the matching and absorption

layers in a given frequency range [207-209]. The FeCoNi/SrF-NZF, BaF-Fe/Fe

composites layers thicknesses were varied from 0.3-1.7 mm in 2-18GHz frequency

range and obtained RL of -70 dB and -47 dB at a total thickness of 3 mm and 2 mm

respectively [210-211].

The honeycomb sandwich structures with metal magnetic particles (FeCo, rare

earth Tb) and nickel coated glass fibres exhibited good RL due to the multiple internal

reflections and absorption provided by the fillers [157-198]. The multi layered (five,

three, two layers) Ni coated glass fibres/epoxy composites revealed as efficient fibre

reinforced RAM to reduce the RCS with a low weight percentage of the filler (<10

wt%) and thickness less than 4 mm [15-16, 23 and 129].The results of some papers

were presented in Table 2.2. Its details are summarized as the magnetic materials weight

percentages in RAMs are not less than 50 wt%. These materials have the advantage that

their EM properties can be tailored by adjusting the composition of their constituent

elements. Furthermore, even though magnetic materials have higher densities than

dielectric materials, thinner microwave absorbers can be made.

57
 2.4.4 Gaps identified in literature
 Very few researchers focused on the effect of ferrites weight percentages on their

EM properties.

 Limited research is available on magnetic RAMs using less than 30 wt% of the

filler, which can produce lightweight and low-cost RAMs.

 The research presented on effect of thickness of magnetic RAMs on absorption

properties is limited

 Few research works are available on microwave absorbing properties of multi-

layered E-glass/epoxy/NZF nanocomposites.

Table 2.2 Details of M.A properties of magnetic RAMs

S.No. Ref. Filler/Matrix Filler Thickness Maximum Application

loading (mm) & RL (dB) @
(wt%) Bandwidth GHz
(GHz) for 10
dB RL
1 [183] CoFe2-2xZrMnxO4 100 7 500 -25 @ 1.8 EMI/EMC
(x=0.1-0.4) MHz for applications
x=0.3
2 [205] BaFe12- 86 2.1 7.68 for -60.6 @ EM shielding
2xNixZrxO19 x=0.6 15.9 devices
(x=0-0.8)/PVA
3 [153] LiZnTi 45 6.1 1.323 -52.9 @ 3 Microwave
ferrite/PVC absorber
4 [60] NF-NZF/epoxy 90 1.72 4 -45 @ 9.5 Stealth
technology
5 [192] Fe0.5Ni0.5/paraffin 50 2.5 1 -40 @ 1.1 Thinner
microwave
absorber
6 [212] Fe0.64Ni0.36- 50 3.5 2 -24.8 @ 14 Highly
NiFe2O4/paraffin efficient
microwave
absorber
7 [194] FeCo-B/paraffin 50 2 7.4 -29.3 @ Microwave
13.2 absorber
8 [197] Carbonyl 72 1.5 6.8 -27.5 @ Broad band
iron/PDMS 14.6 microwave
absorber
9 [23] Ni, Ni-4.95, 3.3 11.7 -69 @ 16.3 Low
Co/E-glass/ Co-47.55 observable
epoxy technology
10 [198] Ni/E-glass/epoxy Ni-7.51 9 10.5 -38.1 @ 8.2 Stealth
with honeycomb aircrafts
structure

58
2.5 Hybrid materials for Radar absorption

For the practical application of RAMs, they are designed based on low weight,

cost and thickness, maximum reflection loss and wide bandwidth. In order to meet these

requirements, the single materials (dielectric or magnetic) are not sufficient due to lack

of impedance matching condition and attenuation constant [61 and 213-220]. The

dielectric carbon-based materials (MWCNT, reduced graphene oxide, graphene, carbon

black and carbon fibre) combined with magnetic materials (metals, alloys and ferrites)

in different polymers (epoxy, paraffin, polystyrene and TPU) are the preferred hybrid

composites for a highly efficient microwave absorber [49, 50, 61, 63, 81, 152, 213-216,

218 and 220-225]. This is due to the synergistic effects of, high electrical conductivity,

notable dielectric loss, high specific strength, high chemical stability, lightweight of

carbon-based materials and high permeability, magnetic loss of magnetic materials,

which augment the microwave absorption. Other than carbon materials, Ti, TiO2,

PbZrTiO2, dielectric materials combined with magnetic materials were also used as

hybrid radar absorbing materials [84 and 226-228].

In order to secure the environmental resistance and strength characteristics,

hybrid fillers are reinforced by E-glass, carbon fibres and honeycomb sandwich

structures in polymer matrices [4, 9, 23, 93-94 and 229-230]. The enhancements in

permittivity and permeability and the corresponding reflection losses in hybrid RAMs

were studied by the amalgamation of different dielectric and magnetic materials,

variation in the filler loadings, variation in thickness of the composites and the multi

layered design.

59
2.5.1 Effect of weight percentages on absorption properties

The addition of magnetic metals, alloys and ferrites to MWCNT, Graphene,

carbon black and the variation in corresponding filler loading enhances the complex

permittivity and permeability of the composites depending on the type of the filler

added. Especially the imaginary values of complex permittivity and permeability,

representing the dielectric and magnetic loss characteristics, should be more than zero.

[5, 23, 50, 61, 82, 213-223 and 231-234]. The inherent property of magnetic materials

i.e. magnetic loss plays a significant role in microwave attenuation. The transition

metals Fe, Co, Ni [50, 81, 213 and 221-222] and alloys FeCo, FeNi [214 and 223]

coated or filled with MWCNT imparts the ferromagnetic nature to the composites,

which induces the magnetic loss to the dielectric MWCNT.The changes in weight

percentages of Ni@MWCNT in polystyrene, MWCNT in Co-C/paraffin, MnCoTi-BaF

in epoxy, N doped MWCNT-COZnF in paraffin NiZnF/MWCNT in rubber and epoxy

matrices has shown significant changes in their reflection loss values [49, 63 and 213-

216].

The blending of magnetic materials with graphene and reduced graphene oxide

has advantages of enhancement of electromagnetic losses at fine thicknesses and low

weight percentages of the composites [152, 220 and 224]. The variation in loading of

reduced graphene oxide from 5 to 60 wt% in NZF/RGO, NZCoF/RGO Paraffin

composites suggested that the optimal reflection loss can be attained at a particular

weight percentage where the proper matching of the dielectric and magnetic losses

occurs [61, 218 and 225]. The optimum filler loading of vertically arranged Fe coated

CF/epoxy radar absorbing structures resulted in maximum RL of -16.2 dB@ 6.1 GHz,

-26.8 dB @ 4.9 GHz owing to the appropriate conductivity, interface polarization and

microwave’s multi reflection inside the structure [9 and 93].

60
2.5.2 Effect of thickness on absorption properties

By varying the thickness of the composite, the reflection loss can reach to a

maximum value and the reflection peak values shifts towards lower frequency if it

complies with quarter wavelength matching theory. The attenuation of the incident

wave reaches to a maximum value due to the effect of phase cancellation [61, 81-82,

87, 152, 213-214, 216-220, 222-225, 231-237 and 238-241]. In the literature, studies

were conducted on the changes in reflection loss values of magnetic MWCNT by

varying the thickness of the composites from 1-10 mm [62, 81-82, 213-214, 216, 222-

223 and 235-236]. The increase in thickness of Fe, Ni, FeCo, FeNi-MWCNT, NiZnF-

MWCNT hybrid composites resulted in the change in the reflection peak value towards

the lower frequency range [62, 81, 213 and 222-223]. Besides the quarter wavelength

matching theory, in the design of RAM, two conditions have to be ensured. One is

impedance matching condition and the other high attenuation constant value. These two

conditions were evaluated for the magnetic MWCNT RAMs of N doped Co-

C/MWCNT, zinc ferrite/MWCNT, COZnF/N doped MWCNT composites for the

maximum reflection loss [82, 214 and 216].

The thickness variation studies from 2-5 mm of the Fe3O4 and SiO2@NiO

graphene composites resulted in maximum reflection losses at 5 and 3 mm respectively

[224 and 239]. The substantial changes were occurred in the absorption frequency

ranges of RGO- Co-C,Fe3O4, NiZnCoF composites due to the thickness variation [217,

220 and 225]. When the normalized characteristic impedance value is equal to one, the

absorber gives the maximum reflection loss value at a particular thickness. The research

works [61, 218-219, 231 and 237] discussed the importance of normalized

characteristic impedance value with reference to the better performance of RGO based

magnetic materials.

61
2.5.3 Effect of multi-layer design on absorption properties

The implementation of the impedance matching condition and high attenuation

constant can be done effectively by using multilayer design in the hybrid absorbing

materials [51,149, 151 and 242-248]. Comparison studies were conducted in the past

literature to demonstrate the superiority of the double absorber over the single layers

absorbers [149, 244-245 and 247]. Either by the combination of the dielectric and

magnetic materials in each individual layer [243 and 247] or by using the dielectric or

magnetic materials separately in different layers of multi-layered absorbers, the

required reflection loss and bandwidths are gained with lower thickness values [51,

149, 242, 244-246 and 248].

The increase in weight percentage of SiO2, CI and CB in matching and absorber

layers in CI-CB composites and doping of CoTiMn in matching layer of

BaHF/CCB/TiO2 composites enhanced the bandwidths [242-243 and 248]. The

variation in the thickness of the first and second layers of NZF/CB, BaLaCoF/CF, FeNi-

C/MWCNT double layered composites influenced the absorption performance in terms

of increased maximum reflection loss and bandwidths [149 and 245-246].

The double layered E-glass and MWCNT reinforced FeNi, Co & MnF, Fe3O4,

CNF/NiFe epoxy composites with 4, 3.3, 1.8 mm and 3.43 mm thickness exhibited

excellent EM absorption properties [23, 94, 229 and 249]. The honeycomb sandwich

structures with CI, nickel fibres, titanium and carbon black, exhibited an RL of -10 dB

for broad bandwidth of 9 GHz, 15 GHz in the 2-18 GHz frequency range [4 and 230].

Results of some of the published papers of hybrid RAMs are shown in Table

2.3. It summarises that microwave absorbers with fine thickness can be made by

utilizing the weight percentages from 10 to 30 wt% of hybrid fillers. They exhibited 90

% absorption for 4-11 GHz bandwidths and 99% absorption at their respective

matching frequencies.

62
 Table 2.3 Details of M.A properties of hybrid RAMs

S.No. Ref. Filler/Matrix Filler Thickness Maximum Application

loading (mm) and RL(dB)
(wt%) bandwidth @GHz
(GHz) for
-10 dB RL
1 [223] FeCoC- 20 2 6.3 -79.2 @14 Microwave
MWCNT/paraffin absorber
2 [84] Fe3O4- 30 2 3.25 -42.53 @10.98 Microwave
TiO2@MWCNT/TPU absorber
3 [82] ZnCoF- 35 2.4 4.2 -79.08 @10.5 Promising
MWCNT/silicone microwave
rubber absorbing
material
4 [224] Fe3O4-graphene/wax 20 5 2 -40.36 @ 7.04 Lightweight
and strong
EM
attenuation
material
5 [217] Fe3O4@RGO/paraffin 15 2.7 6 -20.59@14.43 EM
absorber at
an industrial
scale
6 [61] NZF-N doped 40 2.91 5.4 -63.2 @ 8 High
RGO/paraffin efficient
microwave
absorber
7 [246] NZF-CB/epoxy 60- 2 4.8 -24 @13.9 Microwave
NZF,5- absorber
CB
8 [244] CoZnF-TiO2/epoxy 30- 2 4.2 -24.3 @12.02 Microwave
COZnF absorber
30-TiO2
9 [9] FeNP-CF/epoxy 30- 4.32 11 -26.8 @ 4.9 Excellent
Fe,5.52 - RAS
CF
10 [4] CB,CI/epoxy HSS 30- 9 13.1 -27 @ 14 Lightweight
CB,70- and efficient
CI broad band
microwave
absorber

63
2.5.4 Gaps identified in literature

 In hybrid RAMs, the combination of MWCNT with NZF could be an effective

method to enhance the absorption performance of MWCNT. But limited

research work is focused on MWCNT/nickel zinc ferrite RAMs.

 Very few research works are available on effect of weight percentages and

thickness on hybrid RAMs having thickness less than 1mm.

 Research work presented is limited on utilization of hybrid materials for double

layered RAMs regardless of their advantages.

 The E-glass reinforced single layered or multi-layered MWCNT/NZF radar

absorbing materials EMW absorption properties were focussed by few

researchers.

2.6 Synthesis of NZF by Sol-gel auto combustion method

The microstructural and magnetic properties of magnetic RAMs in the high

frequency range directly relies on the synthesis process. So it is pivotal to select the

right method of synthesis to attain the required properties of absorbing materials. The

sol-gel auto combustion technique was a more suitable method to prepare nano ferrites

compared to other methods like high energy ball milling, hydrothermal, solid state

reaction, co precipitation. This is due to the attributes like better control over the

composition, easy availability of raw materials, low processing time and low cost [65

and 250-252].

64
2.6.1 Effect of fuel agents and heat treatment on ferrites properties

The crystallite size, nature of agglomeration, surface area, magnetic properties

etc., are governed by the nature of fuels used in the combustion process [253-259].

The fuel agents like PVA, PEG, hydrazine, citric acid, acetic acid, carbamide,

carbohydrazide were utilized for the comparative analysis on the properties of ferrites

[253-260]. The studies conducted on the synthesis of ferrites using urea and glycine

revealed that the ferrites particles were having less crystallite size and larger surface

area when urea was the complexing agent [254-255, 257, 260].

The microstructural and magnetic properties of ferrites prepared by sol-gel were

also prominently influenced by the calcination temperatures (2000C to 9000C) [64, 72

and 261-265]. These temperatures raise caused the shift in high and low frequency

bands corresponding to tetrahedral and octahedral units of nickel zinc ferrites [72, 262

and 264] and also led to increase in crystallinity, particle sizes and saturation

magnetization values [64, 261, 263 and 265].

2.6.2 Doping of elements in ferrites by sol-gel

Researchers extensively investigated the doping of ferrites by the sol-gel

method to make them suitable for diverse applications as this method is more precise

to control the required composition of doped ferrites. Grain size, structure, cations

distributions among the crystal lattice sites, porosity are the factors affecting the

microstructural, optical, electrical and magnetic properties of the ferrites [251 and 266-

274]. The cobalt ferrites were doped by Na, Ni, Bi and Mg to vary electrical and

magnetic properties, which are correlated to changes in the microstructural,

morphological and optical properties [251 and 266-268]. Mn+2 doped magnesium silver

ferrites and zinc ferrites displayed an increase in lattice parameter and saturation

65
magnetization values to equip them for electromagnet and photocatalyst applications

[269-270]. The substitution of Zn, Co, Cr, Mg imparted the required crystal structure,

crystallite size, morphology, saturation magnetization, coercivity, resistivity, initial

permeability in nickel, copper, cobalt zinc ferrites [271-274]. All the doped ferrites

synthesized by sol-gel method have shown no impurity or secondary phase in the

composition.

2.6.3 Microwave Absorption properties of ferrites prepared by sol-gel

The preparation of ferrites by sol-gel method and their microstructural,

magnetic and dielectric properties were studied to utilize as microwave absorbers in a

selected frequency range [60, 181-182, 184-185, 244-245, 265 and 275-276]. The effect

of doping of Zn, Mn, Mg, Ti, Co, Cu, La in various ferrites and varying their

composition have shown significant effects on dielectric properties [181-182, 184 and

275-276]. The zinc doped NZF and Ti doped LiZF composites exhibited RL of -17.54

dB (3.5 mm),-18.87 dB (5 mm) at 9.62 GHz and 3.5 GHz, respectively [181-182]. The

annealing temperature in sol-gel method has a significant effect on the crystallite size

in turn on magnetic and microwave absorption properties. The maximum reflection loss

and bandwidths of the doped nickel zinc ferrites polymer composites were better when

annealing at 5000C and 8500C temperatures because of the enhanced magnetic

properties at those particular temperatures [185 and 265]. The double layered

microwave absorbers prepared with NZF, CoMnNZF and BaCoLaF shown better

microwave absorption in the X-band due to impedance matching condition and

morphology, crystallite size and porosity of ferrites prepared by sol-gel method [60 and

244-245].

66
2.6.4 Gaps identified in literature

 Limited reports are available on the usage of urea as a fuel agent in the sol-gel

synthesis of ferrites.

 Research works focussed on the effect of doping Co, Zn etc. elements in different

compositions in nickel ferrites to study the changes in electromagnetic properties

are limited.

 Microwave absorption properties are enhanced by changing the annealing

temperature of ferrites. But the effect of annealing temperatures on microwave

absorption properties of ferrites is not analysed well.

 The synthesis of ferrites by sol-gel method and utilization as microwave absorber

in high frequency range can produce low cost and efficient RAM. Even so, few

researchers focused on this.

2.7 Fabrication of fibre reinforced Radar Absorbing materials

In the preparation of polymer-based fibre reinforced RAMs, hand layup method

with combination of either autoclave or compression molding is most commonly used

fabrication method compared to the RTM and VARTM methods [9, 15-16, 23, 25, 90-

97, 108, 110, 112-114, 129, 198, 229 and 277]. In these methods, the reinforcing

elements were coated with polymer resin solution with absorbing materials. Then the

samples were cured under specified conditions of temperature and pressure, given by

the polymer manufacturer. The polymer-based fibre reinforced RAM curing can be

done in either room temperature [26, 92, 111 and 114] or high-temperature conditions

(80-1300C) [18, 25, 90-91, 95-97, 108-110, 112, 123 and 174] and at vacuum [92 and

174-175] or at high pressures (3-8 atm) [18, 25, 90-91, 95-97, 108-111, 113, 172 and

67
277]. The RAM cured high temperature has greater thermal stability, chemical stability,

mechanical properties and environmental resistance. The research works [172 and 278]

implemented the flexible designs of RAM by varying the curing pressure of the

composites during the fabrication process. This method was used to overcome the

limitations of controlling the EM properties by increasing the filler loading and

thickness of composites.

2.7.1 Preparation of pre mixture in fibre reinforced RAMs fabrication

Proper dispersion of nanomaterials in the polymer resin is the major challenge

in RAMs preparation as it significantly alters the electrical and magnetic properties. In

the preparation of fibre reinforced RAMs, to ensure good dispersion, the solution

containing calculated amounts of polymer resin and absorbing materials was prepared

using physical methods like sonication or mechanical mixing methods [6, 26, 90-93,

96, 111, 113 and 157]. Instead of directly mixing the lossy materials like CB, FeCO

etc. to the epoxy resin, initial mixing with acetone reduces the agglomerations

formation [111 and 157]. The ultrasonic oscillations were used to ensure the uniform

dispersion of MWCNT, graphene, Fe nanoparticles in polymer matrices [6, 26, 92, 93

and 113]. The 3-roll mixers and magnetic stirrers with hot plates rotating at 500 -800

rpm were used to facilitate the uniform mixing and reduction of viscosity during the

coating of pre mixture to E-glass fabrics [90-91 and 96].

Along with the above mentioned physical methods for uniform dispersion

ability, chemical methods of surface modification were also utilized. The acid

(H2SO4:HNO3::3:1) treated MWCNT and silane coupling agent(KH-550) coated Fe

nanoparticles resulted in uniform dispersion and consequently produced efficient fibre

reinforced RAM [9, 93-94 and 112]. Recently, a new technique was adopted in the

68
literature to overcome the difficulty of uniform dispersion of absorbing fillers in the

polymer matrices. In this method E-glass, honey comb structures were coated with Ni

and Co using electroless plating, sputtering method and succeeded in the development

of lightweight RAS with wide bandwidths of 10 GHz for -10 dB of RL [15, 16, 23, 129

and 198].

2.7.2 Temperatures and pressures in fabrication process

The reinforcing elements were coated with premixture and further subjected to

required pressure and temperature during the curing process. The CB,MWCNT, CNF,

FeNi based RAM were fabricated using autoclave with maximum temperature and

pressure of 1300C and 6 atm [25, 97 and 108-111]. The Fe/CNF, NiFe/MWCNT/E-

glass/epoxy composites were kept in the hot air oven at 1240C for 12 hr and 1800C for

3hr of post curing process [9 and 93-94]. The Ni coated E-glass/epoxy RAM were

manufactured by curing cycle of 30 min at 800C & 7 atm followed by 120 min at 1300C

&10 atm pressure for high strength applications in aerospace [15, 23, 129 and 198].

The pressure needed for compaction of the stacked plies in composite laminates

was also applied by heavy weights or a hydraulic press [ 6, 26, 92, 94, 112, 157, 171,

175 and 230]. In the fabrication of sandwich RAS composed of honey comb and foam

structures, epoxy based adhesive films were used to bind the different layers consisting

of absorbing fillers. Further, autoclave was utilized to implement the curing cycles with

specified temperatures, pressures and duration [4, 18, 90, 95-97, 174 and 198].

2.7.3 Gaps identified in the literature

 Enhanced microwave absorption is possible by uniform dispersion and the greater

bonding of nanomaterials with the matrix material. Limited researchers focused

69
 on the surface modification of nanomaterials utilized to fabricate fibre reinforced

RAMs.

 In the fabrication methods of fibre reinforced RAMs, few research works are

available on using the techniques like electroless plating, sputtering methods,

which can avoid the issue of agglomeration of lossy fillers.

 Very few research works are conducted on the enhancement of microwave

absorbing properties of dielectric RAMs without increasing the filler content by

changing the curing pressure of the composites.

2.8 Evaluation of Thermal and Mechanical properties of RAMs

In all practical circumstances, the radar absorbing materials have to satisfy both

functional and structural requirements. To ensure the RAM’s capability to resist the

deformation under stress and environmental endurance, their mechanical properties and

thermal properties were investigated along with their broadband absorbing capacity in

ref [9, 31 and 122-123]. The DMA analysis is used to determine the thermomechanical

response of RAM used in specific applications like missiles and aircrafts [31, 128, 130-

131 and 279-280]. Thermal degradation and fire resistance of radar absorbing materials

were determined by TG and DTG/DT analysis by varying the temperature from room

temperature to maximum of 12000C in presence of nitrogen or air [9, 47, 84, 87, 89,

122-126, 128, 131, 168, 216, 202, 225 and 281-288] . TGA can probe the thermal

stability and the filler percentage, purity of components, defects presented and effect of

reinforcements on the thermal stability of microwave absorbing materials.

70
2.8.1 Thermal properties of RAMs

The defective CNTs exhibiting high permittivity in the X-band and CNTs with

different helicities were synthesized and their defects and purity were characterized by

remnant obtained from TGA curves [281-282]. The CB/PU and cobalt ferrite-

PACB/paraffin composites displayed their weight loss in various continuous steps up

to 7000C due to multiple decompositions of the components [87 and 126]. The

microwave absorption properties of composites largely depend on the weight

percentage of absorbing fillers; therefore the thermal stability of composites with

different weight percentages were compared based on their degradation temperatures

like IDT(initial degradation temperature), Tmax (temperature at maximum mass loss

rate), FDT (final degradation temperature) [9, 47, 128 and 283-284].

The TGA was also used to determine the relative amounts of the fillers in hybrid

radar absorbing materials. In the porous SiC@MWCNT, barium ferrite@C, cobalt

ferrite@C, CoZF@NMWCNT, Fe@MWCNT microwave absorbing composites, the

relative amounts of SiC, carbon, NMWCNT and Fe were determined by performing

TGA in air from room temp. to 8000C at a heating rate of 100C /min [89, 125, 168, 216

and 285]. The effect of the addition of lossy fillers on MA properties and thermal

stability of polymer composites were studied in ref [84, 123-124,128 and 286-287]. The

enhancement in the thermal stability was reported due to the nature of filler and better

interaction between components of the composites. The weight percentages and ratios

of the components in MWCNT/epoxy, NZCoF@RGO/ paraffin,

PANI@Fe3O4/paraffin, cobalt/polyster composites were obtained by the residual

weights at 6000C of their TGA curves [122, 202, 225 and 288]. In radar absorbing

structures reinforced with silica textile, carbon fibres and composed of MWCNT, RGO

and Fe nano particles, the TGA was used to determine the percentage of filler and its

71
effect on thermal stability and degradation temperatures [9 and 122-123]. All these

structures exhibited thermal stability of greater than 3000C with 99 wt%.

2.8.2 Mechanical properties of RAMs

The study of mechanical properties of radar absorbing materials is necessary to

resist the damage from environmental influence and in service loading conditions. The

tensile, flexural properties (Young’s modulus, tensile strength, elastic deformation,

flexural modulus, flexural strength and strain) are the most studied mechanical

properties of microwave absorbing materials [9, 24, 47, 91, 93, 122-123, 127-128, 147,

177, 202-203, 232, 280 and 289]. These properties decide the suitability of the materials

in practical applications of EMI shielding and stealth technology. These characteristics

were tested according to standards ASTM D3039 and ASTM D790 and values are

obtained from stress - strain curves of the composites [24, 127-128 and 147]. Due to

the high aspect ratio of MWCNT and their homogeneous dispersion in polymer

matrices of epoxy, PPCP and PMMA, higher tensile strength and Young’s modulus

were obtained compared to their unfilled composites [47, 91, 122 and 177]. The

addition of fillers like reduced graphene oxide, carbon black, strontium ferrite,

manganese zinc ferrite, carbonyl iron, cobalt, lanthanum oxide and samarium oxide

enhanced the tensile properties of nanocomposites proportional to their weight

percentages [123, 202-203, 232, 280 and 289]. On the other hand, reduction in tensile

properties was observed due to non-homogeneous dispersion of fillers in

lanthanum/PVC and RGO-Fe2O3/epoxy composites [24 and 128].

The radar absorbing structures with Fe nanoparticles/CF/epoxy exhibited the

greater flexural strength of 102 MPa compared to MWCNT/PMMA (64 MPa),CO/PS

(75 MPa), Zno/wood fibre/polyethylene (43 MPa) polymer composites [9, 93, 177 and

72
202]. The shear strength, shear modulus, impact strength and hardness of the EM wave

absorbing composites are also important properties to be considered for their utility in

the real world [25, 128, 202-203, 289 and 290]. Recently to investigate the nickel coated

E-glass fibre reinforced RAMs, load bearing efficiency, effect of light striking

conditions, flatwise and residual compressive tests were conducted [15 and 198].

Different fibres like carbon, E-glass, aramid fibres are coated with nano absorbing

fillers during the fabrication of radar absorbing structures. The determination of peel

strength, lap shear strength and adhesive power of RAM is significant as they ensure

the functional requirements of MAMs without any failure like delamination during their

service [90, 129, 203 and 279].

The viscoelastic nature characterizes the processing and useful properties of

polymer composites [31, 128, 130-131 and 279-280]. The DMA (dynamic mechanical

analyser) is used to investigate the viscoelastic nature by determining the storage

modulus, loss modulus and glass transition temperature and conducted at different

temperature ranges (-800C to 3000C), frequencies(1 Hz-5 Hz) and amplitudes of the

applied loads [128 and 130]. The ability to store the energy (storage modulus) and glass

transition temperature (tan∆) were enhanced due to the improved interface between

fillers and polymer, stress transfer between the interface layers and resistance provided

by the fillers like CNT to the movement of molecular chains of polymers [31, 131 and

279-280]. Recently, the elastic moduli of cobalt sulphide, SiC/PVDF (polyvinylidene

fluoride) radar absorbing composites were simulated using finite element based

softwares ANSYS and COMSOL. Further verified experimentally that the addition of

the above fillers enhanced their absorption properties and mechanical properties [127

and 147].

73
2.8.3 Gaps identified in the literature

 Limited research is available on thermal properties of fibre reinforced RAMs. A

few research reports analysed the TGA of E-glass/Epoxy/NZF and E-

glass/Epoxy/ MWCNT/NZF composites.

 Very few researchers focused on mechanical properties evaluation of fibre

reinforced RAMs despite of their importance in load bearing capabilities. The

mechanical properties of E-glass/Epoxy/MWCNT/NZF radar absorbing

materials are not well analysed.

 For radar absorbing materials, research work presented on dynamic mechanical

analysis (DMA) is limited.

 Few simulation studies conducted in the literature for determination of

mechanical properties of RAMs.

2.9 Multi Criterion Decision Making (MCDM) Methods

Decision making (DM) activity is an integral and vital part of every research as

it aids in ranking the possible alternatives depending on the decision makers tendencies

with relevance to a given set of criteria [134, 137, 145 and 291]. Multi criteria decision

making (MCDM) is the well-known tool that helps the DM process by analysing the

set of options formulated on multi conflicting criteria transparently and explicitly [133,

142 and 292-293]. Some of the popular methods employed for solving MCDM

problems in the literature were AHP, ANN, ANP, ASHBY, BWM, COPRAS, CRITIC,

DEA, DEMATEL, ELECTRE, GRA, GC, MAUA, MOORA, PROMETHEE II, SAW,

TOPSIS, VIKOR, WPM and WSM [135, 294-297]. These techniques were used in

ranking the alternatives in the area of process selection, system selection, supplier

74
selection, personnel selection, technology selection and materials selection [133, 137,

141 and 298-301].

The AHP method was developed by Saaty and laid the foundation for MCDM

methods, which determines the ranking of alternatives from the matrix of comparison

and values of weight criteria i.e., relative importance of each criterion [137, 298 and

301-303]. The AHP is not suitable in case of a large number of alternatives and criteria

because more comparisons are required. The TOPSIS method is the second most widely

utilized method, which gives preferential rankings in terms of a numerical value to

make it easy to understand, but it doesn’t provide any criteria weights and consistency

check [135-136, 296-297 and 304-306]. The methods of hybridization, fuzzification

and modification of MCDM were introduced to reduce the uncertainty and

disadvantages (lack of correlation between criteria, need of separate tools for

calculation of criteria weights, applicable to same type of criteria etc.) associated with

usage of each AHP, TOPSIS,WSM and VIKOR etc. approaches [3, 132, 138-145, 158,

291-295, 299-300 and 307-313]. In hybridization, the combination of MCDM methods

TOPSIS, VIKOR, PROMETHEE, GRA with either subjective or objective weight

(entropy, CRITIC) criteria methods or with combined weight criteria methods were

considered [3, 138-142, 145, 158, 291-295, 300 and 307-309]. Bellman and Zadesh

started using fuzzy MCDM techniques to aid linguistic variables to be described

suitably since natural language is usually employed for the articulation of thinking and

evaluation and enhanced the quality of decision making [143, 299 and 310-311].

The modification of TOPSIS with double hierarchy (DH), grey correlation(GC)

techniques and VIKOR with interval numbers, target based criteria and new

quantitative ranking index methods resulted in better choices compared to simple

MCDM methods [132, 144 and 321-313] . The suitability and applicability of different

75
MCDM methods were determined by their level of agreement using Spearman’s rank

correlation coefficient (varies from (+1 to -1) and Kendall’s coefficient of concordance

(varies from 0 to 1) [314-316].

2.9.1 Application of MCDM methods for material selection

The electromagnetic shielding materials with appropriate mechanical properties

were important for public health safety and stealth technology. They were selected from

number of alternatives using MCDM methods [3, 313 and 316]. Investigations were

carried out with AHP, entropy, TOPSIS and PSI techniques to select the composite

possessing suitable mechanical properties and physical properties for automotive and

aerospace applications [138-139, 292, 302-303, 305 and 309] . Along with mechanical

properties, water absorption properties were included in the conflicting criteria of

MCDM methods of natural fibre reinforced composites, as these properties were

significant for the structural integrity of underwater applications [158, 302, 304 and

308]. Moreover researchers are updating many MCDM methods for the prioritization

of materials for various applications like green materials for interior decoration, bio

medical equipment etc. for performance improvement and minimization of the cost

[142, 144-145, 291, 293-294, 296 and 312].

2.9.2 Gaps identified in the literature

 In MCDM methods, limited research is available on the usage of both subjective

and objective weightage methods for the material selection process.

 The research work presented is limited on the application of MCDM techniques

for the selection of EMW absorbing materials.

 Researchers less focused on evaluating the similarity of the ranks obtained from

different MCDM methods.

76
2.10 Numerical simulation of EM properties

The modern technology of EM simulation enables a better and clear

understanding of the response of electromagnetic components to the EM waves. With

the aid of EM simulation tools, design, analysis and optimization of radar absorbing

materials could be completed in a fast and accurate manner [1, 5-6, 16, 18, 23, 90-91,

95, 129, 146-150, 159-160, 167, 174, 198, 229 and 317-321].

Various commercial softwares including COMSOL Multi physics [1, 5, 6, 146-

147, 150, 159-160 and 317-318], ANSYS HFSS [148, 167 and 319], CST microwave

studio [4, 16, 18, 23, 90-91, 95, 129, 149, 174, 198, 229 and 320-321] are available for

the simulation of EM absorption properties of composite materials in the frequency

range of 0.5-50 GHz. The reflection loss values and shielding effectiveness were

obtained by entering the permittivity and permeability values determined from VNA as

input material parameters [1, 4-6, 16, 23, 95, 129, 147, 149, 150, 160, 167, 198 and

319-320]. But in some research reports, real and imaginary permittivity values of

dielectric microwave absorbing composites were estimated using EM simulation

softwares and they were validated also [95, 146 and 319]. In the research works

conducted by ref [8, 148, 159 and 317], the EM properties were taken from the previous

experimental works and determined the reflection loss and microwave attenuation

energy values.

2.10.1 Modelling in EM simulation

The numerical modelling of electromagnetic interference of various microwave

absorbers has been widely carried out using FEM based softwares like COMSOL and

HFSS. The composites with graphene, cobalt sulphide, carbonyl iron carbon black and

MWCNT were modelled including the geometry and material properties of the

77
composites [6, 147, 150, 159 and 317]. The S-parameters are obtained by imposing

suitable boundary conditions and solving the electromagnetic wave theory equations

for the computational domain. The effect of dielectric fillers like graphene

nanoplatelets, MWCNT in polymer composites on shielding effectiveness was obtained

in numerical simulations [5-6 and 321-322]. Recent studies modelled the geometries of

spherical inclusions, pores, carbon foams and cylindrical arrays successfully to

investigate their effect on the absorption properties [5, 146, 148 and 160]. The default

geometry tools in the simulation soft wares facilitate the modelling process. The EM

simulation promotes the parametric studies by changing the filler percentage, the

diameter of the pores, the thickness of the samples, radii and height of cylinders in

modelling of the absorber to get better absorption properties [1, 5, 146 and 148].

2.10.2 Analysis in EM simulation

The polymer based radar absorbing structures with dielectric [90-91, 95-96,

150, 174 and 322], magnetic [16, 23, 129, 198 and 320] and hybrid materials [4 and

229] are analysed to simulate their reflection loss and transmission loss values. Not

only the scattering parameters but the EM simulation tools also help to visualize the

distribution of EM energy density, microwave attenuation energy, power loss, electric

field contours with high quality graphics [1, 159-160 and 318]. This visualization

enables quick and clear identification of the performance of absorbing materials. In the

previous studies on EMW absorption numerical simulations, the results were

experimentally validated with free space measurement [5, 8, 18, 90-91, 96, 146, 148,

150, 167, 174, 198 and 317-318] and analytically with MATLAB code developed for

microwave absorption [23, 129 and 159]. In the numerical simulation of RAMs, virtual

prototype testing of various real world applications such as EMI shielding composite

78
wall, cylindrical dielectric resonator, wing box, wing airfoil model were accomplished

[16, 129, 148, 150 and 198].

2.10.3 Gaps identified in the literature

 Very few research reports are available on the usage of EM simulation software

to determine complex permittivity and permeability values.

 Limited literature is available on modelling of geometric entities like spherical

inclusions, foams, porous structures and their effect on microwave absorbing

properties using EM simulation tools.

 The studies on changes in EM absorption properties utilizing parametric

simulations were less focused.

 Few researchers focused on the simulation of real world applications of RAMs.

2.11 Shortcomings based on the Literature

 The research work on the influence of size and geometry of dielectric materials

on microwave absorption properties was limited. The studies conducted on the

effect of the aspect ratio of MWCNT on microwave absorption can develop

lightweight and high absorption RAMs.

 In dielectric RAMs, although the double layered E-glass/epoxy/MWCNT

nanocomposites result in thinner RAM compared to sandwich type structures,

few research works are available on them.

 Though urea usage as a fuel agent in the sol-gel synthesis of ferrites manifested

in larger surface area of the particles, which is beneficial for microwave

79
 absorption, limited research was presented on the usage of urea for the synthesis

of nano ferrites.

 In magnetic RAMs, few research works were carried out on the effect of weight

percentages of magnetic fillers on EM properties.

 Very few research reports are available on magnetic RAMs with less than 30

wt% of magnetic lossy filler. Research work focused on Multi-layered magnetic

RAMs was limited, especially multi-layered E-glass/epoxy/NZF

nanocomposites RAMs were not well analysed.

 As per the literature survey conducted on hybrid RAMs, double layered

absorbing RAMs with hybrid materials and especially the combination of

MWCNT with NZF were not analyzed well. The microwave absorption

properties of fibre reinforced multi-layered MWCNT/NZF RAMs were studied

limitedly.

 The Available literature on thermal properties of RAMs was limited despite their

importance in temperature resistance. The TGA of E-glass/Epoxy/NZF and E-

glass/Epoxy/ MWCNT/NZF composites was not studied well.

 The mechanical properties of E-glass/Epoxy/ MWCNT/NZF radar absorbing

materials were focussed limitedly even though they represent the load bearing

capabilities.

 From the literature on MCDM methods, issues like the usage of MCDM

techniques to select the best microwave absorbing material, subjective and

objective weightage methods for material selection, evaluation of similarity of

ranks for the application of various MCDM techniques were less focused.

80
  By using EM simulation tools, limited studies were conducted on the parametric

studies and real world component testing of RAMs or RASs. These studies

would lead to the efficient and practical applications of RAMs or RASs.

2.12 Objectives of the present work

Based on the shortcomings observed from the literature, following objectives were

defined for the present work

 Fabrication of the RAMs with two different aspect ratios of 115 and 315 of

MWCNT to study its effect on microwave absorbing properties.

 Exploration of the absorption properties of double layered E-

glass/epoxy/MWCNT RAMs with weight ratios of MWCNT from 0.4 to 2%,

having lesser thickness compared to sandwich structures.

 Synthesis of nano nickel zinc ferrite using urea as fuel agent by sol-gel auto

combustion method and review its microwave absorption properties in the X-

band.

 Analysis of the effect of weight percentages (10, 20 and 25 wt%) of NZF on EM

properties of E-glass/Epoxy/NZF nanocomposites.

 Estimation of the RL values of double layered E-glass/Epoxy/NZF

nanocomposites using less than 30 wt% of the NZF.

 Determination of the microwave absorption properties of double layered E-

glass/epoxy/MWCNT/NZF composites with 0.4-2 wt% of MWCNT and 20 wt%

of NZF.

 Evaluation of the thermal properties of E-glass/Epoxy/NZF and E-glass/Epoxy

MWCNT/NZF composites in the temperature range of 40-9500C.

81
  Investigation of the tensile strength, flexural strength, impact strength and

hardness of double layered E-glass/Epoxy/MWCNT/NZF radar absorbing

materials.

 Selection of RAM using TOPSIS, VIKOR and PROMETHEE II with combinative

weights and evaluate the Kendall’s coefficient to find the similarity between the

applied MCDM methods.

 EM simulation analysis for the design and parametric studies of geometric

elements arrayed RAS utilizing MWCNT/NZF nanocomposites

2.13 Summary

This chapter summarizes

1. The research works related to the theoretical background and applications of

RAMs and comprehensive studies of dielectric, magnetic and hybrid absorbers.

2. The past literature on the influence of weight percentages, doping of elements,

microwave absorption properties of ferrites prepared by sol gel method, various

methods used to control filler dispersion, and details of pressures and

temperatures used in the fabrication process of RAMs.

3. The previous investigations on the thermal and mechanical properties

evaluation, multicriteria decision making methods in the material selection

process and simulation studies of RAMs.

4. The gaps identified in all the studied literature topics, shortcomings of the earlier

research work and formulated the objectives of the present work.

82
Chapter 3 EXPERIMENTAL METHODS FOR
SYNTHESIS, FABRICATION AND
CHARACTERIZATION

3.1 Introduction:

Nowadays nanostructured magnetic materials gained significant attention

compared to the micro sized materials because of their exclusive magnetic and

electrical properties. The presence of a large number of atoms at the surface causes the

interfacial polarization which leads to high dielectric loss and microwave absorption

[60, 67 and 72]. Considering the influence of nanoscale on magnetic material

properties, it is always a real challenge for scientists and researchers to synthesize

materials with required stoichiometry, structure and properties [64 and 323].In order to

prepare the nanocrystalline NZF, sol-gel auto combustion method is simple and

effective synthesis method [65, 181-182, 251, 259-260, 267, 269 and 275-276]. The

procedure of sol-gel auto combustion method used to synthesize the nanocrystalline

NZF is described in this chapter.

The polymer-based radar absorbing materials prepared with hand layup method

resulted in good microwave absorption properties and mechanical properties if the

premixture ensures the uniform dispersion of the lossy fillers [6, 95-96, 112 and 122].

The room temperature cured RAMs are having less thermal stability and mechanical

strength compared to the the high temperature RAMs [9, 15, 93, 123 and 171]. In the

present work, Sonication and ball milling methods are utilized to get uniform dispersion

of MWCNT and NZF nano materials in the epoxy matrix. The MWCNT, NZF and

hybrid MWCNT and NZF RAMs are prepared with hand layup method using high

temperature polymerization and compression molding processes.

83
 An important step before utilizing the material for any purpose is its

characterization. It ensures that the considered material will function without failure for

the life of the end product. The characterization plays an important role in the

understanding structure-property correlation of any material. For the characterization

of nanomaterials, more than a single technique is needed to capture all the pertinent

characteristics of nanomaterial [79-80, 82, 182, 218, 220, 244 and 324-325]. Hence in

this chapter, various characterization techniques including XRD, SEM, EDX, TEM,

FTIR and VSM used to determine the microstructural, morphological, chemical and

magnetic properties of nanomaterials were described. The prepared RAM samples are

tested using VNA and TGA to get EM and thermal properties. The universal testing

machine, impact testing machine and Barcol hardness tester is used to determine the

some of the mechanical properties. The specifications of testing equipment, procedures

to be followed are also discussed subsequently in this chapter.

3.2 Synthesis of NZF by Sol-gel auto combustion method

The chemicals used in the synthesis of Ni0.5Zn0.5Fe2O4 by sol-gel auto

combustion method are as follows: Pure nickel nitrate [Ni(NO3)2·6H2O], iron nitrate

[Fe(NO3)2·9H2O], zinc nitrate [Zn (NO3)2·6H2O] and urea [CO(NH2)2] (all from Sigma

Aldrich). They are used with no further purification in the synthesis process and the

steps followed in the process are shown in Figure 3.1.

The reaction equation for the synthesis of Ni0.5Zn0.5Fe2O4 using sol-gel auto

combustion process is given by

0.5 Ni (NO3)2.6H2O +0.5Zn (NO3)2.6H2O +2 Fe (NO3)2.9H2O +6.6 CO (NH2)2 +3O2

Ni0.5Zn0.5Fe2O4 +6.6 O2+9.6 N2+37.3H2O 3.1

84
 Figure 3.1: Schematic representation of sol-gel auto combustion method

The required stoichiometry of raw materials nitrates and urea according to the

above equation was as followed: The molar ratio of nitrates i.e. Nickel Nitrate:

ZincNitrate: Iron Nitrate are 1:1:4 and that of Iron Nitrate to urea was 1:3.33. Therefore

for each 7.59 g of Nickel Nitrate and Zinc Nitrate, 40.49 g of Iron Nitrate was added to

20 g of Urea according the required stoichiometry. The raw materials were shown in

Figure 3.2. Deionized water was added to the precursors to from the sol, which was

then converted into gel using a magnetic stirrer at 320 rpm and 900C. When introduced

to a muffle furnace preheated to 4500C, the gel boiled, foamed and ignited. The flame

persisted for 30 s. Upon the completion of the combustion reaction, a solid powder was

produced and then the solid powder is grounded in a silica crucible using a porcelain

pestle to produce a fine powder. The dried powder was calcined at 6000C for 6 h to

remove the unreacted volatile organic residues and obtain a pure phase compound. The

sol-gel process was shown in Figure 3.3. Finally the powder was ball milled for 30 min.

at 500 rpm to produce a fine Ni0.5Zn0.5Fe2O4 nano powder.

85
 a b c d

Figure 3.2: Raw materials used in synthesis process: a) Nickel Nitrate b) Zinc nitrate c) Iron

nitrate d) Urea

Figure 3.3: Sol-gel process a) Weighing of elements b)Sol-gel conversion c) Auto combustion d) Before

grinding e) After grinding f) Calcination g) Ball milling h) Nickel zinc ferrite nano powder

3.3 Materials used in Fabrication

3.3.1 Epoxy resin and hardener

Among polymer matrices, epoxy is the most frequently used and excellent

thermosetting resin especially used in space shuttle, aircrafts, electronic products and

other industrial applications [91-92 and 122]. They have excellent directional stability,

stiffness, specific strength, chemical resistance, low viscosity, low price and exhibit

86
good adhesion to the fibre embedded [15, 23 and 129]. Due to clear evidence from the

extensive literature available for epoxy as an excellent resin for composites, it was

chosen as matrix material in this work. Epoxy (Epofine 556) thermoset resin and

Finehard 5200 (with a density of 1.2 g/cm3) supplied by Fine Finish Organics Pvt. Ltd.

were used as the matrix and hardener.

3.3.2 E-glass fibre

E-glass/electrical grade glass fibre was first developed as insulators in electrical

wiring applications subjected to high temperatures. It has high specific strength,

chemical and dimensional stability and resistant to vibration and abrasion [6, 18 and

95]. Nowadays 90% of the reinforcements used in composites or textile industry is E-

glass fibre only. The selection of E-glass fibre as reinforcement element fits naturally

into the framework of this research on RAMs due to its excellent properties [108, 112

and 172]. A Plain-weave E-glass fabric with 12,000 strands per tow and having an aerial

weight of 400 gsm was used in this work. The calculated weight ratio of E-glass fibres

to neat epoxy resin is 42:58 using rule of mixtures of composite density.

3.3.3 MWCNT and NZF

Among the various dielectric absorbing materials, multi-walled carbon

nanotubes (MWCNT), graphene, carbon black, carbon nano fibers and reduced

graphene oxide (RGO) are promising because of their attractive properties such as

excellent electrical characteristics, good thermal stability and high resistance to

chemical agents [108, 114, 123 and 172-173]. MWCNT has been chosen as the

dielectric material in this work. The MWCNT with two different aspect ratios were

utilized to fabricate E-glass/epoxy/MWCNT/NZF composites. The MWCNT having an

outer diameter of 10–25 nm and a length of 3–8 µm (purity: 99%) were procured from

87
Intelligent Materials Pvt. Ltd., India were used as high aspect ratio (315) dielectric filler

in the absorbing materials. The low aspect ratio (115) MWCNT is having an outer

diameter of 80-94 nm and a length of 9-11 µm. The nickel zinc ferrite is chosen as

magnetic filler to prepare the RAMs in this work. The NZF nanopowder with an

average particle diameter of 26 nm, prepared by the sol-gel auto-combustion method

discussed in previous chapter 3, was used as the magnetic filler.

3.4 Fabrication Method of Radar Absorbing Materials

The fabrication procedure adopted here was combination of different techniques

like strirring, ball milling, ultrasonication, used to get better dispersion of the fillers in

epoxy matrix [112 and 122]. The schematic representation of the fabrication process is

shown in Figure 3.4. The usage of high temperature hardener i.e. curing of samples at

high temperatures will ensure the high strength and thermal stability of the fabricated

structures [9 and 108]. In this work four different types of RAMs i.e. dielectric RAMs,

Magnetic RAMs, combination of dielectric and magnetic RAMs with high and low

aspect ratio MWCNT were prepared using MWCNT, Nickel zinc ferrite nano powder

for electromagnetic properties testing. The required samples to evaluate the mechanical

properties were also fabricated according to ASTM standards. The steps of the

fabrication process are summarized as follows:

1. The introduction of nanofillers in powder form in liquid solvent acetone to

facilitate the better mixing in the polymer solution [157 and 329].

2. Evaporation of acetone and the subsequent ball milling to enhance the mixing

of nano fillers and polymer solution [91 and 112].

3. Ultrasonic agitation using bath type sonicator, which uses ultrasound energy to

blend particles in a solution for effective dispersion of fillers [94, 112 and 122].

88
 4. Heating the solution to 900C to reduce the viscosity and to facilitate the uniform

coating of the mixture onto E-glass fabric by hand layup method [95-96].

5. Compaction of the samples by placing them under heavy metal plates after the

entrapped air bubbles were removed by roller [26 and 92].

6. Curing in hot air oven at different elevated temperatures of 700C for 1h, 1100C

for 1h, 1600C for 2 h and 180 0C for 2 h produced the samples [94 and 112].

Figure 3.4: Schematic representation of fabrication process

3.4.1 Fabrication of E-glass/epoxy /MWCNT composites

The measured amounts of Epoxy resin and MWCNT were mixed with acetone

for better blending. After the complete evaporation of acetone the solution was ball

milled (In smart systems) for 1 hr at 500 r.p.m and with a ratio of 100:24 hardener was

added. Bath type sonication (Trans-O-Sonic,M/s Shanti Industrial Estate) at 80Khz

frequency for 30 min was utilized to get homogeneous mixture. By heating the solution

89
to 90oC the viscosity reduced to facilitate the uniform impregnation on E-glass fabric

using hand layup method. The hot air oven was employed to cure the samples at

different temperatures for 6 hrs. The fabrication process is shown in Figures 3.5 to 3.7.

The obtained specimens with a thickness of 1.5 mm were machined to a size of 22.9

mm x10.2 mm to fit into X-band wave guide sample holder .The five samples of varying

MWCNT weight percentages from 0.4% to 2% were fabricated. The five samples were

designated as MWCNT 0.4, MWCNT 0.8, MWCNT 1.2, MWCNT 1.6 and MWCNT

2 respectively.

3.4.2 Fabrication of E-glass/epoxy/NZF composites

The measured amounts of NZF and epoxy were blended with acetone by

vigorous stirring to facilitate better mixing. A magnetic stirrer was then used to

evaporate the acetone at 100 rpm and a temperature of 80 °C. The mixture was ball

milled for 1 h at 500 rpm. The hardener was added at a ratio of 100:24 and subsequently

sonicated in a bath-type sonicator at a frequency of 80 kHz for 30 min. The mixture

was then heated to 90 °C. Following the hand layup technique, the E-glass fabric was

impregnated with the prepared solution. The impregnated fabrics were cured in a hot-

air oven at different elevated temperatures for 6 h to produce samples with a thickness

of 2 mm. The samples were cut to the dimensions of 22.9 mm × 10.2 mm for testing of

microwave absorption properties. The E-glass/epoxy/NZF nanocomposites were

fabricated with varying ferrite weight percentages of 10, 20 and 25 wt% and denoted

as NZF1, NZF2 and NZF3, respectively.

90
3.4.3 Fabrication of E-glass/epoxy / MWCNT/Nickel Zinc Ferrite composites for
microwave absorption properties

Figure 3.5: Fabrication process-Premixture preparation (a) Weighing of components (b) After

ball milling (c) During sonication

Figure 3.6: Fabrication process-Hand layup method (a) Cutting of E-glass fabric (b) Coating on
E-glass fabric (c) Before curing

Figure 3.7: Fabrication Process-Curing of samples (a) Hot air Oven (b) Samples for curing (c)

Prepared samples

To prepare the premixture of epoxy resin and lossy materials, measured amounts of

nanomaterials were first blended with acetone. After complete acetone evaporation, the

mixture was ball milled for 60 min at 500 rpm and the epoxy and hardener were added

at a ratio of 100:24. Subsequently, the mixture was ultrasonicated in a bath sonicator

91
for 90 min at 80 KHz to obtain a homogeneous mixture. To reduce the viscosity of the

mixture, the temperature of the solution was increased to 90 ⁰C for better dispersion.

The E-glass fabric was impregnated with the prepared composition layer-by-layer using

a hand layup technique. The composites were cured in a hot-air oven for 6 h at different

elevated temperatures. The obtained samples had a thickness of 2 mm. All the prepared

samples were cut to the dimensions of 22.9 mm × 10.2 mm for testing of

electromagnetic properties. The five samples prepared with high aspect ratio of

MWCNT are designated as NZFM1, NZFM2, NZFM3, NZFM4 and NZFM5. The low

aspect ratio MWCNT samples are named as NMWCNT 1, NMWCNT 2, NMWCNT

3, NMWCNT 4 and NMWCNT 5. The details of the compositions of the samples are

listed in Tables 3.1 and 3.2

Table 3.1 Weight percentages of high aspect ratio E-glass/epoxy/ MWCNT/NZF samples

S. No. Code of Wt % of Wt % of
sample NZF MWCNT

1 NZFM 1 20 0.4

2 NZFM 2 20 0.8

3 NZFM 3 20 1.2

4 NZFM 4 20 1.6

5 NZFM 5 20 2

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 Table 3.2 Weight percentages of low aspect ratio E-glass/epoxy / MWCNT/NZF samples

S. No. Code of Wt % Wt % of
sample of MWCNT
NZF

1 NMWCNT 1 20 0.5

2 NMWCNT 2 20 1

3 NMWCNT 3 20 1.5

4 NMWCNT 4 20 2

5 NMWCNT 5 20 2.5

3.4.4 Fabrication of E-glass/epoxy / MWCNT/Nickel Zinc Ferrite composites for

mechanical properties

The main advantages of fibre reinforced radar absorbing materials compared to

radar absorbing coatings are their good mechanical properties. In order to evaluate the

tensile strength, flexural strength, impact strength and hardness, samples were

fabricated by following the fabrication process explained in the section 4.4.3.1. The

sample sizes for the tensile and flexural tests were 250 mm × 25 mm × 3 mm and 125

mm× 12.7 mm × 3.2 mm, respectively according to the ASTM D3039 and ASTM D790

standards. The impact test specimens were prepared according to the ASTM D256

standards, with the dimensions of 64 mm × 12.7 mm × 3.2 mm. Hardness of the

samples are determined using ASTM D2583 standards. For each test three specimens

were prepared.

3.5 Characterization Techniques

In many applications, for the adaptation and development of nanomaterial, its

characterization is the keystone. A number of characterization techniques are developed

to measure their novel and unique physic-chemical properties including composition,

93
morphology, surface area, structure, size, optical properties and magnetic properties

etc. [326-327]. The characterization techniques used in this work are described in the

following sections

3.5.1 X-ray diffraction analysis (XRD)

XRD is an analytical technique used for microstructural analysis of materials to

provide in-depth information about the crystalline compounds. The atomic

arrangement, crystallite size, unit cell dimensions, foreign phases and imperfections in

crystalline powders can be determined by using this technique [82 and 182]. When the

finely grounded powder samples were irradiated by X-rays, then the measured

diffracted X-rays angles and intensities provides the information regarding the crystal

structure of the sample. The identification of phases was done by the comparison of

diffraction patterns obtained in the sample with the standard reference patterns,

published by ICDD (International Centre for diffraction data). In addition to crystalline

phase identification, the peak intensities and shapes measured during XRD analysis

provides the information regarding the crystallite size and percentage of crystallinity

[64 and 218].

The applications of XRD includes the identification of the crystalline phases

and orientation, determination of microstructural properties like lattice parameters,

strain, grain size, epitaxy, phase composition etc. The advantages include the non-

destructive nature of the technique, powerful and rapid technique (< 20 min) to

determine the unknown material, minimum sample preparation and its straight forward

data interpretation. The compulsion of having access to standard reference files,

complicated data interpretation for non-isometric crystal systems and requirement of

94
tenths of a gram of material in powder form are generally considered as the limitations

of this analysis.

XRD Equipment Specifications:-The crystallographic structure of the synthesised

NZF nanoparticles was determined using an X’Pert Pro diffractometer (PAN analytical)

available at IIT Hyderabad as shown in Figure 3.8, with 1.54 Å Cu Kα radiation,

varying 2θ from 10° to 90°. The electric current and operating voltage were

maintained at 30 mA and 40 kV, respectively. Before the measurement, equipment was

calibrated using multiple reflections per phase method (one of the available calibration

techniques) specified by the manufacturer.

Goniometer

X-ray source
Detector

Sample stage

Figure 3.8: XRD equipment at Dept. of chemistry, IIT Hyderabad, Telangana

3.5.2 Scanning electron microscope (SEM)

The shrinkage of dimensions of devices and materials led to no longer

characterization of many structures by light microscope. The wavelength of light is the

95
limiting factor in obtaining a better resolution of the light microscope. The electron

microscopes were developed to overcome this shortcoming of microscopes as electrons

are having shorter wavelengths compared to light. A scanning electron microscope

(SEM) uses a focussed electron beam to scan a surface, to produce an image. Depending

upon the sample density and accelerating voltage, the electron beam penetrates the

samples up to a depth of few microns. The electron-sample interactions generate a

number of signals due to the emission of secondary electrons (SE), backscattered

electrons (BSE) and characteristic x-rays. These signals are processed to obtain

information about the sample’s composition and topography. The application of SEM

includes the determination of texture or external morphology, crystal structure,

chemical composition and the orientation of materials in the sample etc.

Even though it has limitations like expensive to procure, bulky to carry, the

requirement of consistent voltage and cooling systems, an environment free of

vibrations and electromagnetic elements etc., its advantages of easy to acquire data in

a short period (5 min) in digital format, user-friendly interfaces, easy to operate and

high resolution of about 20 nm, makes it as a better choice for morphological

characterization especially for nanomaterials [80 and 225]. This research is an attempt

to utilize the nanomaterials for radar/ microwave absorption applications, the effective

and appropriate instrument to characterize the materials is SEM.

SEM equipment Specifications :-The size and morphology of the materials were

determined by using JSM-7100f field-emission scanning electron microscope (Jeol

India Pvt.Ltd.) as shown in Figure 3.9 at AU centre for Nanotechnology,

Visakhapatnam, Andhra Pradesh, with accelerating voltage of 0.5-30 kV, working

distance: 0-40 mm, magnification: 10X-1000000X. Other two scanning electron

microscopes at University of Hyderabad and IIT Hyderabad in Telangana were also

96
utilized for obtaining micrographs of the materials. The SEMs are calibrated for

magnification using the calibration standards specified by the maker. While calibrating

for magnification it is always recommended to consider the working distance as it has

significant effect on magnification.

3.5.3 Energy dispersive X-ray (EDX) analysis

EDX analysis also referred to as EDAX or EDS is an X-ray technique

commonly used for chemical composition analysis of materials. The characteristic X-

rays emission in the atoms of the specimen caused by the incident electron beam was

involved in the EDX analysis. In the EDX spectrum, the Y-axis indicates the counts of

number of X-rays received and detected), the X-axis indicates those counts energy

level.

Figure 3.9: FESEM at AU Centre for Nanotechnology, Visakhapatnam, Andhra Pradesh

It works on the principle of spectroscopy, which deals with the study of

electromagnetic radiation and matter interaction in terms of frequency of radiation or

wavelength function. It is generally attached to electron microscopes like SEM or TEM.

97
The characterization capabilities of EDX depends on the unique atomic structure of

each element, exhibiting a unique set of peaks in its electromagnetic emission spectrum.

When electrons bombarded the elements in the specimen, leads to the emission of X-

rays at the element’s characteristic frequencies.

By proper calibration, the relative amounts of the elements present in a material

are given by the number of X-rays emitted. The composition or relative amount of the

elements in nanomaterial can be easily detected when they are composed of heavy metal

ions like gold, palladium and silver compared to low atomic elements by this technique.

The important advantages include quick analysis, easy interpretation of spectrum, good

spatial resolution and improved quality control of the product. Its applications include

identification of materials, contaminant analysis and hence used widely in industries

like manufacturing, research, consumer packaged goods, energy and resource

management etc. The energy dispersive X-ray (EDX) spectrums were recorded on

spectroscopes attached to the scanning electron microscopes.

3.5.4 Transmission electron microscope (TEM)

TEM is considered as indispensable, powerful and popular technique in

nanomaterial characterization by electron microscopy [73]. This is due to their unique

spatial resolution in atomic scale which facilitates the study of nanostructured materials.

In TEM, the high energy E-beam (60 - 350 kV) is transmitted through a thin specimen

and transformed into elastically or inelastically scattered electrons. The data

interpretation in TEM is complex due to dynamical diffraction effects of the strong

interaction of electrons with the matter. Majorly it differs from SEM in two aspects.

One is the higher accelerating voltages (100-300 kV) needed for the high resolution

98
(0.1 to 0.2 nm). Second is the signal collected for image formation made up of

transmitted electrons.

In TEM the reliability of analysis depends upon the effective transferability of

the representative fraction of the specimen with a sufficient amount of particles to the

sample carrier. The high accelerating voltages limit the analysis of soft materials like

porous materials, polymers, carbon-based nanomaterial etc. It has more advantages like

higher spatial resolution, powerful magnifications up to two million times, provision of

information regarding element and compound structures etc. The disadvantages

include, expensive to purchase, the requirement of special maintenance and training for

operation and analysis, laborious sample preparation and black & white images as

output.

Figure 3.10: Transmission Electron Microscope at SAIF lab, IIT Bombay, Mumbai,

Maharashtra

99
TEM Equipment Specifications:-The diameter and multi-layered structure of

MWCNT, morphology and SAED patterns of NZF were determined by an FEI Tecnai

TEM microscope at as shown in Figure 3.10 at 300 kV with a resolution of 2 Å located

at SAIF lab, IIT Bombay, Mumbai, Maharashtra. A flat field calibration has to be done

before taking the micrographs using TEM.

3.5.5 Fourier transform infrared spectrometer (FTIR)

FTIR spectrometer is used to identify organic, inorganic and also polymer

materials. It utilizes the infrared light to get the interferogram by scanning the test

sample. The Fourier transform of the interferogram gives the spectrum which is the

molecular vibrational spectrum and the FTIR spectrometer digitizes the spectrum to get

the chemical properties of the sample. In this technique, the emissive and absorptive

properties of the materials were studied [77, 251 and 269]. When exposed to infrared

radiation of the FTIR spectrometer, specific wavelength radiation was selectively

absorbed by the sample molecules. It leads to the change in sample molecules dipole

moment and corresponding vibrational energy levels of the sample. The detector senses

the resulting signal converts into a spectrum, which was the molecular fingerprint of

the sample. Therefore abundant microstructural information about a molecule can be

readily obtained by the analysis of the spectrum.

The fact that each chemical structure or molecule gives unique spectral

fingerprint was the reason for the enhancement of FTIR as a great tool for chemical

analysis. This method is used to identify unknown materials and contaminations. FTIR

is used in various industries like organic synthesis, petrochemical engineering, polymer

science, pharmaceutical industry, biological research, forensic industry etc. This

method has advantages of high spectral accuracy and quickly acquired spectra.

100
Equipment Details: -The Fourier-transform infrared (FTIR) spectrum was recorded

using a Hyperion 3000FTIR microscope (Bruker) in the region of 4000–400 cm–1 at

SAIF lab, IIT Madras, Chennai, Tamilnadu as shown in Figure 3.11. Standard operating

procedure specified in the guide lines provided by manufacturer is followed before

performing the experiment.

Figure 3.11: FT-IR at SAIF lab IIT Madras, Chennai, Tamilnadu

3.5.6 Vibrating sample magnetometer (VSM)

The magnetic moment which is the most fundamental quantity in magnetism

was measured by the instrument known as vibrating sample magnetometer (VSM). It

is a versatile and sensitive instrument utilized for determining different materials like

diamagnetic, paramagnetic, ferromagnetic and antiferromagnetic material’s

magnetization as a function of temperature and magnetic field. A VSM works by

placing the sample material in a uniform magnetic field, then a dipole moment

proportional to the sample’s susceptibility and applied field is induced. The applied

constant magnetic field aligns the individual magnetic spins or the magnetic domains

in the sample material with the magnetic field. As the sample is given sinusoidal

101
motion, the magnetic stray field developed in the material varies as a function of time

and sensed by suitably located stationary pick up coils.

According to Faraday’s law of induction, the alternating magnetic field will

produce an electric field in pickup coils. The magnetization of the sample depends on

the current produced. By using controlling and monitoring systems, the sample’s

magnetic moment can be measured. This VSM is used to find the magnetic moment of

materials with high precision and its application involves the study of nanocrystalline

alloys, nanoscale wires, magnetic thin films, semiconducting ferrofluids, permanent

and natural magnets, ferrites etc. [82, 215, 261, 323 and 328].

Figure 3.12: Vibrating Sample Magnetometer at SAIF lab, IIT Madras, Chennai, Tamilnadu

Equipment Details:- Magnetic characterisation was conducted using a 7410VSM

(Lakeshore) shown in Figure 3.12, at 300 K with the applied fields of ±15 × 103Oe at

SAIF lab, IIT Madras, Chennai, Tamilnadu. The equipment is calibrated using standard

VSM calibration file before measurement.

102
3.6 Testing of RAMs for EM, Thermal and Mechanical properties

3.6.1 Vector network analyser (VNA)

A vector network analyser (VNA) is the most versatile, complex and essential

test equipment in the field of microwave and RF (radio frequency) engineering research

and development and also in production for test purposes. It measures the component

or a network’s frequency response [79 and 181]. It calculates the going into and coming

back power of a high-speed signal, from a network or a component. At each frequency

point, the high-frequency signal’s amplitude and phase are captured. The equipment

contains both source (for the generation of stimulus signal) and receivers to estimate

the changes in the stimulus signal resulted due to the component under test. It measures

and compares both the signals i.e. reflected from the input side and transmitted through

the output side of the component under test or a network under the test with the known

stimulus signal. Processing of the measured signals by an external or internal PC

displays the output values.

The two types of measurements performed in vector network analyser are

reflection and transmission. The transmitted signal received on the other side of the

component under test gives the most common S-parameters ‘S21’ and ‘S12’. Examples

of other transmission measurements include insertion loss, group delay, electrical

length and gain etc.

103
 Figure 3.13: VNA at Dept. of M.E, AUCE (A), Visakhapatnam, Andhra Pradesh

The signal travels backwards and towards the source caused by the reflections,

gives the common reflection S-parameters ‘S11’ and ‘S22’ [9, 230 and 249]. The four

S- parameters are most commonly measured in most of the VNAs. They are also

capable of presenting and visualizing the output values in different formats like smith

charts, real/imaginary magnitude and phase values etc. In the calibration of VNA by

wave guide method LRL (Line Reflect Line), TRL (Through Reflect Line) and LRM

(Line, Reflect, Match) methods are utilized for broad frequency range. The ease in

making and a high level accuracy at microwave frequencies made the calibration by

TRL method advantageous compared to others. This method utilizes a known length of

transmission line and impedance as one standard. The main drawback of this method is

that the line needs to be longer in electrical length than the through line. In addition

TRL also needs a high reflection standard (usually open or short) whose impedance

must be electrically the same for both test ports and doesn’t have to be dwell

characterized.

VNA Specifications:-The electromagnetic properties in the X-band were obtained

using a ZVB 20 vector network analyser (Rhodes & Schwarz) as shown in Figure 3.13

104
at Dept. of M.E, AUCE, Visakhapatnam, Andhra Pradesh. The tests were conducted

using WR90 wave guides in accordance with Electronic Industries Alliance (EIA)

standards. The size of the samples is 22.86 mm X10.16 mm. The VNA is calibrated

before measuring the complex permittivity and permeability by TRL (Thru Reflect

Line) method using calibration kits provided by the manufacturer.

3.6.2 Thermogravimetric Analyzer (TGA)

Thermogravimetric analysis is a thermal analysis technique which measures the

thermal stability of a material and fraction of its volatile components by measuring the

material’s weight change as a function of temperature/ time under a controlled

atmosphere [9 and 202]. By gradually increasing the temperature of the sample at a

constant rate in a furnace, the weight is measured by an analytical balance placed

outside the furnace. The mass losses were observed in chemical reactions including

combustion, decomposition, evaporation, reduction, desorption and not in physical

changes like melting. Due to the unique sequence resulting from physiochemical

reactions occurring over a specific range of temperatures and heating rates,

characteristic thermogravimetric curves are developed for chemical compounds and

specific materials. These unique properties are correlated to the structure of the

molecules in the sample [330-331].

The combination of the TGA with FTIR can be used for the detailed chemical

analysis of evolved gases from the sample. The technique’s applicability includes the

determination of material’s thermal stability, oxidative stability, plasticizer content in

polymers, decomposition temperature, carbon black content, estimated lifetime of the

product, etc. It has advantages like high accuracy, reliable data and minimal sample

105
preparation etc. The disadvantages of this technique are a limited range of samples,

destructive nature of the test, interpretation of the data is not always straight forward.

Figure 3.14: TGA at Dept. of chemistry, IIT Madras, Chennai, Tamilnadu

TGA specifications: -Thermogravimetric analyses (TGA) of the fabricated samples

were conducted using a Q500 high-resolution TG analyser as shown in Figure 3.14 at

a heating rate of 20°C/min and temperature range of 40–950°C under a nitrogen

atmosphere available at department of chemistry lab, IIT Madras, Chennai,

Tamilnadu,. The testing standards are ASTM E2550-21. The equipment is calibrated

using melting point standard method based on the curie temperature of standard

reference material.

3.6.3 Universal testing machine (UTM)

One of the essential reason for the growth in the manufacturing industry is the

advanced composite materials like reinforced polymer composites. UTM is used to

determine the suitability of the composites to meet the particular end-use applications,

to optimize the material formulations and quality control. The advances in electronics

which favoured the data acquisition from sensors, together with analysis software

106
improved the UTM’s performance. The major components of it are the loading unit,

deals with the loading of the specimen with required force, control unit to apply the

required amount of the load via control valves and display unit to present the response

of the specimen.

A wide variety of tests can be performed on a vast range of materials,

component and structures on this UTM including tensile, compressive, shear, flexural

and fatigue tests [47, 290 and 332]. Different varieties of UTMs are available in the

market nowadays for example table-mounted, floor mounted, static, dynamic,

electronic and hydraulic UTM’s. In static UTMs loading of the specimen (i.e. the speed

of the force) generally ranging from 0.001-20 inch per min. In dynamic or cyclic tests

like fatigue tests, the servo-hydraulic UTMs applies reduced load for long periods. In

some UTM’s environmental chamber was inbuilt to facilitate the testing at high

temperatures ranging from -196 0C to 1000 0C. The load application at a uniform rate,

selection of proper dimensions for the specimen are the precautions to be taken.

UTM specifications:-The mechanical properties (tensile and flexural strength)

of the double-layered RAMs were determined according to the ASTM D3039 and

ASTM D790 standards using a universal testing machine (HLC 693, HEICO) as shown

in Figure 3.15, at a crosshead speed of 50 mm min−1, available at CIPET Vijayawada

lab. The sample sizes for the tensile and flexural tests were 250 mm ×25 mm × 3 mm

and 125 mm× 12.7 mm × 3.2 mm, respectively. The impact testing machine is

calibrated and certified by National Accreditation Board for testing and calibration

laboratories (NABL) regularly.

107
 Figure 3.15: Universal Testing Machine at CIPET, Vijayawada

3.6.4 Impact testing Machine

Impact testing machine evaluates the material or component capacity to

withstand high-rate loadings and at varying temperatures. Impact resistance is one of

the important phenomena in governing the life of a structure. Ex: aircraft, automobiles

etc. Generally, izod and charpy tests are the two tests that are performed to evaluate the

resistance of materials to the external impacts. The notched specimens (V-notch, U-

notch) were used for impact testing [25 and 333-334]. The Izod impact strength test

according to ASTM standards has become popular for comparing the polymer

composites impact resistance.

By releasing a pivot arm after rising to specific height (constant potential

energy), the notched specimen hit by the arm swinging down. The energy was absorbed

by the specimen until it yields. When a fracture occurs, the specimen can absorb no

more energy. The height of the arm swings after hitting the sample was used to calculate

the energy absorbed by the specimen. Ductile materials are having more impact strength

108
compared to brittle materials. The materials transition from ductile to brittle materials

can be determined by testing the number of samples at varying temperatures. By

plotting impact energy values against the temperatures, the sudden decline of the impact

energy curve gives the temperature of transition.

Figure 3.16: Impact testing machine at CIPET, Vijayawada

Impact testing machine specifications:- To find the impact strength of the E-

glass/epoxy reinforced composites, an Izod impact test was conducted according to the

ASTM D256 standards with the dimensions of 64 mm × 12.7 mm × 3.2 mm on an

impact testing machine (Presto) as shown in Figure 3.16, located at CIPET Vijayawada

lab. The impact testing machine is calibrated and certified by National Accreditation

Board for testing and calibration laboratories (NABL) regularly.

3.6.5 Barcol hardness tester

The Barcol hardness tester mainly characterizes the indentation hardness of composite

materials like reinforced thermosetting plastics and also for aluminium and aluminium

109
alloys. It measures the depth of penetration of indentation and compares it to the

reference material penetration. The test complements the measurement of glass

transition temperature and also used to determine the resin’s degree of curing. By

keeping the indenter perpendicular to the test surface, the instrument is taken onto the

sample and uniform pressure is applied on the instrument, the spring-loaded indentor

pointer penetrates the sample. The depth of penetration is converted and displayed as

Barcol hardness value instantly on the dial indicator [335-336]. It has many advantages

like easy and single-hand operation, inexpensive, portable weighing 1 kg, no experience

is needed, minimum size of the sample (<1/16 th of an inch) and quick results. In this

work, the hardness of double-layered materials was determined using a Barcol hardness

tester at CIPET Vijayawada lab as shown in Figure 3.17 according to ASTM D2583. It

is calibrated and certified by National Accreditation Board for testing and calibration

laboratories (NABL) regularly.

Figure 3.17: Barcol hardness tester at CIPET, Vijayawada

110
3.7 Summary

This chapter summarises

1. The synthesis procedure of NZF using sol-gel auto combustion method such as

raw materials metal nitrates and urea weights and compositions, the conditions

required to the sol to gel conversion and heat treatments to form pure nickel zinc

ferrite nanopowder.

2. The details of materials used to fabricate the RAMs with dielectric and magnetic

lossy nanofillers MWCNT and NZF such as specifications and manufacturer.

3. The experimental procedures consisting of hand layup method followed by

compression molding with required mixing ratios of raw materials,

temperatures, frequencies of sonicator, speeds of the magnetic stirrer and curing

time etc.

4. The operating principles, precautions to be followed, applications, merits and

demerits of the equipment used for nanomaterials characterizations in the

present work.

5. The specifications like operating voltages, magnifications, resolutions etc. of

FESEM, TEM, XRD equipment used for microstructural and morphology

characterization. The features of EDX, FTIR and VSM like operating voltages,

range of wave number, applied magnetization etc. which were employed to

determine the nano materials (MWCNT and NZF) chemical and magnetic

properties. These materials are used in the present work to fabricate the RAMs.

111
6. The equipment details, testing procedures and calibration methods for testing

the electromagnetic and mechanical properties including VNA, TGA, impact

testing machine and Barcol hardness tester.

112
Chapter 4 MICROSTRUCTURAL, CHEMICAL,
MAGNETIC AND THERMAL
CHARACTERIZATIONS OF MICROWAVE
ABSORBING MATERIALS
4.1 Introduction:
The nanomaterial’s surface to volume ratio leads to an exceptional increase in

the reactivity at the molecular level. This makes the difference in properties of

nanomaterials compared to their bulk counterparts. The size and its distribution, shape

of the nanoparticles are the main parameters in the characterization of nanomaterials.

The chemical composition and crystal strucuture are investigated in depth as initial step

after synthesis of nanoparticles to use it for specific applications. For magnetic fillers

in the RAM, the value of saturation magnetization, coercivity are to be determined to

find its magnetic nature. The microwave absorption properties are largely influenced

by the size, shape, chemical composition, crystal structure, nature of magnetization of

the nanomaterials. The thermal stability of RAM is important as it determines the

suitability of operating in high temperature environments.

4.2 Characterization of Synthesized Nickel Zinc Ferrite

4.2.1 Morphological characterization of NZF

The SEM and TEM micrographs are used to determine the microstructural

properties, sized distributions, agglomeration state, dispersion state and for 3D

visualization of nanomaterials. The microstructure and morphology of the nano-NZF

particles synthesized by sol-gel method is verified by SEM and TEM are shown in

Figures 4.1 (a) & (b). The SEM micrographs were taken at the operating voltage of 15

kV, working depth of 5.2 mm and magnification of 50,000X. Thermionic emission gun

is utilized to generate the electron beam of SEM at an operating current of 33-500 ρA.

The particles of NZF are agglomerated due to its magnetic nature. The TEM operating

113
conditions are 300 kV with a point resolution of 2 Å and a line resolution of 1 Å. The

particle size distributions were obtained by measuring the diameters of over 150

particles form TEM micrographs are shown in Figure 4.2. The distributions were found

to be asymmetrical, with a mean value of 26 nm. On ferrites, studies have reported that

the presence of zinc and variations in grain size distribution support loss mechanisms

by enhancing magnetic properties and the permeability loss component, subsequently

leading to microwave absorption [60, 266, 267 and 268]. In this work, the average size

of the particles was 26 nm and the spherical morphology of NZF was confirmed by

SEM and TEM micrographs. The NZF prepared by solgel and microwave auto

combustion methods in the earlier research works [60 &323] are having spherical

morphology close to present work but they have different particle sizes of 16 nm and

47 nm respectively. And it is noted that the double layered RAMs prepared with 16 nm

NZF exhibited good reflection loss. It is expected that present NZF also results in better

microwave absorption in the X-band. The particle size distributions in [53 and 323]

given the mean diameter of NZF as 5 nm and 47 nm. The present synthesis resulted

particle size distribution with mean diameter of 26 nm. The synthesis methods might

be the reason behind such larger difference in particles.

Figure 4.1: a) SEM image b) TEM image of NZF

114
 Figure 4.2: Particle size distribution of NZF

4.2.2 Microstructural characterization of NZF

The XRD patterns of the Ni0.5Zn0.5Fe2O4 nanoparticles produced by the sol-gel

auto-combustion technique are shown in Figure 4.3. The peak positions at 2θ = 180,

300, 35.50, 430, 53.50, 570, 62.60 and 890 were corresponding to crystalline planes ( 1 1

1 ), ( 2 2 0 ), ( 3 1 1), ( 4 0 0 ), ( 4 2 2 ), ( 3 3 3 ), ( 4 4 0 ) and ( 5 3 3 ). They comply

with JCPDS file no. 8-0234, in accordance with literature works [52, 59, 60, 72 and

250] and attributed to the single-phase, face centred cubic spinel structure of

Ni0.5Zn0.5Fe2O4 with no impurity phase [225 and 323]. The presence of sharp peaks

indicates high crystallinity. The crystallite size was determined by applying the Debye-

Scherrer formula.

t=0.9λ/B cos θ 4.1

where‘t’ is the crystallite size, ‘λ ‘ is the radiation wavelength, ‘B’ is the width

at the half-height of the diffraction peak in radians and θ is the diffraction angle. The

estimated crystallite size was 24 nm. In nanostructured materials, interfacial

polarization occurs, leading to high dielectric loss due to the greater surface area, as

most active atoms exist at the surface. The average size of the synthesized NZF particles

obtained from TEM is consistent with that estimated from the XRD analysis.

115
 Figure 4.3: XRD of synthesized NZF

The lattice parameter a was calculated by using the relations, 𝑎 = 𝑑 ∗

√ℎ2 + 𝑘 2 + 𝑙 2 and Bragg’s law of diffraction 𝜆 = 2𝑑 𝑠𝑖𝑛𝜃 . Where d is the interplanar

spacing, h, k, l, are the miller indices of the planes, ′𝜆′ is the wave length of x − rays,

𝜃 is the diffraction angle. The values of lattice parameter values in ref [52 and 72] are

8.397 Å and 8.35 Å. The obtained value of 8.382 Å in this work agreed with the

expected value of lattice constant for ferrites [52 and 72]. The selected area electron

diffraction (SAED) pattern is used to determine the d – spacing of crystal planes. These

are identified by measuring the radius of spots from bright centre and using the camera

constant. The SAED patterns further confirmed the expected crystal structure of the

nanosized NZF with corresponding planes of ( 1 1 1 ), ( 2 2 0 ), ( 3 1 1), ( 4 0 0 ), ( 4 2

2 ), ( 3 3 3 ), ( 4 4 0 ) and ( 5 3 3 ) as presented in Figure 4.4 and these patterns are

similar to the patterns obtained in the literature [67 and 264].

116
 Figure 4.4: SAED patterns of NZF

4.2.3 Magnetic characterization of NZF

The magnetic characterization of Ni0.5Zn0.5Fe2O4 was conducted at room

temperature of 24°C using a VSM with the field varying from -15 to +15 k Oe. The

applied field increase resulted in a rapid increase in the magnetization, as shown in

Figure 4.5. In magnetic properties, the coercivity is the strength of magnetic field to be

applied to decrease the material magnetization to zero. The retentivity indicates the

ability of a material to retain its magnetism, even after the ceasing of magnetizing force.

The hysteresis loop in the M-H curve of Ni0.5Zn0.5Fe2O4 indicates the presence of

coercivity and remnant magnetization, thereby indicating its ferromagnetic nature at

room temperature. The ferromagnetism is one of the reasons for ferrite’s microwave

absorption properties along with the resonance and eddy current losses [73, 189 and

212]. The porous activated carbon balls showed excellent microwave absorption

properties due to the ferromagnetic nature of CoFe3/Co3O7 and graphitized carbon

composites [87]. The saturation magnetization value of the NZF was 52.312 emu/g

which is comparable to the findings of previous studies [56, 67 and 244]. The values in

117
the ref [56, 67 and 244] are 54, 20 and 59 emu/g respectively. The larger saturation

magnetization values are responsible for better microwave absorption due to enhanced

magnetic loss mechanism. Das et al. [244] confirmed that an increase in crystallinity

and grain size leads to an increase in the average magnetization. Moreover, the addition

of zinc to ferrites enhances the magnetic properties of the material.

Figure 4.5: VSM of NZF

4.2.4 Chemical characterization of NZF

The elemental composition of NZF was determined by the EDX spectrum, from

which the atomic ratio of Ni: Zn: Fe was found to be 1:1:4. It is in consistent with

stoichiometry used in synthesis of NZF using sol-gel method. The EDX profiles as

shown in Figure 4.6 (a) also indicated the presence of O2 along with Ni, Zn and Fe and

these compositions are also obtained by other authors for nickel zinc ferrite in research

works [56 and 181]. The EDX Spectra of NZF prepared by solvothermal method and

solgel combustion method in the above mentioned works coincides with the spectra

obtained in the present work in terms of intensity peaks of elements Ni,Zn,Fe, and O2

118
and the energy levels of received X-rays. No presence of contamination elements in

EDX spectrum indicates the high purity of the NZF, which is one of the advantages of

the sol-gel method.

a b

b b

Figure 4.6: a) EDX and b) FTIR of synthesized NZF

Functional groups in a chemical compound can be determined by infrared

spectroscopy and used as an index to identify the bonds between the atoms in a

molecule using their unique vibrational frequency. The FTIR absorption spectra of the

synthesized NZF nanoparticles are presented in Figure 4.6 (b), with inset graphs that

119
show the clear visibility of the absorption bands. The stretching vibrations of metal at

tetrahedral sites and octahedral sites of NZF prepared from microwave combustion

method in ref [323] is observed at 600-500 cm-1 range and 400-385 cm-1 range. The

present sample exhibits two absorption bands in the 650-400 cm-1 range, which is a

feature of the ferrite spinel structure with two sub-lattices of tetrahedral (A) and

octahedral (B) sites. The high-frequency band of 650-500 cm-1 corresponds to the

stretching vibration of the tetrahedral metal-oxygen bond. The low-frequency band in

nickel-zinc ferrites usually observed in the range of 440-410 cm-1 is assigned to the

octahedral metal-oxygen bond, while the absorption bands at 1640 and 3420 cm-1 are

assigned to the adsorbed water present on the surface of the ferrite nanoparticle. The

similar absorption bands for nickel zinc ferrite were also obtained in the earlier research

works [52]. The FTIR spectra further confirms the formation of single-phase nickel

zinc ferrite with no impurities.

4.3 Characterization of MWCNT

4.3.1 Morphological and chemical characterization of MWCNT

The unique structure and high aspect ratio of MWCNT are responsible for its

microwave attenuation capability. MWCNT are usually bundled because of Vander

Waals forces (Figure 4.7 (a)); most of these bundles unbind when a strong shear force

is applied. This shear force is applied by means of sonication process used in fabrication

process. The diameter of high aspect ratio MWCNT used to fabricate MWCNT RAMs

and high aspect ratio MWCNT/NZF RAM was 10-25 nm and the length was 3-8 µm.

These dimensions of MWCNT were confirmed before the fabrication process using the

SEM and TEM micrographs as shown in Figure 4.7 (a) & (b), Figure 4.8 (a). The high

aspect ratio of MWCNT is responsible for enhanced microwave absorption properties

120
[29 and 321]. TEM micrograph clearly revealed the multilayered structure of

MWCNT. The operating voltages, working depth and magnification details of the SEM

used to capture the details of MWCNT are also shown in the respective micrographs.

The low aspect ratio MWCNT SEM image is shown in Figure 4.7 (b). Its diameter is

80-94 nm and length is 9-11 µm. This MWCNT is used to fabricate the hybrid low

aspect ratio MWCNT/NZF radar absorbing materials. The TEM micrographs of

MWCNTs are similar to the micrographs of the MWCNTs used in the previous

literature [10, 36 and 48]. All the multiwalled carbon nanotubes in the above references

are having diameters less than 10 nm and bundled due to Vander Waal forces; similar

nature is observed in present MWCNTs. In order to make them, disentangled,

dispersion methods like sonication and ball milling methods are incorporated in the

fabrication process in the present work. The MWCNT’s EDX analysis results are

illustrated in Figure 4.8 (b). The EDX spectrum of MWCNT are same as the patterns

obtained in the research work [351] with respect to the elements present and intensity

peaks and X-ray energy level. It shows the presence of no impurities and the elemental

composition of the MWCNT contains only carbon.

Figure 4.7: SEM image of a) high and b) low aspect ratio MWCNT

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 Figure 4.8: a) TEM image and b) EDX of high aspect ratio MWCNT

4.4 Microstructural and chemical characterization of fabricated

RAMs

The FESEM images of the fabricated composites of dielectric MWCNT RAM,

magnetic NZF RAM, combined (MWCNT + NZF) RAM were shown in Figure 4.9 (a),

Figure 4.10 (a), Figure 4.11 (a) respectively. The prepared samples have been subjected

to EDX analysis to study and identify the elemental compositions of radar absorbing

materials. The chemical compositions were obtained by EDX analysis of corresponding

samples were shown in Figure 4.9 (b), Figure 4.10 (b) and Figure 4.11 (b). From the

FESEM micrographs it was observed that the size of E-glass fibres was 14 microns. In

dielectric RAM, the presence of carbon confirms the existence of dielectric lossy filler

MWCNT in Figure 4.9 (b) and the appearance of Ni, Zn, Fe and O can be observed

from the magnetic RAM EDX analysis in Figure 4.10 (b). Furthermore in hybrid RAM,

composed of both MWCNT and NZF, the presence of C along with Ni, Zn, Fe and O

in EDX pattern as shown in Figure 4.11 (b) represents its chemical composition [52 and

84]. The FESEM and EDX of fabricated RAMs are similar to the results described in

ref [94, 112 and 352]. Additionally, the presence of silicon, magnesium and calcium

elements along with nickel, zinc, iron and oxygen in EDX of all radar absorbing

122
materials in the above cited literature are due to the presence of reinforcing elements

E-glass fibers in all the nanocomposites which are identical to the current research.

Figure 4.9: a) FESEM and b) EDX of fabricated MWCNT RAM sample

Figure 4.10: a) FESEM and b) EDX of fabricated NZF RAM sample

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 Figure 4.11: a) FESEM and b) EDX of fabricated NZFM RAM sample

4.5 Thermogravimetric analysis of RAMs

4.5.1 Thermogravimetric analysis of magnetic (NZF) RAMs

The degradation mechanism of the epoxy network samples followed three phases,

i.e., initiation, propagation and termination, as observed in other epoxy-based materials

[284].The TGA results of the Neat E-glass/epoxy composite and E-glass/epoxy/NZF

composites are shown in Figure 4.12. They are tested according to ASTM E2550-21

standards. The TGA curves of NZF are similar to the TGA curves obtained in the

previous literature works on nickel zinc ferrites [263 and 331]. The NZF prepared by

solgel auto combustion method, exhibited a thermal stability in terms of decomposition

temperature of 250 oC [263]. In the present work, improved thermal stability was

observed for the E-glass/epoxy/NZF composites relative to the Neat E-glass/epoxy

composite. The Neat E-glass/epoxy composite starts to lose mass (>2 wt%) upon

heating, even below 200°C, which is associated with the elimination of loosely bound

or adsorbed water and gas molecules. The initial major mass loss upon heating can be

observed in the temperature range 320–440 oC, due to the decomposition of the epoxy

matrix. According to Doyle et al., to find the thermal stability of the samples with

124
overlapping degradation steps, the integral procedural decomposition temperature

(IPDT) is more suitable. The IPDT can be determined using the following equation:

IPDT = AK(Te − Ts) +Ts 4.2

where Ts and Te represent the starting and ending temperatures of the degradation

process, respectively; A denotes the ratio of the area beneath the TGA curve to the total

area in the graph and K denotes the ratio of the area beneath the TGA curve to the area

under the residual curve. The calculated IPDT values of the three composites are 410
o
C, 413oC, 411oC respectively. The values are almost same for all the samples

irrespective of their composition. This can be attributed to the lesser value of aspect

ratio of NZF nanoparticles i.e for spherical particles aspect ratio is one. In the research

work by Crespo et al., [284] the IPDT values of epoxy based Cu – Ni nanoferrites filled

silica micro particles shown an IPDT value of 342 0C for 25 wt% of the filler. The

NZF/PU RAM in ref [331] with 30 wt% of filler resulted in thermal stability upto

3000C. In the present work, it was observed that E-glass/epoxy/NZF composites

exhibited a delayed decomposition (355oC) compared to the Neat E-glass/epoxy

composite (320oC) which is a better result than above cited works.

Table 4.1 TGA details of E-glass/epoxy/NZF composites

S. No. Sample Filler T5% in °C Residue % at

(NZF) 940°C
wt%
1 Neat E- 0 327 42
glass/epoxy
2 NZF 1 10 374 (14% raise w.r.t 53
neat E-glass/epoxy)
3 NZF 2 20 378 (15.5% raise w.r.t 62
to neat E-glass/epoxy )

The differences between the residual masses of the three samples at 940°C clearly

indicated the weight percentage of the filler NZF [225] and shown in Table 4.1. From

that table, the T5% temperatures of NZF1 and NZF2 samples increased by 14 % and

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15.5% compared to the neat E-glass/epoxy composites. It confirmed that the thermal

stability of the E-glass/epoxy/NZF composites was enhanced relative to that of the Neat

E-glass/epoxy composites by increasing the inorganic filler content.

Figure 4.12: TGA curves of E-glass/epoxy/NZF composites

4.5.2 Thermogravimetric analysis of hybrid (MWCNT+NZF) RAMs

The TGA curves of the NZFM 2 and NZFM 4 samples determined according to

ASTM E2550-21 standards at the temperature ranging from 40 0C to 950 0C are shown

in Figure 4.13. The details of T5% values and residue of the composites at 940 0C are

given in the Table 4.2 The input of heat energy initiates the thermal degradation of the

samples at 250 ⁰ C without significant weight loss. From 380–450 0C, a major reduction

in weight occurs, following which termination commences through different reaction

mechanisms that associate radicals from the initial degradation process.

126
 Table 4.2 TGA details of E-glass/epoxy/MWCNT/NZF composites

Sample Filler wt T5% in °C Residue %

% at 9400C
NZFM2 20+0.8 381 62
NZFM4 20+1.6 383 68

Figure 4.13: TGA curves of NZFM composites

The IPDT values were calculated to be 449 ⁰ C and 460 ⁰ C for NZFM 2 and

NZFM 4, respectively. In a previous study by S. E. Lee et al. [337], the decrease in

thermal stability of epoxy composites with the increasing wt % of MWCNT was found

to be due to the poor dispersibiliy and increased aggregation of the filler. In the present

work, the increasing IPDT values (2% increase) with the increasing wt. % of MWCNT

(0.4 %) indicates that the fabricated samples have good thermal stability because of the

increase in contact surface area between the polymer and filler materials. Here the TGA

results are validated with the TGA results obtained in ref [84, 123, 124 and 128]. The

thermal stabilities of polymer based Ti//Fe/MWCNT composites, graphene silica textile

composites, CO/graphene composites, RGO/iron oxide composites were 3300C, 1320C,

3500C and 3600C respectively. As shown in the thermograms, in the present work, the

composites were stable up to 370 ⁰ C which is much greater than earlier research

127
reports mentioned. Such an excellent thermal stability at temperatures higher than 360

⁰ C at > 98 wt. % indicates that these polymeric composites can be utilized in aircrafts

and high-speed vehicles where high temperature resistance is required.

4.6 Summary

This chapter summarizes

1. Spherical morphology, size, crystallinity, saturation magnetization, chemical

composition details of nickel zinc ferrite synthesized by sol-gel auto combustion

method using FESEM, TEM, XRD, VSM, FTIR and EDX.

2. The formation of nano NZF with 26 nm, with no impurities and 52.312 emu/g

saturation magnetization. Furthermore the diameters of two different MWCNT

responsible for aspect ratios of 115 and 315 are also confirmed.

3. Degradation temperatures of magnetic RAMs and hybrid RAMs using TGA.

The advantage of adding the high aspect ratio MWCNT and NZF to epoxy

matrix in terms of thermal stability is explored.

4. All the magnetic and hybrid RAMs have shown thermal stability up to 3000C

which shows the applicability in high temperature service condition of proposed

RAMs..

128
Chapter 5 EM CHARACTERIZATION AND
MULTILAYER ANALYSIS OF RAMs

5.1 Introduction:

The microwave absorption properties of RAMs are determined from the

measurement of complex permittivity and complex permeability which are known as

the electromagnetic characteristics of the RAM. The real and imaginary parts indicate

the storage and dissipation capabilities of absorbing material and they are

electromagnetic wave frequency dependent. In the design of RAM, asorbing properties

can be enhanced by using multi-layered design and the reflection loss of multi-layered

RAMs are obtained from transmission line theory. In this chapter the EM

characterization of fabricated RAMs composed of MWCNT, NZF and combination of

MWCNT and NZF with different aspect ratios of MWCNT in the X-band are obtained

from vector network analyser. The variation in dielectric loss and magnetic loss

tangents with frequency are used to determine the prominent loss mechanisms in the

radar absorbing material.The multi-layered RAM are designed based on the impedance

matching condition and the reflection loss values of total thirty six multi-layered RAMs

are obtained.

5.2 Electromagnetic characterization of RAMs

5.2.1 EM characterization of dielectric (MWCNT) RAMs

Microwave absorption properties depend on basic parameters such as complex

permittivity (𝜖𝑟 = 𝜖 ′ − 𝑗𝜖 " ) and complex permeability(𝜇𝑟 = 𝜇′ − 𝑗𝜇" ), where the

associated real parts are regarded as the storage of electric and magnetic energies and

the imaginary parts serve as the loss and dissipation of both energies. In a lossy

dielectric material the electromagnetic field propagation induces two categories of

129
electrical currents: displacement current and current due to conduction. Interaction of

bound charges i.e. displacement current causing the polarization effect describes the

complex permittivity real part also known as storage capacity of lossy material. The

imaginary part indicates the capacity of dissipation due to free electrons increase

(conduction current) [32 and 162]. Figure 5.1 shows the dielectric permittivity real part

of epoxy -MWCNT composites as a frequency function for different weight

percentages of MWCNT. It is observed that variation in dielectric constant with respect

to change in frequency is negligible and also increase in loading of MWCNT increases

the real part of permittivity as found in previous literature with other carbon materials

also [80 and 165]. This is due to an increase in displacement currents causing the

enhancement of polarization effects. The value of real part for lowest weight percentage

is 3.4 and for the highest loading of MWCNT 2 % gives rise to 5.84 [95, 160 and

318].The variation in imaginary part of the complex permittivity is shown in Figure 5.2.

Figure 5.1: Real values of complex permittivity of MWCNT samples

130
Here the variation with respect to frequency is significant and also the values increases

for higher loadings and it attains a max value of 1.2 at the frequency of 8.2 GHz. The

real and imaginary values of complex permittivity values in ref [162] vary from 0 to

6.2 and 0.1 to 0.5 with an increase in MWCNT weight percentage from 1 to 3 wt%.

Increase in MWCNT content favors the development of conductive network, porosities

formation which leads to the increase in permittivity values. In the research work [165]

the 1 wt% MWCNT (with aspect ratio 325) epoxy composites are having 4 as real

values of complex permittivity and this value is almost constant in the X-band ,which

is coinciding with the present result because of almost same aspect ratio (315). Due to

increase of viscosity with increase in MWCNT weight percentage in the epoxy matrix

higher loadings than 2% were not preferred.

Figure 5.2: Imaginary values of complex permittivity of MWCNT samples

The real values of permeability are shown in Figure 5.3 and increases from 0.224 to

1.2. As shown in the Figure 5.4, the imaginary values are increased from 0.04 to 0.9. In

the literature on RAMs with MWCNTs [112], the real values of permeability change

131
from 0.3 to 1.1 and imaginary values from 0.1 to 0.6, increasing MWCNTs wt% from

0.5 to 2.5%. The research work [176] shows the real and imaginary permeability values

from 1.1 to 1.1 and 0.1 to 0.2 with MWCNTs from 1 wt% to 10 wt%. Figure 5.5, Figure

5.6 shows the average values of the dielectric and magnetic loss tangents of the prepared

samples. Loss tangent is the factor of attenuation to convert the stored energy to the

heat dissipation [30].The absorption improves with the raise in loss tangent. The values

of dielectric loss tangent of MWCNT-epoxy composites increased from 0.06 to 0.23

and the magnetic loss tangent values increased from 0.07 to 0.97. In the previous work,

the values of loss tangents are 0.04 and 0.1 for 1 wt% and 10 wt% MWCNT composites

at 8.2 GHz frequency [176]. Moreover, in the ref [277], the loss tangents of dielectric

RAM vary from 0.1 to 0.5 at 10 GHz, varying the filler percentage from 0 to 0.025.

These findings further confirm the current research results that an increase in weight

percentage of filler leads to an increase in loss mechanisms. Due to increase of viscosity

with increase in MWCNT weight percentage in the epoxy matrix higher loadings than

2% were not preferred.

132
 Figure 5.3: Real values of complex permeability of MWCNT samples

Figure 5.4: Imaginary values of complex permeability of MWCNT samples

133
 Figure 5.5: Dielectric loss tangents of MWCNT samples

Figure 5.6: Magnetic loss tangents of MWCNT samples

5.2.2 EM characterization of magnetic (NZF) RAMs

The real and imaginary complex permittivity (𝜀 ′ , 𝜀 ′′ ) and complex permeability

(𝜇 ′ ,𝜇 ′′ ) values represent the storage and dissipation capabilities of radar absorbers.

134
Figures 5.7 a) & 5.7 b) and Figures 5.8 a) & b) shows the variations in the measured

complex permittivity and permeability values with frequency in the X-band range. The

variations in the real permittivity values (i.e., the dielectric constant) remain almost

constant throughout the X-band and mainly depend on the amount of intrinsic dipolar

polarization in the material. Maximum and minimum values of 4.7 and 4.3 were

achieved for sample NZF1 at 11.6 and 12.4 GHz, respectively, while sample NZF2

exhibited a maximum value of 5.8 at 12.4 GHz. Sample NZF3 exhibited smaller values

of 𝜀 ′ than those of the other samples. The imaginary values of the samples 𝜀 ′′ range

from 0.7 to 0.1 and their plot exhibits a decreasing tendency with increasing frequency.

The 30 wt% filler loading in NZF/epoxy composites exhibited real and imaginary

values as 4 and 0.01 in the entire X-band [244] which are less than the present work

results. This may be due to larger particle size in the above mentioned research work

compared the particle size of synthesized NZF in this work. According to Pan et al.,

the respective ion and electron polarizations occur at frequencies outside of the

microwave range [39]. For heterogeneous systems, including nanocomposites,

polarization occurs at the interface between the polymer matrices and nanofillers.

Therefore, for the fabricated samples, electric dipolar polarization and interfacial

polarization are the main causes for the dissipation of the electric-energy component.

135
 Figure 5.7: a) Real values of Complex permittivity of NZF samples

Figure 5.7: b) Imaginary values of Complex permittivity of NZF samples

136
 Figure 5.8: a) Real values of Complex permeability of NZF samples

Figure 5.8: b) Imaginary values of Complex permeability of NZF samples

137
 The real permeability value (𝜇 ′ )ranges from 1.5 to 0.6, with the highest value

observed in sample NZF2. The imaginary values ( 𝜇 ′ ′) range from 0.4 to 0.3 and the

maximum value was achieved for sample NZF3. In the research work [244], the real

and imaginary values of complex permeability of nickel zinc ferrite polymer

composites varies non linearly in the similar manner to the current research. In all three

samples, the real permeability increased with frequency. Sample NZF2 exhibits a

resonance peak at 11.4 GHz, which then shows a decreasing trend. In this work, at

higher frequencies, the imaginary permeability values decrease with increasing

frequency as the magnetic dipole realignment becomes too difficult with the external

field [73].The magnetic loss in absorbing materials is caused by eddy-current loss,

magnetic hysteresis, natural resonance, domain-wall resonance and exchange-wall

resonance. The electrical conductivity (σ) and thickness (d) of the composites influence

the eddy-current loss and are expressed by

𝝁′′ (𝝁′ )−𝟐 𝒇−𝟏 = 𝟐𝝅𝝁𝟎 𝒅𝟐 𝝈 5.1

where 𝜇0 is the permeability of a vacuum [87]. As inferred in previous research,

if the frequency changes and the evaluated values of 𝜇 ′′ (𝜇 ′ )−2 𝑓 −1 remain constant,

then the magnetic loss is induced by the eddy-current loss [89]. In this study, the

observed values of the composites are not constant with frequency as depicted in Figure

5.9. Therefore, the eddy-current loss has no significant effect on the microwave-

absorption properties. At higher frequencies, like those in the GHz range, irreversible

magnetization causing hysteresis loss is negligible. Additionally, for single-domain

NZF nanoparticles, the domain-wall resonance typically observed in multi-domain

materials can be ignored [193]. Therefore, the remaining natural and exchange

resonances are the causes of magnetic loss exhibited by the fabricated samples.

138
 Figure 5.9: Dependence of 𝝁′′ (𝝁′ )−𝟐 𝒇−𝟏 on frequency for NZF composites

To further understand the absorption properties, the loss tangents of the

absorption materials were explored. Wang et al. [206] found that lossy materials should

exhibit high magnetic and dielectric loss to achieve excellent microwave absorption.

Figure 5.10 shows the frequency dependence of the dielectric and magnetic loss

tangents, which are the ratios of the imaginary complex permittivity and permeability

values to their real values, respectively [41 and 152]. The largest dielectric and

magnetic loss values were observed for sample NZF3, indicating that it possesses better

absorption properties. As demonstrated in previous work [39], magnetic loss has a more

dominant effect on radar absorption. For the prepared composites, as the values of

‘tan𝛿𝑀 ’ exceed those of ‘tan𝛿𝐸 ’, magnetic loss contributed more to microwave

absorption than dielectric loss. This scenario is similar to the results obtained in other

magnetic RAMs prepared by cobalt zinc ferrite and Ti doped lithium zinc ferrite epoxy

composites [41 and 182].

139
 Figure 5.10: Loss tangents of NZF samples

5.2.3 EM characterization of combined (MWCNT+NZF) RAMs

The frequency dependence of the permittivity and permeability of the fabricated

high aspect ratio hybrid samples is illustrated in Figure 5.11 to 5.14. With the increasing

frequency, the variation of the imaginary part of the complex permittivity is almost

constant, whereas the real part increases slightly. The real and imaginary parts of

permittivity depend on the amount of polarization occurring in the material. The values

of real and imaginary permittivity increase from 3.9 to 4.7 and 0.25 to 0.65,

respectively, with the increase in wt. % of MWCNT [92 and 94]. The increase in

MWCNT wt% in manganese ferrite/epoxy composites results in enhancement of

permittivity values as occurred in the current research [80]. The polarization

mechanisms responsible for the dielectric performance of an absorbing material are due

to the relative displacement of the electron cloud and nuclei, separation of positive and

negative ions, dipolar orientations and interfacial effects. In the microwave frequency

range, electronic and atomic mechanisms are comparatively weak and normally

constant.

140
 Figure 5.11: Real values of complex permittivity of NZFM samples

Figure 5.12: Imaginary values of complex permittivity of NZFM samples

According to the free electron theory, imaginary permittivity, 𝜖 " , is given by the
summation of polarization relaxation (𝜖𝑝 " ) and conduction loss ( 𝜖𝑐 " ) [219].
𝟐𝝅𝒇𝝉 𝟏
𝝐" = 𝝐𝒑 " + 𝝐𝒄 " = (𝝐𝒔 − 𝝐∞ ) + 5.2
𝟏+(𝟐𝝅𝒇)𝟐 𝟐𝝅𝝐𝟎 𝝆𝒇

141
 where 𝜖0 , 𝜖∞ , 𝜖𝑠 , 𝜌, 𝑓 𝑎𝑛𝑑 𝜏 denote the permittivity in vacuum, relative

permittivity at high-frequency limit, static permittivity, electrical resistivity, frequency

and polarization relaxation time, respectively. The presence of MWCNT is conducive

for the formation of dipole moments because the directional migration of positive and

negative charges was restricted, leading to dipolar polarization. The multiple interfaces

between MWCNT/epoxy, MWCNT/NZF and NZF/epoxy hinder the charge transfer,

resulting in charge accumulation, thereby promoting interfacial polarization. The NZF

nanoparticles predominantly contributed to this polarization because of their nano size

and the larger number of active atoms at the surface provided larger specific area and

enhanced the heterogeneous interfaces with epoxy and MWCNT. A noticeable increase

in the value of 𝜖 " with the increase in wt. % of MWCNT indicates increased

conductivity due to decreased resistivity, resulting in conduction loss [2 and 216].

Figure 5.13: Real values of complex permeability of NZFM samples

142
 Figure 5.14: Imaginary values of complex permeability of NZFM samples

In general, magnetic loss at higher frequencies in a lossy material occurs due to

the exchange resonance, natural resonance and eddy current effect. The loss caused by

the eddy current effect is related to the thickness (d) and electrical conductivity (σ) of

the composites and is expressed by 𝜇 " (𝜇 ′ )−2 𝑓 −1 = 2𝜋𝜇0 𝑑 2 𝜎, where 𝜇0 is the

permeability of vacuum [225 and 338-339]. If the values of 𝜇 " (𝜇 ′ )−2 𝑓 −1 remain

constant even when the frequency changes, it can be inferred that eddy current effects

cause the magnetic loss. With varying frequency, the observed values of the composites

are almost constant without any fluctuations (Figure 5.15); therefore, it can be

confirmed that eddy current loss is the reason behind magnetic loss. The real part of the

complex permeability changes from 0.85 to 1.28 and the imaginary part from 0.4 to

0.78; the rate of increase in this case is smaller than that in the case of permittivity,

because MWCNT are dielectric materials. Both the imaginary parts 𝜖 " and 𝜇 " are greater

than zero, indicating that better absorption occurs due to the combined effect of

dielectric and magnetic losses.

143
Figure 5.15: Dependence of 𝝁′′ (𝝁′ )−𝟐 𝒇−𝟏 on frequency for NZFM composites

Figure 5.16: Dielectric loss tangents of NZFM samples

144
 Figure 5.17: Magnetic loss tangents of NZFM samples

To explain the reasons more clearly for microwave absorption, the dielectric

𝜖" 𝜇"
and magnetic loss tangents, i.e., tan 𝛿𝐸 = 𝜖′ and tan 𝛿𝑀 = 𝜇′ , were measured and

plotted (Figure 5.16 and Figure 5.17). The influential material in the loss mechanism

in determined from the magnetic and dielectric loss tangent values in a hybrid RAM

[80 and 236]. In the research work [216] cobalt zinc ferrite/N-doped MWCNT epoxy

composites, the magnetic loss exceeded the dielectric loss and similar behavior is

observed in the current research. From the loss tangent graphs for the prepared

composites, the values of tan𝛿𝑀 exceed those of tan𝛿𝐸 , establishing that the magnetic

loss provided by the NZF nanoparticles is the major contributor for microwave

absorption. As stated in the introduction, it was confirmed that inclusion of the

magnetic materials intrinsically enhances the magnetic permeability, resulting in

greater magnetic loss.

145
 Figure 5.18: Complex permittivity of NMWCNT samples

The possible mechanism of radar absorption of low aspect ratio hybrid samples

was investigated with the help of the real and imaginary part of complex permittivity

and permeability. Figure 5.18 shows the real and imaginary parts of complex relative

permittivity spectra for all five sample respectively. The real part of relative complex

permittivity of composites varies from 3 to 4.98. The maximum value was obtained for

sample NMWCNT 5 as it contains 2.5 wt% of MWCNT .The real part of the

permittivity increases with increase in frequency as shown in Figure 5.18. The

MWCNT cause a rapid increase of real permittivity which was in the range from 9.2

GHz to10.2 GHz. The imaginary part of complex relative permittivity varies from 0.02

to 1.98 lowest values are obtained for sample NMWCNT 1 since it contains low filler

concentration of MWCNT as 0.5%.The increase in real and imaginary permittivity with

increase in frequency is attributed to enhancement of interfacial polarization.

146
 Figure 5.19: Complex permeability of NMWCNT samples

The real part of complex relative permeability increases from 1.0 to 1.6 for

different weight % of MWCNT and for each composite the values are declining with

increase in frequency as shown in Figure 5.19. The variations in imaginary part of

relative permeability are also shown in Figure 5.19.

The values are declining for all composites with increase in frequency. The

dielectric and magnetic loss tangents were shown in Figure 5.20 and Figure 5.21 As

observed from these figures, the magnetic loss dominates compared to dielectric loss in

these low aspect ratio hybrid composites like high aspect ratio hybrid composites. In

the literature R.Shu [219] et.al, showed that the enhancement of permittivity and

permeability occurs similar to the present work, due to the addition of dielectric fillers

RGO in the Fe3O4-C/RGO hybrid RAMs. In this work, the major contribution of loss

mechanism is by the dielectric filler carbon and RGO compared to the ferro ferric oxide.

147
The EM properties of MWCNT+NZF samples are validated with the previous research

works [80, 81 and 94]

Figure 5.20: Dielectric loss tangents of NMWCNT samples

148
 Figure 5.21: Magnetic loss tangents of NMWCNT samples

5.3 Multilayer Analysis of RAMs

Multilayer radar-absorbing materials exhibit better performance than single-layered

materials due to the possibility of multiple internal reflections and the absorption of incident

waves by lossy materials [2, 26, 60 and 172]. The reflection losses of the multi-layered

radar-absorbing materials were determined using a MATLAB code developed

according to the transmission line theory given by [60 and 193]

(𝒁 −𝒁𝒂 )
𝑹. 𝑳. = 𝟐𝟎𝒍𝒐𝒈 |(𝒁𝒊 | 5.3
𝒊 +𝒁𝒂 )

Where ‘Zi ‘ is the input impedance at the first air-absorbing interface and ‘Za ‘ is

the free-space impedance. For each layer i, the impedance of the input wave of the

multi-layered structure backed by a perfect electrical conductor (PEC) as shown in

Figure 5.22 is expressed as [26 and 112]

149
 (𝒁 𝒄𝒐𝒔𝒌𝒊 𝒕𝒊 +𝒋𝜼𝒊 𝒔𝒊𝒏𝒌𝒊 𝒕𝒊 )
𝒁𝒊 = 𝜼𝒊 {(𝜼𝒊+𝟏 } 5.4
𝒊 𝒄𝒐𝒔𝒌𝒊 𝒕𝒊 +𝒋𝒁𝒊+𝟏 𝒔𝒊𝒏𝒌𝒊 𝒕𝒊 )

Where ‘ηi ‘ and ‘ti ‘ are the values of the intrinsic impedance and thickness of

the ith layer, respectively. The propagation constant ki is expressed as

𝒌𝒊 𝟐 = (𝟐𝝅𝒇)𝟐 𝝁𝟎 𝝐𝟎 𝝁𝒓𝒊 𝝐𝒓𝒊 5.5

Where ′𝑓′ is the electromagnetic wave frequency, 𝜇0 and 𝜖0 denote the free-

space permeability and permittivity, respectively and 𝜇𝑟𝑖 and 𝜖𝑟𝑖 are the relative

permeability and permittivity of the ith layer estimated by the vector network analyzer

measurements, respectively. As indicated by equation 5.3, to achieve maximum

reflection loss, the impedance of the input wave should be equal to the impedance of

free space. A favorable impedance match and moderate attenuation will result in better

absorption properties [167 and 188]. When designing double-layered RAMs based on

the impedance matching condition, the first layer must be the matching layer, while the

second is the absorbing layer that absorbs the maximum electromagnetic wave energy.

Figure 5.22: Multi-layer Radar absorbing structure

5.3.1 Multilayer analysis of dielectric (MWCNT) RAMs

The details of double layered RAMs with a thickness of 1 mm for the first layer

and 2 mm for the second layer were considered for numerical simulation as shown in

Table 5.1

150
 Table 5.1 Various double layered MWCNT Radar Absorbing Materials

S. No. Sample First layer Second layer

1 MRAS 1 MWCNT 0.4 MWCNT 0.8
2 MRAS 2 MWCNT 0.4 MWCNT 1.2
3 MRAS 3 MWCNT 0.4 MWCNT 1.6
4 MRAS 4 MWCNT 0.4 MWCNT 2
5 MRAS 5 MWCNT 0.8 MWCNT 1.2
6 MRAS 6 MWCNT 0.8 MWCNT 1.6
7 MRAS 7 MWCNT 0.8 MWCNT 2
8 MRAS 8 MWCNT 1.2 MWCNT 1.6
9 MRAS 9 MWCNT 1.2 MWCNT 2
10 MRAS 10 MWCNT 1.6 MWCNT 2

The reflection loss values of the proposed radar absorbing materials with a

thickness of 3 mm in the X-band were shown in Figure 5.23. In the research work [112],

a four layered RAS with MWCNTs with maximum filler loading of 2.5 wt% exhibited

-10 dB R.L for the entire X band and a maximum R.L of -29 dB at 11.5 GHz with a

thickness of 8 mm. A maximum R.L of -24 dB at 11.3 GHz and -5 dB R.L in the X-

band was shown by MWCNT/epoxy nanocomposites with 4 mm thickness in the

research work [161]. In the current research, the three composites RAS 10, RAS 9 and

RAS 5 has exhibited a band width of 3.8 GHz with a reflection loss of -10 dB i.e. from

8.2 GHz to 12.0 GHz corresponding to 90% absorption and at central frequency of 9.8

GHz shown -18 dB RL . These results are showing better microwave absorption

properties of dielectric RAM compared to the above mentioned literature may be due

proper impedance matching and attenuation constant values. Out of all the radar

absorbing material RAS 8 maintained -10 dB in the entire frequency range of the X-

band. RAS 6 and RAS 3 has reflection loss -10 dB for band width of 3.4 GHz and at

central frequencies of 10.6 GHz and 11.0 GHz exhibited reflection loss of -32 dB and

-35 dB respectively corresponding to 99% absorption of incident electromagnetic

radiation. Here MRAS 3, 6 and 8 are having MWCNT 1.6 wt% as second layer and 0.4,

0.8, 1.2 wt% of MWCNT as first layers respectively. Therefore their attenuation

151
constant values are same and they are having similar patterns of reflection loss. But due

to difference in the first layers impedances they are having different reflection loss

values. The same is happening in case of MRAS 4, 7, 9 and 10. They are having

MWCNT 2 wt% as second layer and 0.4, 0.8, 1.2 and 1.6 wt% of MWCNT as first

layers respectively. All the dielectric RAMs except RAS 1 displayed a reflection loss

of more than -5 dB.

Figure 5.23 Reflection loss of double layered MWCNT RAMs

5.3.2 Multilayer analysis of magnetic (NZF) RAMs

The proposed two-layered radar-absorbing materials based on the impedance

matching condition are composed of E-glass/epoxy/NZF with a PEC as the final layer,

as summarized in Table 5.2.

Table 5.2 Details of the double layered NZF RAMs

S. No. Sample First layer Second layer

1 NRAS 1 NZF 1(1 mm) NZF 2(2 mm)
2 NRAS 2 NZF 1(1 mm) NZF 3(2 mm)
3 NRAS 3 NZF 2(1 mm) NZF 3(2 mm)
4 NRAS 4 NZF 1(2 mm) NZF 2(2 mm)

152
 5 NRAS 5 NZF 1(2 mm) NZF 3(2 mm)
6 NRAS 6 NZF2(2 mm) NZF 3(2 mm)
The RL dependence of the E-glass/epoxy/NZF RAMs in the X-band frequency is

shown in Figure 5.24. A double layered NZF polymer based composites with a thickness

of 1.72 mm resulted in a maximum R.L of -43 dB at 9.6 GHz [60]. The epoxy based NZF

composites shown a maximum R.L of -18 dB at 9.5 GHz with 3.5 mm thickness [181]. In

the present work, microwave absorption corresponding to a reflection loss of -10 dB, which

is considered suitable for a microwave absorber, was observed in RAS 5 and RAS 6, with a

thickness of 4 mm. The better absorption properties of present magnetic RAM compared to

ref [181] are due to its smaller size of NZF (26 nm) compared to literature NZF size (37

nm). In a recent study [206], a 3-GHz bandwidth and an RL of -33 dB at 17.6 GHz were

achieved; however, a high weight percentage (60%) of magnetic filler was required. In this

work, RAS 5 exhibited a maximum RL of -33 dB at a frequency of 9.6 GHz consisting of

10 and 25 wt% of NZF in the first and second layers, respectively. Additionally, a maximum

RL of -10 dB for the bandwidth of 2.4 GHz (8.2 - 10.6 GHz) was observed for this structure.

Figure 5.24: Reflection loss of double layered NZF RAMs

153
 The superior performance observed in RAS 5 is due to the impedance matching of

the first layer (NZF1) and the absorbing layer (NZF3). By studying the electromagnetic

properties, it was confirmed that NZF3 is suitable as the absorbing layer material as it

exhibits high magnetic and dielectric loss values. An RL exceeding -15 dB for a bandwidth

of 1.0 GHz (8.2-9.2 GHz) was achieved by RAS 6. The poor results observed for the

remaining RAMs are due to the poor impedance matching and improper matching of the

electromagnetic parameters. The microwave absorption properties of NZF RAM are

comparable with RL values of past research works on magnetic RAMs [60, 88, 181 and

331].

5.3.3 Multilayer analysis of RAMs with low aspect ratio MWCNT and NZF

In general, a multilayer RAM is characterized by a set of layers with different

microwave absorbing materials to enhance the overall absorption features. One of the

main issues for the design of such absorbers lies in the minimization of the overall

reflection coefficient in a specific frequency range and a specific range of incidence

angles. The front layer is expected to give the best impedance match while the

absorbing layer is supposed to dissipate the microwave energy as much as possible and

the last layer is expected to be reflective to simulate actual operation conditions, i.e. it

must be Perfect Electric conductor. The designed multilayer structure is based on four

layers of different weight percentages of MWCNT and Nickel Zinc Ferrite

nanomaterials and Epoxy and PEC were taken as first layer and last layers respectively.

The details of four layered RAMs are shown in Table 5.3.

Numerical simulations are performed in order to assess how the use of Nickel

zinc ferrite and MWCNT as filler affects the EM performance of the RAMs. The values

of reflection loss for four layered RAMs with different weight percentages of fillers

154
were determined as shown in Figure 5.25 by using impedance matching condition and

transmission line theory.

All the RAMs have shown good radar absorbing properties more than 5 dB trough out

the- band. The hybrid RAM with MWCNTs and Ti/Fe exhibited -10 dB R.L for a band

width of 3 GHz [84]. The MWCNT/NiFe RAMs shown -12 dB R.L for a bandwidth of

1.6 GHz [94]. Where as in the current research, out of all the four layered RAMs based

on Nickel Zinc Ferrite and MWCNT, better microwave absorption is observed for RAS

10 and RAS1 which is attributed to surface anisotropy of Nickel Zinc Ferrite

nanoparticles which are spherical in shape, dielectric losses of the conductive and

magnetic fillers, layer order

155
 Table 5.3 Details of the four layered low aspect ratio MWCNT and NZF RAMs

S. No. Sample First layer Second layer Third layer Fourth layer
1 RAS 1 Epoxy NMWCNT 1 NMWCNT 2 NMWCNT 3
2 RAS 2 Epoxy NMWCNT 1 NMWCNT 2 NMWCNT 4
3 RAS 3 Epoxy NMWCNT 1 NMWCNT 2 NMWCNT 5
4 RAS 4 Epoxy NMWCNT 1 NMWCNT 3 NMWCNT 4
5 RAS 5 Epoxy NMWCNT 1 NMWCNT 3 NMWCNT 5
6 RAS 6 Epoxy NMWCNT 1 NMWCNT 4 NMWCNT 5
7 RAS 7 Epoxy NMWCNT 2 NMWCNT 3 NMWCNT 4
8 RAS 8 Epoxy NMWCNT 2 NMWCNT 3 NMWCNT 5
9 RAS 9 Epoxy NMWCNT 2 NMWCNT 4 NMWCNT 5
10 RAS 10 Epoxy NMWCNT 3 NMWCNT 4 NMWCNT 5

Figure 5.25: Reflection loss of low aspect ratio E-glass/epoxy/MWCNT/NZF RAMs

and thickness of the layers. RAS 1 at central frequency of 12.0 GHz shown the max

reflection loss of -31 dB and -15 dB corresponding to 95 % absorption for a bandwidth

of 1GHz. RAS 10 exhibited the reflection loss as -14 dB at central frequency of 10.2

GHz and -5dB for entire band ,-10 dB (90 % absorption) for more than 3 GHz

bandwidth was maintained.

156
5.3.4 Multilayer analysis of RAMs with high aspect ratio MWCNT and NZF

The two following conditions must be considered when designing double-

layered RAM for optimum performance: (a) the first layer must satisfy the impedance

matching condition, i.e., its impedance should be closer to the impedance of free space,

𝑍
or the normalized characteristic impedance |𝑍 𝑖 | value should be close to 1, so that the
𝑎

reflection at the air–absorber interface is minimal; (b) the second layer, known as the

absorber layer, must absorb the maximum amount of microwave radiation from the first

layer, i.e., it must possess the maximum attenuation constant value, α, given by the

following equation [267]:

α=√𝟐𝝅𝒇
𝑪
∗ √(𝝁" 𝝐" − 𝝁′ 𝝐′ )𝟐 + √(𝝁" 𝝐" − 𝝁′ 𝝐′ )𝟐 + (𝝐′ 𝝁" + 𝝐" 𝝁′ )𝟐 5.6

Different possible two-layered RAMs having thicknesses of 1 mm and 2 mm

for the first and second layers, respectively, with PEC as the final layer (Table 5.4),

were analyzed for microwave absorption.

The RL values obtained for the double-layered RAMs from the measured

complex permittivity and permeability of the samples are shown in Figure 5.26. With

the increasing weight percentage of MWCNT, the RL curves shift toward the lower

frequency range. Of all the RAMs, NMRAS 10, which has a matching thickness of 3

mm, exhibited an RL of -16 dB (94% absorption of EM waves) for a bandwidth of 2.2

GHz (8.4–10.6 GHz) and a maximum RL of -22 dB at 9.6 GHz. Zhang et al. [338]

reported that Co–C nanofibers with 50 wt. % of filler exhibited a maximum RL of -40

dB at 7.1 GHz and < -10 dB for 1 GHz bandwidth with a thickness of 2.4 mm.

157
 Table 5.4 Details of the double layered high aspect ratio MWCNT and NZF RAMs
S. No. Sample First layer Second layer
1 NMRAS 1 NZFM 1 NZFM 2
2 NMRAS 2 NZFM 1 NZFM 3
3 NMRAS 3 NZFM 1 NZFM 4
4 NMRAS 4 NZFM 1 NZFM 5
5 NMRAS 5 NZFM 2 NZFM 3
6 NMRAS 6 NZFM 2 NZFM 4
7 NMRAS 7 NZFM 2 NZFM 5
8 NMRAS 8 NZFM 3 NZFM 4
9 NMRAS 9 NZFM 3 NZFM 5
10 NMRAS 10 NZFM 4 NZFM 5

Here, note that the absorption bandwidth is more important than the intensity of

the absorption peak in many practical applications; to realize a wide absorption

bandwidth, the filler morphology and performance control are being actively studied.

In this part of present work, the NMRAS 3, 4, 6, 7, 8, 9 and 10 showed RL values of -

10 dB for a bandwidth of 4 GHz. All the samples exhibited an RL of more than -6 dB

over the entire frequency range. The obtained reflection loss values are comparable to

literature results [62, 284 and 286]. Detailed comparisons with literature are shown in

Table 6.19 in the next section.

To further investigate the causes of the RL of the double-layered materials, their

normalized characteristic impedance and attenuation constant values (α) were evaluated

(Figure 5.27 and 5.28). The research works [41 and 206] demonstrated that the RAMs

with high attenuations constant values are resulting in betters RAMs compared to

RAMs having lower attenuation constant values. The characteristic impedance values

and attenuation constant values are used in the previous works [2, 216 and 246] to

design the multilayered RAMs. Here in the present work, the superior performance of

NMRAS 10 can be primarily attributed to the impedance matching condition of its first

layer (NZFM 4), i.e., the normalized characteristic impedance of the first layer of

NMRAS 10 is close to 1 and secondarily to the highest attenuation constant of the

absorber layer (NZFM 5). Therefore, this RAM, consisting of lightweight MWCNT as

158
the dielectric material and NZF as the magnetic material and having a thickness of 3

mm, is promising as a lightweight microwave absorber in the X-band.

Figure 5.26: Reflection loss of high aspect ratio E-glass/epoxy/MWCNT/NZF RAMs

Figure 5.27: Normalized characteristic impedance values of NZFM samples

159
 Figure 5.28: Attenuation constant values of NZFM samples

Figure 5.29: Absorption mechanism in MWCNT/NZF composites

160
5.3.5 Absorption mechanism in hybrid (MWCNT+NZF) RAM

The possible mechanisms of the microwave absorption of the MWCNT/NZF

nanocomposites are illustrated in Figure 5.29. Here, normal incidence of microwaves

is assumed. First, the high aspect ratio and conductivity properties of the MWCNT

induced the conduction loss and dipolar polarization in the fabricated samples. Second,

the multiple heterogeneous interfaces between MWCNT/epoxy, MWCNT/NZF and

NZF/epoxy developed numerous polarization centers that caused notable interfacial

polarization, resulting in greater dielectric energy loss. Third, the NZF nanoparticles

enhanced the magnetic loss by causing eddy current loss, thereby enhancing the

absorbing properties. Finally, the double-layered materials provided the impedance

matching and attenuation characteristics required for an efficient and thin microwave

absorber due to the synergistic effects of MWCNT and NZF.

5.4 Summary

This chapter summarises

1. Variations of complex permittivity and permeability values of different types

of RAMs with respect to X-band frequency and their magnetic and dielectric

loss tangent values.

2. Multilayer analysis of MWCNT, NZF and hybrid MWCNT and NZF radar

absorbing materials with different thicknesses and combinations of the layers.

3. Possible absorption mechanisms such as dielectric and magnetic loss

mechanisms, impedance matching condition, attenuation constants responsible

for reflection loss of multi-layered RAMs.

161
Chapter 6 SELECTION OF RAM USING MCDM
METHODS AND IT’S MECHANICAL
PROPERTIES
6.1 Introduction

The multi criteria decision making (MCDM) methods are most useful

techniques in the selection of planning and designing process or choosing the best

alternative from available systems [134, 293 and 302]. From the previous chapter, the

multilayer analysis of fifteen materials composed of MWCNT, NZF and

MWCNT/NZF, five of them namely MRAS 8, MRAS 6, MRAS 3, NRAS 5 and

NMRAS 10 are showing better performance in terms of @15 dB, @10 dB reflection

loss bandwidths in frequencies, maximum reflection loss (peak of the reflection loss

curve) and thickness. The performance values of the RAMs are tabulated in Table 6.1.

As observed from the table, no single RAM is having optimum values in all the above

said performance criteria. Therefore to select one RAM, MCDM methods are needed

to be implemented [142, 292, 296 and 304].

In MCDM methods, criteria weights are the relative importance of each criteria

given by DM, which are significantly influencing the outcome of a decision making

process. Incorrect evaluation of these may leads to unpredicted results [132 and 141].

The techniques used to determine the criteria weights are classified as subjective,

objective and combinative based upon the data availability and intervention of decision

maker (DM) [137 and 295]. In this work, AHP (Analytical Hierarchy Process) and

entropy methods were utilized to determine the subjective and objective weights and

compromised criteria weights are determined to include both subjective and objective

weights. By using these compromised criteria weights, three MCDM methods TOPSIS

(Technique for Order Performance by Similarity to Ideal Solution), VIKOR

162
(Vlsekriterijumska optimizacija Ikompromisno Resenje) and PROMETHEE-II

(Preference Ranking Organization Method for Enrichment Evaluations) are utilized to

choose the one alternative from the five RAMs. After selecting the RAM, its

mechanical properties tensile, flexural and impact strength and hardness were

determined to evaluate its suitability to act as radar absorbing structure.

Table 6.1 Performance details of the RAMs considered for MCDM methods

S. Nanofiller Sample Bandwidth Bandwidth Maximum Thickness

No. @15 dB @10 dB RL (dB) (mm)
(GHz) (GHz)

1 MRAS 8 2 4 -29 3
MWCNT
2 MRAS 6 1.8 3.6 -31 3

3 MRAS 3 1.8 3.2 -34 3

4 NZF NRAS 5 1.2 2.2 -34 4

5 MWCNT/NZF NMRAS 10 2.6 4 -22 3

6.2 Subjective Weights by AHP

The AHP method, developed by Saaty, converts the complex problems into

number of criteria, sub criteria and alternatives hierarchically so that decision maker

can select the best alternative through a simple process [298 and 303]. Here the

preferences of DM in the form of matrix representing the pairwise comparisons of

criteria are expressed. This enables the determination of criteria weights and ranking of

alternatives by utilizing the subjective aspects of the complex problems. Like AHP,

techniques including ANP, BMW and MDL etc. are used to determine the subjective

weights of the criteria by considering opinion of the experts. The AHP has advantages

like simplicity and robustness in determining the subjective weights. It also

incorporates the consistency checking of decision maker’s evaluation by calculation of

163
a parameter known as consistency ratio [3 and 133]. But this method is not feasible in

case of many alternatives are to be analysed as more number of comparisons are needed.

In order to implement the AHP method and to make pair wise comparisons of

the selected criteria, five members group was constituted. Two members of the group

are scientists from defence research and three are researchers in the field of EMI

shielding and microwave absorbers. After several discussions among the group, a

common opinion was arrived on pair wise comparison matrix. The stepwise procedure

followed in the AHP method is discussed

Step 1: -Pairwise comparison matrix formation

The pair wise comparison matrix is first formed with size as n X n where ‘n’ is

the number of performance criteria in the given problem. In this work four performance

criteria were selected to choose the RAM with strong absorption and low thickness in

the X-band region. They are @15 dB, @10dB bandwidths, maximum reflection loss

and thickness. Therefore the size of the pairwise comparison matrix is 4X4.

Step-2: -Quantifying the pair wise comparisons of criteria using Saaty’s scale

To perform the comparisons of criteria in pairwise, Saaty proposed a numerical

scale of relative importance [298 and 309]. The scale varies from 1to 9 indicating the

importance of one criterion over the other criterion in the selected pair. It helps the

decision maker to express the qualitative opinions in quantitative form. For example

equally preferred is expressed by giving a value of 1 in the pair wise comparison matrix.

In this work the strong preference of 15 dB bandwidth compared to min RL is indicated

by 3 in the corresponding cell of the pairwise comparison matrix. The details of the

164
scale and its verbal indications are shown in Table 6.2 and the pair wise comparison

matrix for the present work is shown in Table 6.3.

Table 6.2 Saaty’s scale for comparison

S. No. Numerical Verbal judgments

Description
value of preferences
1 Two activities contribute equally to
1 Equally preferred
the objective
2 Moderately Experience and judgment slightly
3
preferred favour one activity over another
3 Experience and judgment strongly
5 Strongly preferred
favour one activity over another
4 Experience and judgment very
Very strongly
7 strongly favor one activity over
preferred
another
5 Experience and judgment are of the
highest possible order of
9 Extremely preferred
affirmation in terms of favour one
activity over another
6 Intermediate
preferences between When compromise in preference is
2,4,6,8
the two adjacent needed
judgments

Table 6.3 Pair wise comparison matrix

15dB 10dB Maximum Thickness

bandwidth bandwidth RL
15 dB
1 3 5 5
bandwidth
10 dB
1/3 1 3 3
bandwidth
Maximum RL 1/5 1/3 1 3
Thickness 1/5 1/3 1/3 1

165
 Step-3: -Finding the criteria weights

The criteria weights are determined by first performing the normalization of

decision matrix. The normalization is a transformation method used to convert the

entities in the decision matrix with different units to numerical data using a common

scale. Here in this work Saaty’s suggested columns normalization method is used. In

that process, adding the values in each column of pairwise matrix and then division of

each element in the matrix by the corresponding sum obtained for each column results

in normalized pair wise comparison matrix. Finally adding all the elements in each row

of this matrix and divide with number of elements in each row gives the criteria weights

or subjective weights by AHP method. The normalized pair wise matrix and criteria

weights obtained by AHP method is shown in Table. 6.4 & 6.5.The highest weightage

of 0.54 is obtained for 15 dB bandwidth corresponding to 97% microwave absorption.

Table 6.4 Normalized pair wise matrix

15 dB bandwidth 10 dB bandwidth maximum RL Thickness

15 dB
0.57692 0.64285 0.53571 0.41666
bandwidth
10 dB
0.19230 0.21428 0.32142 0.25
bandwidth
Maximum RL 0.11538 0.07142 0.10714 0.25
Thickness 0.11538 0.07142 0.03571 0.08333

Table 6.5 Weightages of performance criteria

S. No. Performance characteristics Weightages

1 15 dB bandwidth 0.54
2 10 dB bandwidth 0.24
3 Maximum RL 0.14
4 Thickness 0.08

Step-4: -Consistency check of pair wise comparisons

166
 In the process of determining the criteria weights by AHP method, the

judgement of DM is the most important aspect. Its consistency can be found by

parameter namely consistency ratio (CR) which is given by Saaty in terms RCI

(Random Consistency Index) and CI (consistency Index) as expressed by following

equation.

𝐂𝐈
𝐂𝐑 =
𝐑𝐂𝐈
6.1

𝛌𝐦𝐚𝐱−𝐧
𝐂𝐈 =
𝒏−𝟏
6.2

Where n= pairwise matrix order and λmax= max. principal Eigen values of comparison

matrix

The λmax is obtained by first multiplying the criteria weights column by each

row of pairwise comparison matrix [302]. Then each element in the resulting column

matrix is divided by the corresponding criteria weights and adding all the elements then

dividing with number of elements or order of the pairwise comparison matrix resulted

the value of λmax as 4.20. The RCI (Random Consistency Index) value depends on the

order of the matrix and are given in the Table. 6.6. If the CR ratio is ≤0.1, then the DM

judgement is accepted. Otherwise new comparison matrices have to be formed until it

satisfies the CR requirement. The consistency ratio obtained for the above pair wise

comparison matrix is 0.08, which confirmed the consistency of present DM judgement.

The subjective weights of criteria obtained from AHP in ref [139] are 0.5173, 0.1680,

0.0771 & 0.2375; this indicates that out of four criteria (compressive strength,

instantaneous density coefficient, instantaneous hardening exponent and formability

index), the criteria having a maximum value of subjective weight, i.e., compressive

strength is most significant in the selection of Al/SiC composite for workability and

strength combination. The research work [158] is regarding the water absorption

167
parametric selection for ship full applications; here, the five criteria subjective weights

are calculated as 0.55, 0.55, 1.3, 0.94 and 1.65 mentioning the importance of first

criteria initial weight over the remaining. The subjective weights obtained from AHP

in the present work for four criteria, i.e., -15 dB bandwidth, -10 dB bandwidth,

maximum reflection loss and minimum thickness are 0.54, 0.24, 0.14 & 0.08,

respectively, indicating that -15 dB bandwidth corresponding to 97% absorption is

more important in the selection of preferred RAM than other criteria.

Table 6.6 RCI average values by Saaty

n 1 2 3 4 5 6 7 8 9

RCI 0 0 0.58 0.90 1.12 1.24 1.32 1.41 1.45

6.3 Objective Weights by ENTROPY method

The Shannon entropy method was discovered by Claude Elwood Shannon in

1947, for measuring the information uncertainty in the information theory. It has been

largely used in many fields for example management, finance, engineering etc. It is a

suitable method to determine the objective weights of various criteria used in multi

criteria decision making techniques [291 and 307]. The objective weights are

determined by considering the statistical data of decision-making problem and it

doesn’t depend upon DM’s judgement in ranking the criteria. The entropy calculated in

this method ascertain the degree of disorder in each criteria and smaller the entropy

value, smaller the degree of disorder. Shannon entropy method supports the various

MCDM methods like TOPSIS, VIKOR, PROMETHEE-II and grey rational analysis

etc. by evaluating the variation in each criteria to get accurate results [295 and 308].

The procedure followed in the entropy weight method is discussed

168
Step 1: - Decision matrix construction

This matrix consists of criteria and alternatives in the decision-making process.

Here the alternatives are represented as Ai (i=1, 2, 3…n) and criteria with Cj(j=1, 2,

3…m). The decision matrix denoted by X and order nxm is given by

𝑥11 𝑥12 … 𝑥1𝑚

𝑥21 𝑥22 … 𝑥2𝑚
X= 𝑥31 𝑥32 … 𝑥3𝑚
… … … …
[𝑥𝑛1 𝑥𝑛2 … 𝑥𝑛𝑚 ]

In the above matrix, the crisp value representing the performance of Ai (each

alternative) with respect to Cj (each criteria) is expressed by xij. The decision matrix for

the present work is shown in Table 6.7.

Table 6.7 Decision matrix

S. No. RAMs 15dB 10dB Maximum Thickness

bandwidth bandwidth RL (dB) (mm)
(GHz) (GHz)
1 MRAS 8 2 4 -29 3
2 MRAS 6 1.8 3.6 -31 3
3 MRAS 3 1.8 3.2 -34 3
4 NRAS 5 1.2 2.2 -34 4
5 NMRAS 10 2.6 4 -22 3

Step 2: - Formation of normalized decision matrix (P)

In this entropy method vector normalization method is used and the

normalization of decision matrix was done by using the following equation

𝒙𝒊𝒋
Pij = i=1,2,3….n 6.3
√∑𝒏
𝒑=𝟏 𝒙𝒑𝒋
𝟐

The normalized decision matrix in the present work is given by

169
 0.46274 0.51626 0.42675 0.41602
0.41647 0.46460 0.457169 0.41602
P= 0.41647 0.41298 0.50141 0.41602
0.27764 0.28392 0.50141 0.5547
[0.60156 0.51622 0.32444 0.41602]

Step 3:-Entropy measure calculation

The following equation is used to calculate the entropy measure

𝒆𝒋 = −𝒌 ∑𝒏𝒊=𝟏 𝒑𝒊𝒋 𝐥𝐧(𝒑𝒊𝒋 ) 6.4

1
Where k is a constant and expressed as ln(𝑛) and ensures that 0 ≤ 𝑒𝑗 ≤ 1

Table 6.8 Entropy measure of performance characteristics of RAMs

Performance characteristics of RAMs

15 dB 10 dB Maximum Thickness
bandwidth bandwidth RL
Entropy
measure 1.085902 1.094491 1.105091 1.109911

Step 4: - computation of degree of divergence

The degree of divergence is the inherent contrast intensity of each criterion and

calculated by following equation

𝒅𝒋 = 𝟏 − 𝒆𝒋 6.5

Step 5:- Calculation of each criteria objective weights

The following formula is used to calculate each criteria objective weights which

represents the importance of each criteria

𝒅𝒋
𝒘𝒋 = ∑𝒎 6.6
𝒋 𝒅𝒋

Table 6.9 Degree of divergence and objective weights by Entropy method

Degree of Objective
S. No. Performance criteria
divergence weights

170
 d 
j  
j

1 15 dB bandwidth 0.08590 0.21725

2 10 dB bandwidth 0.09449 0.23897
3 Maximum RL 0.10509 0.265787
4 Thickness 0.10991 0.27797

In the weights evaluation process by Shannon entropy method since no

subjective factors are involved, the result can be more accurate. The larger the value of

entropy, smaller the entropy weight which indicates that the corresponding criteria in

the decision-making process provides less information compared to other criteria. The

objective criteria weights in research work [138] are 0.20134, 0.39475, 0.22708,

0.21041, 0.2059 &0.23949, revealing that from the performance data available, the core

hardness is an important attribute in the selection of optimum material in the

engineering design against the other attributes surface hardness, surface fatigue limit,

bending fatigue limit, ultimate tensile strength and cost. The optimum weave pattern

selection in fibre reinforced composites, the exterior visible damage area is having

highest (0.319) weightage compared to other nine criteria [295].In the current research,

the calculated objective criteria weights are 0.21725, 0.23897, 0.26578 & 0.27797,

implying that from the objective perspective, minimum thickness has more weightage

than the remaining criteria.

6.4 Evaluation of compromised weights

In order to select one RAM from the available alternatives, the compromised

weighting method is used to calculate the criteria weights implemented in the TOPSIS,

VIKOR and PROMETHEE-II methods. The advantage of this method is inclusion of

both subjective and objective weights to obtain a single, quantified set of criteria

171
weights. The weights obtained from AHP and Shannon entropy method are used to

calculate the compromised or combinative weights of the criteria [294 and 340].

By using the following equation, synthesis weight (wj) for jth criteria is obtained

𝜶𝒋 𝒙𝜷𝒋
𝒘𝒋 = ∑𝒏 6.7
𝒋=𝟏 𝜶𝒋 𝒙𝜷𝒋

Where 𝛼𝑗 and 𝛽𝑗 are the subjective and objective weights obtained from AHP

and Shannon Entropy method. The calculated synthesis weights for the present work is

shown in Table 6.10.

Table 6.10 Subjective, objective and synthesis weights of criteria

Material Subjective Objective Synthesis

weights weights weights Priority
selection
S.
No.
criteria ( j )  
j w 
j
order

15 dB
1 0.54304 0.217257 0.504593 1
bandwidth
10 dB
2 0.244505 0.238979 0.249911 2
bandwidth
Maximum
3 0.135989 0.265787 0.154587 3
RL
4 Thickness 0.076465 0.277977 0.090909 4
6.5 Determination of Ranks of RAMs
The selection of one RAM from the five alternatives having different

performances were done by utilizing three popular MCDM methods namely TOPSIS,

VIKOR and PROMETHEE-II. In order to enhance the accuracy of results the

compromised criteria weights were calculated in the previous section is used to obtain

the preferential ranks of the five alternative RAMs. The block diagram of the

methodology followed in the determination of ranks of RAMs was shown in

Figure 6.1

172
6.5.1 TOPSIS method

Hwang and Yoon designed the TOPSIS method in 1981 for solving multi

criteria decision making problems. It has been commonly employed in many fields, e.g

material selection, process selection, prioritization and alternative selection etc. This

method was developed based on the fact that the best alternative will be at the least

distance from positive ideal solution (PIS) and greatest distance from negative ideal

solution (NIS) [292 and 297]. The best alternative is selected by calculating the relative

closeness coefficients and its value for least priority alternative has the minimum value

(closer to 0) and highest priority alternative has the maximum value (closer to 1).

It has been become useful ad realistic tool for choosing and rating of alternatives

by measuring the Euclidian distances. This method has many advantages like 1) no

need of pair wise comparisons 2) provides ranking of alternatives in numerical form for

easy understanding of preferences of alternatives 3) systematic approach and simple

computation. The TOPSIS method is used to solve various evaluation/selection

problems with finite no. of alternatives in the integer form and decreasing or increasing

monotonically [295 and 308]. The step by step procedure followed in TOPSIS method

is discussed as below:

173
 Figure 6.1: Methodology used in the determination of ranks

Step 1:- Decision matrix formulation

In a decision making process if ‘n’ number of alternatives (A) and ‘m’ no.of

criteria(C) are involved, the decision matrix is formulated as shown in Table 6.11

Table 6.11 Form of generalized decision matrix

Criteria (C)
C1 C2 C . . Cm
3

A1 x11 x12 x13 . . x1m

A2 x21 x22 x23 . . x2m
Alternatives (A)

A3 x31 x32 x33 . . x3m

. . . . . . .
. . . . . . .
An xn1 xn 2 xn 3 . . xnm

174
 Here Ai= the ith alternative (i=1,2, 3,……n)

Cj= the jthcriterion (j=1,2, 3,….m)

xi j = alternatives performance in a particular criterion

Step 2:- Normalized decision matrix establishment

It is formulated using vector normalization method and calculated by the

following formula

𝒙𝒊𝒋
𝒓𝒊𝒋 (𝒙) = 6.8
√∑𝒏
𝒊=𝟏 𝒙𝒊𝒋
𝟐

And the normalized decision matrix is obtained as

0.46274 0.51626 0.42675 0.41602

0.41647 0.46460 0.457169 0.41602
𝑅 = 0.41647 0.41298 0.50141 0.41602
0.27764 0.28392 0.50141 0.5547
[0.60156 0.51622 0.32444 0.41602]

Step 3: - Weighted normalized decision matrix construction

The results of TOPSIS method are largely dependent on the criteria weights

which are evaluated in this work using compromised weights composed of subjective

and objective weights. The weighted normalized decision matrix is obtained by using

the following eqn

𝒗𝒊𝒋 (𝒙) = 𝒘𝒋 [𝒓𝒊𝒋 (𝒙)] 6.9

0.23349 0.12901 0.06611 0.03782

0.21014 0.11610 0.07067 0.03782
V= 0.21014 0.10320 0.12530 0.03782
0.14009 0.07095 0.07751 0.05042
[0.30354 0.12901 0.05015 0.03782]

Step 4:- Determination of PIS (positive ideal solution) and NIS(negative ideal solution)

175
 The positive and negative ideal solutions represented as 𝑉 + and 𝑉 − were

determined by using the following formulas

𝑽+ = {𝒗(𝒙)+ + + +
𝟏 , 𝒗(𝒙)𝟐 , 𝒗(𝒙)𝟑 … . 𝒗(𝒙)𝒎 } 6.10

= {(𝑚𝑎𝑥𝑗 𝑣(𝑥)𝑖𝑗 |𝑗 ∈ Ω𝑏 ), (𝑚𝑖𝑛𝑗 𝑣(𝑥)𝑖𝑗 |𝑗 ∈ Ω𝑛𝑏 )}

𝑗 = 1,2, … . 𝑚

𝑽− = {𝒗(𝒙)− − − −
𝟏 , 𝒗(𝒙)𝟐 , 𝒗(𝒙)𝟑 … . 𝒗(𝒙)𝒎 } 6.11

= {(𝑚𝑖𝑛𝑗 𝑣(𝑥)𝑖𝑗 |𝑗 ∈ Ω𝑏 ), (𝑚𝑎𝑥𝑗 𝑣(𝑥)𝑖𝑗 |𝑗 ∈ Ω𝑛𝑏 )}

𝑗 = 1,2, … . 𝑚

Where Ω𝑏 and Ω𝑛𝑏 are the beneficial and non-beneficial criteria respectively.

The values of PIS and NIS obtained for the present work were as shown below

𝑉 + = {30354, 0.12901, 0.12530, 0.03782}

𝑉 − = {0.14009,0.07095, 0.05015,0.05042}

Step 5:- Evaluation of each alternative separation measure by using Euclidian distance

measure

The value of separation measure of each alternative from PIS and NIS is

calculated using Euclidian distance in n-dimensional method and expressed as:

𝑫𝒊+ = √∑𝒎 + 𝟐
𝒋=𝟏[𝒗𝒊𝒋 (𝒙) − 𝒗𝒋 (𝒙) ] 6.12

𝑫𝒊− = √∑𝒎 − 𝟐
𝒋=𝟏[𝒗𝒊𝒋 (𝒙) − 𝒗𝒋 (𝒙) ] 6.13

176
Step 6:- Estimation of closeness coefficient

The closeness coefficient which decides the rank of the alternative having

maximum value for the most preferable alternative and least value for the least

preferable alternative is calculated as follows:

𝑫−
𝑪+
𝒊 = +
+
6.14
𝑫𝒊 +𝑫−+

Where i = 1, 2, 3,……n

Step 7:- Ranking of the alternatives and selection of the best alternative

The preferential rankings were given to the alternatives by giving rank 1 to the

alternative having the highest closeness coefficient and rank 5 to the alternative having

least closeness coefficient. The four coal mines, A, B, C and D, are ranked as 2, 1, 4

and 3 in ref [141] against nine evaluation indexes for coal mines safety evaluation. Coal

mine B is ranked 1 due to its highest closeness coefficient of 0.8932 compared to other

coal mines. In preparing automotive brakes using natural composites, four materials,

nylon 6, HDPE, LDPE and PP, are ranked as 4, 2, 3 and 1 in the research work [309]

depending on their closeness coefficients using the TOPSIS method. In the present

work, the NMRAS 10 radar absorbing structure is ranked 1 with the highest closeness

coefficient of 0.689, and MRAS 8 is ranked 2. The least preferred alternative is NRAS

5, with 0.131 as the closeness coefficient. The details of separation measures, closeness

coefficient values and ranks of the alternatives are shown in Table 6.12.

177
 Table 6.12 Details of separation measures, closeness coefficient and ranks from TOPSIS

Separation measures Closeness

RAMs coefficient Rank
Di  Di 
 
Ci 
MRAS 8 0.091711 0.111836 0.549436 2
MRAS 6 0.108972 0.086751 0.443233 4
MRAS 3 0.096898 0.108416 0.528051 3
NRAS 5 0.180358 0.027357 0.131705 5
NMRAS 10 0.075153 0.17391 0.698256 1

6.5.2 VIKOR method

In 1998, Opricovic developed the VIKOR method, to solve the multi criteria

optimization of complex systems. In Serbian its name is Vlse Kriterijumska

Optimizacija Kompromisno Resenje meaning multi criteria optimization and

compromise solution [134 and 143]. VIKOR focusses on the compromised ranking of

alternatives having possibly conflicting and non-commensurable attributes or decision

criteria. This method assumes that to resolve conflicts, compromising is acceptable

similar to TOPSIS. The obtained compromised solution from this method is a possible

solution which is closest to the ideal solution and it establishes an agreement by mutual

concessions [3 and 140]. The ranking index provided by this method is a measure of

proximity to the ideal solution.

Step 1:- The multi criteria decision matrix formation and its normalization

The formation of decision matrix is same as the decision matrix in TOPSIS

method and is shown in Table 6.7. The vector normalization method is used for the

normalization of entities in the decision matrix using the following equation

𝑭 = [𝒇𝒊𝒋 ]
𝒏𝒙𝒎
6.15

𝒙𝒊𝒋
𝒇𝒊𝒋 = 6.16
√∑𝒏
𝒊=𝟏 𝒙𝒊𝒋
𝟐

178
 𝑖 = 1,2 … … 𝑛; 𝑗 = 1,2, … . 𝑚; and 𝑥𝑖𝑗 is the performance of alternative𝐴𝑖 with

respect to jth criteria.

The normalized decision matrix is obtained as follows

0.46274 0.51626 0.42675 0.41602

0.41647 0.46460 0.457169 0.41602
𝐹 = 0.41647 0.41298 0.50141 0.41602
0.27764 0.28392 0.50141 0.5547
[0.60156 0.51622 0.32444 0.41602]

Step 2:- The positive and negative ideal solutions identification

𝐴+ = {(max 𝑓𝑖𝑗 |𝑗 ∈ J) 𝑜𝑟 (min 𝑓𝑖𝑗 |𝑗 ∈ 𝐽, )}

i=1,2,…..n

= {𝑓1+ , 𝑓2+ , … 𝑓𝑗+ . . … 𝑓𝑚+ }

𝐴− = {(min 𝑓𝑖𝑗 |𝑗 ∈ J) 𝑜𝑟 (max 𝑓𝑖𝑗 |𝑗 ∈ 𝐽, )}

i=1,2,…..n

= {𝑓1− , 𝑓2− , … 𝑓𝑗− . . … 𝑓𝑚− }

Where J and J’ are beneficial and non-beneficial criteria respectively

The positive ideal solutions and negative ideal solutions for the present work is

A+= {0.602, 0.516, 0.501, 0.416}; A-={0.278, 0.284, 0.324, 0.555}

Step 3:- The utility measure and regret measure calculation

The TOPSIS and VIKOR methods are resulting in compromised solution and

depend on distance measure from ideal solutions. Apart from TOPSIS, in VIKOR

method, the solution obtained is with maximum group utility and minimum individual

regret of opponent. This is ensured by, utility measure and regret measure represented

by Si and Ri and for each alternative they are calculated using the following equations:

(𝒇+
𝒋 −𝒇𝒊𝒋 )
𝑺𝒊 = ∑𝒎
𝒋=𝟏 𝒘𝒋 [ ] 6.17
(𝒇+ −
𝒋 −𝒇𝒋 )

(𝒇+
𝒋 −𝒇𝒊𝒋 )
𝑹𝒊 = 𝒎𝒂𝒙𝒋 [𝒘𝒋 [
(𝒇+ − ]] 6.18
𝒋 −𝒇𝒋 )

179
 The corresponding values are tabulated in Table 6.13.
Table 6.13 Utility measure and regret measure of alternatives in the VIKOR method
S. No. RAMs Utility measure 𝑺𝒊 Regret measure𝑹𝒊
1 MRAS 8 0.091 0.088
2 MRAS 6 0.165 0.191
3 MRAS 3 0.177 0.191
4 NRAS 5 0.5 0.5
NMRAS 10 0 0
Step 4:- The VIKOR index computation and Order of preference ranking

The equation utilized to determine the VIKOR index is as follows:

𝑺𝒊 −𝑺∗ 𝑹𝒊 −𝑹∗
𝑸𝒊 = 𝛎 [ − ∗ ] + (𝟏 − 𝛎) [ − ] 6.19
𝑺 −𝑺 𝑹 −𝑹∗

Where the ith alternative VIKOR value is represented by Qi

𝑆 ∗ = 𝑚𝑖𝑛𝑖 (𝑆𝑖 ); 𝑆 − = 𝑚𝑎𝑥𝑖 (𝑆𝑖 )

𝑅 ∗ = 𝑚𝑖𝑛𝑖 (𝑅𝑖 ); 𝑅 − = 𝑚𝑎𝑥𝑖 (𝑅𝑖 )

And ν is the maximum group utility and its value is taken as 0.5 [294 and 312]
and 1- ν represents the individual regret weight.

Table 6.14 Details of VIKOR indices and ranks from VIKOR

RAMs MRAS 8 MRAS 6 MRAS 3 NRAS 5 NMRAS 10

VIKOR Index 0.179 0.356 0.368 1 0
Ranks 2 3 4 5 1

The best alternative from the VIKOR method is given by the minimum value of

VIKOR index. The selection of core shell material based electromagnetic wave

absorbers in 2-18 GHz is made using the VIKOR method, and Fe/CO material is chosen

depending upon the smallest VIKOR index of 0.05 [3]. To pick the best material for

working under hard milling conditions, from nine alternative materials, the VIKOR

index is utilized, and an alloy material is chosen, which is having minimum index value

of 0.00 [294]. From Table 6.14, in the present work, the RAM represented by NMRAS

10 has the least value of 0.00, and NRAS 5 has the highest value of the VIKOR index

180
as 1. They are the best and least preferred RAM for the given criteria.They are the best

and least preferred RAM for the given set of criteria.

6.5.3 PROMETHEE-II method

PROMETHEE-II is a tool used to solve decision making problems with

conflicting multicriteria on the basis of alternatives performance deviation with respect

to decision criteria. It was invented by J.P. Brans and P.Vincke in 1982 and considered

as a simple and easy to use outranking method. Unlike TOPSIS and VIKOR methods

it doesn’t depend on the distance from ideal solution. This method needs the

information regarding the criteria weights and preferences of alternatives given by the

decision maker. In this method pair wise comparisons of alternatives are obtained as

the difference between their performance evaluations [134 and 158]. They are

translated into preference functions representing the preference degree of each

alternative with respect to another alternative and it varies from 0 to 1. The aggregated

weighted average of preference function and net flow of each alternatives are

determined to find the ranks of the alternatives [133 and 143]. The procedure followed

in this method is explained as below:

Step 1:-Formation of evaluation matrix and its normalization

The data related to the performance of each alternative for each criteria is placed

in the evaluation matrix and the max-min normalization is used to normalize the

performance scores of the alternatives using the following equations:

(𝒙𝒊𝒋 −𝐦𝐢𝐧(𝒙𝒊𝒋 ))
𝑹𝒊𝒋 =
(𝐦𝐚𝐱(𝒙𝒊𝒋 )−𝐦𝐢𝐧(𝒙𝒊𝒋 ))
6.20

𝑖 = 1,2, … 𝑛; 𝑗 = 1,2, … . 𝑚 (For beneficial criteria)

(𝒎𝒂𝒙(𝒙𝒊𝒋 )−𝒙𝒊𝒋 )
𝑹𝒊𝒋 = (𝐦𝐚𝐱(𝒙 6.21
𝒊𝒋 )−𝐦𝐢𝐧(𝒙𝒊𝒋 ))

181
 (For non-beneficial criteria)

The resulted normalized evaluation matrix is as follows:

0.57142 1 0.58333 1
0.42857 0.77777 0.75 1
0.42857 0.55555 1 1
0 0 1 0
[ 1 1 0 1]
Step 2:- Calculation of performance differences

The performance differences of each alternative with respect to other

alternatives are determined using the following equation

𝒅𝒋 (𝒂, 𝒃) = 𝒈𝒋 (𝒂) − 𝒈𝒋 (𝒃) 6.22

Where 𝑑𝑗 (𝑎, 𝑏) represents the difference between alternative performances and

𝑔𝑗 (𝑎), 𝑔𝑗 (𝑏) are the alternative performances of alternatives a and b in jth criteria. The

calculated performance differences are shown in Table 6.15

Table 6.15 Performance difference of RAMs

S. 15 dB
10 dB Maximum Thicknes
No Evaluative Difference bandwidt
bandwidth RL s
. h
1 MRAS 8 MRAS 6 0.142857 0.222222 -0.16667 0
2 MRAS 8 MRAS 3 0.142857 0.444444 -0.41667 0
3 MRAS 8 NRAS 5 0.571429 1 -0.41667 1
4 MRAS 8 NMRAS 10 -0.42857 0 0.583333 0
5 MRAS 6 MRAS 8 -0.14286 -0.22222 0.166667 0
6 MRAS 6 MRAS 3 0 0.222222 -0.25 0
7 MRAS 6 NRAS 5 0.428571 0.777778 -0.25 1
8 MRAS 6 NMRAS 10 -0.57143 -0.22222 0.75 0
9 MRAS 3 MRAS 8 -0.14286 -0.44444 0.416667 0
10 MRAS 3 MRAS 6 0 -0.22222 0.25 0
11 MRAS 3 NRAS 5 0.428571 0.555556 0 1
12 MRAS 3 NMRAS 10 -0.57143 -0.44444 1 0
13 NRAS 5 MRAS 8 -0.57143 -1 0.416667 -1
14 NRAS 5 MRAS 6 -0.42857 -0.77778 0.25 -1
15 NRAS 5 MRAS 3 -0.42857 -0.55556 0 -1
16 NRAS 5 NMRAS 10 -1 -1 1 -1
17 NMRAS 10 MRAS 8 0.428571 0 -0.58333 0
18 NMRAS 10 MRAS 6 0.571429 0.222222 -0.75 0
19 NMRAS 10 MRAS 3 0.571429 0.444444 -1 0
20 NMRAS 10 NRAS 5 1 1 -1 1

182
Step 3:- Calculate the performance function
The DM may allot small preference or zero preference if the difference is

negligible and larger preference if the difference is large. The preference functions may

vary in-between 0 to 1.The performance functions are determined using the following

relations and shown in Table 6.16.

𝑝𝑗 (𝑎, 𝑏) = 0 if 𝑑𝑗 (𝑎, 𝑏) ≤ 0 and they are represented in Table 6.15

𝑝𝑗 (𝑎, 𝑏) = 𝑑𝑗 (𝑎, 𝑏) if 𝑑𝑗 (𝑎, 𝑏) >0

Step 4:- Determination of the aggregated preference function

For each pair of alternatives the aggregated preference function is calculated by

using the following equation

𝝅(𝒂, 𝒃) = ∑𝒎
𝒋=𝟏 𝒘𝒋 𝒑𝒋 (𝒂, 𝒃) 6.23

Where 𝜋(𝑎, 𝑏)is the overall preference of alternative “a” over alternative “b”
and 𝑤𝑗 represents the weights associated with jth criteria.

Step 5:- Calculation of the leaving and entering outranking flows

The leaving and entering outranking flows∅+ (𝑎) and ∅− (𝑎)of each alternative
are calculated by using the following relations and shown in Table 6.17.

𝟏
∅+ (𝒂) = ∑𝒏𝒊=𝟏 𝝅(𝒂, 𝒃) (a≠b) 6.24
𝒏−𝟏

𝟏
∅− (𝒂) =
𝒏−𝟏
∑𝒏𝒊=𝟏 𝝅(𝒃, 𝒂) (a≠b) 6.25

183
 Table 6.16 Preference functions of alternatives
S. 15dB 10dB Maximum RL Thickness
Preference function
No. bandwidth bandwidth
1 MRAS 8 MRAS 6 0.142857 0.222222 0 0
2 MRAS 8 MRAS 3 0.142857 0.444444 0 0
3 MRAS 8 NRAS 5 0.571429 1 0 1
4 MRAS 8 NMRAS 10 0 0 0.583333 0
5 MRAS 6 MRAS 8 0 0 0.166667 0
6 MRAS 6 MRAS 3 0 0.222222 0 0
7 MRAS 6 NRAS 5 0.428571 0.777778 0 1
8 MRAS 6 NMRAS 10 0 0 0.75 0
9 MRAS 3 MRAS 8 0 0 0.416667 0
10 MRAS 3 MRAS 6 0 0 0.25 0
11 MRAS 3 NRAS 5 0.428571 0.555556 0 1
12 MRAS 3 NMRAS 10 0 0 1 0
13 NRAS 5 MRAS 8 0 0 0.416667 0
14 NRAS 5 MRAS 6 0 0 0.25 0
15 NRAS 5 MRAS 3 0 0 0 0
16 NRAS 5 NMRAS 10 0 0 1 0
17 NMRAS 10 MRAS 8 0.428571 0 0 0
18 NMRAS 10 MRAS 6 0.571429 0.222222 0 0
19 NMRAS 10 MRAS 3 0.571429 0.444444 0 0
20 NMRAS 10 NRAS 5 1 1 0 1

Table 6.17 Net out ranking of RAMs from PROMETHEE-II

S No RAMs Leaving Entering Net flow
Flow Flow  a Rank
 a

 a


1 MRAS 8 0.257528 0.09271 0.164817 2

2 MRAS 6 0.174695 0.137197 0.037498 3
3 MRAS 3 0.175912 0.159525 0.016387 4
4 NRAS 5 0.064411 0.605528 -0.54112 5
5 NMRAS 10 0.451238 0.128823 0.322415 1
The ranks of alternatives are determined from net outranking flow, i.e., the

higher the value of out ranking flow of an alternative, it will be the most preferred

alternative. The selection of natural composites for water absorption parameters is

successfully made using PROMETHEE- II, and the composite having the higher net

flow (0.1445) is given rank 1 in the literature [158]. The tungsten carbide is chosen as

tool holder material since it is having highest net flow, 0.4779 in the research work

[294]. Therefore in the current work, NMRAS 10 is selected as the best alternative from

the PROMETHEE-II method as it has the highest value of 0.322415.

184
 Table 6.18 Scores & ranks provided by TOPSIS, VIKOR and PROMETHEE-II

TOPSIS VIKOR PROMETHEE-II

Net
S. No. RAMs Closeness VIKOR
Rank Rank outranking Rank
coefficient index
flow
1 MRAS 8 0.549 2 0.179 2 0.165 2
2 MRAS 6 0.443 4 0.356 3 0.037 3
3 MRAS 3 0.528 3 0.368 4 0.016 4
4 NRAS 5 0.132 5 1 5 -0.541 5
5 NMRAS 10 0.698 1 0 1 0.322 1
6.6 Similarity of Ranks and Selection of RAM

The calculated ranks of the RAMs from the three MCDM methods are shown

in the Table 6.18. As observed from the table even though the ranks of RAMs obtained

from VIKOR and PROMETHE-II same, they differ with ranks given by TOPSIS

method. The important point to mention is all the methods given rank 1 to the NMRAS

10. To check the similarity matching between the three methods Kendall’s coefficient

is calculated using the following formula [314 and 315]

𝒏 𝟐
∑𝒊=𝟏 𝒔𝒊
∑𝒏
𝒊=𝟏[𝒔𝒊 − ]
𝒏
𝒘
̃= 𝟏 𝟐 6.26
𝒌 𝒏(𝒏𝟐 −𝟏)
𝟏𝟐

Where k= Number of techniques utilized

𝑠𝑖 = sum of ranks assigned to a alternative I for all the k methods

n= number of alternatives in the rank evaluation

The value of Kendall’s coefficient which is a measure of similarity index of the

three methods incorporated in the present work is 0.95 i.e. there is a good agreement

(95%) between the ranks provided by the methods. Kendall's coefficients computed in

research works [314, 315] are greater than 0.85, confirming the selected MCDM

methods' similarity in the respective reports. It was summarized from the

implementation of three MCDM methods in the present work, NMRAS 10 composed

185
 of MWCNT and NZF double layered structure with 3 mm thickness is the best RAM

having strong absorption and low thickness in the X-band.

6.7 Comparison of M.A properties of NMRAS 10 with literature

The reflection loss values of NMRAS 10 are compared with R.L values of the

hybrid radar absorbing materials in the literature as shown in Table 6.19

Table 6.19 Comparison of R.L values of NMRAS 10 with literature results

Bandwidth Maximum
S. Filler Thicknes
Ref. Materials (GHz) R.L(dB)
No. wt % s (mm)
@dB @ GHz
1 [94] Epoxy/Mwcnt/NiFe 0.5 +15 4 1.6 @12 -19 @ 8.2
Paraffin/MWCNT/
2 [341] 5 4 4.6 @10 -23.1@ 8.0
Ni nanowire
3 [342] PU/Barium Titanate 30 1.1 1.6 @10 -37.2 @14
4 [84] TPU/Mwcnt/Tio2/Fe3O4 30 2 3 @10 -42.5@10.98
5 [62] Epoxy/MWCNT/NZF 60 3 1.24 @10 -19.3@8.46
6 [244] Epoxy/CoZnFe/TiO2 30 % 2 4.2 @10 -24.3@12.02
7 [217] Paraffin/RGO/Fe2O4 20 % 4 3.9 @10 -23.09@9.16
8 [93] Epoxy/CF/Fe NP 30 % 4.2 4.5 @10 -16.2@ 6.1
Present work
9 Epoxy/MWCNT/NZF 2 %+20 % 3 4 @10 -22@ 9.6
(NMRAS 10)

6.8 Mechanical Properties of MWCNT/NZF RAMs

The FRP composites have promising multifunctional applications including the

radar absorbing materials. These RAMs not only absorb the electromagnetic radiation

but they also act as load bearing structures [279 and 290]. The load bearing capabilities

of RAM are determined by conducting various mechanical testings including tensile

test, flexural test, shear test, compression test etc. [9 and 93]. The mechanical properties

of selected RAM from the MCDM methods i.e. NMRAS10 which is a double layered

structure composed of MWCNT and NZF were determined according to ASTM

standards. The samples prepared for mechanical properties are shown in Figure 6.2 (a)

to Figure 6.2 (c) It ensures the suitability of it as a RAS along with the microwave

absorbing properties.

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 aa

Figure 6.2: a) Tensile and b) Flexural and c) impact test samples

6.8.1 Tensile and flexural strength

The tensile and flexural properties are associated with the reaction of the

material when it is subjected to tension and bending respectively. In the present work

they were tested according to ASTM D3039 and ASTM D790 [91 and 95], on

HEICO/HLC 693.95 universal testing machine using three samples for each test and

error is expressed in standard deviation as shown in Figure 6.3. (a) and (b). For

conducting the tests on computer aided UTM, the data related to the testing such as

gauge length, range of the extension, machine speed etc. details have to be entered

before clamping the sample into the grips.

The stress strain diagram of NMRAS 10 sample in tensile loading is shown in

Figure 6.3 (a) the strain in percentage and stress in MPa are the X and Y-axis

coordinates. From the curve, it is clear that the MWCNT/NZF/E-glass/epoxy composite

has brittle behaviour with ultimate tensile strength `of 216 N/mm2 corresponding to a

strain of 47%. The E-glass/ Epoxy radar absorbing structures having a thickness of

2.34 mm with 3wt% of MWCNTs displayed tensile strength of 383 MPa [91]. The

shear mix process with 3 roll milling and vacuum bag degassing in an autoclave in the

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fabrication process and the presence of MWCNTs imparted this tensile strength value

to the mentioned RASs. Wei-LI et al. [123] reported tensile strength of 40 MPa, which

is attributed to the synergistic effects of the multiphase interfaces in RGO/silica

textile/PF microwave absorbers. The research work [95] reported 222 MPa tensile

strength for E-glass/ Epoxy RAS with MWCNTs with a thickness of 2.22 mm. A tensile

strength of 77.78 MPa was achieved for radar absorbing materials composed of carbon

fibre, epoxy composites with Fe nanoparticles in the study by Ashifshah et al.[93]. The

obtained values of tensile strength, young’s modulus and deformation at peak load are

shown in Table 6.20.

19 %

18 %

Figure 6.3: a) Tensile and b) flexural stress strain diagram of E-glass/epoxy/ MWCNT/NZF

composites

The flexural properties of a radar absorbing structure are important as they have

to support the loads without any flexing/bending. They were determined using three

point bending test as shown in Figure 6.4. The stress- strain diagram of NMRAS 10 in

flexural loading is shown in Figure 6.3 (b). The flexural strength is property of material

given by the maximum stress developed in a material before it reaches the yield point

in a bending test. As observed from Table 6.19, the flexural strength and modulus are

higher than the corresponding tensile properties. This is due to the nature of tests

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involved in tensile and flexural testing. In bending, the upper and lower fibre are
b
subjected to compression and tension respectively. Where as in tension all the fibres
)
are subjected to tension only. Further in flexural testing the compression in upper fibres

helps to close the cracks instead of opening them [9 and 202]. The obtained results are

validated with previous research works results obtained from ASTM D790 [18 and 96].

I.Choi et. al.[18] detailed the strength in flexural loading of aramid/E-Glass/ epoxy

composites with a thickness of 4 mm as 69.8 MPa. The sandwich RAS composed of

PMI foam/E-Glass/CNT/epoxy composites displayed 90 MPa with 18 mm thickness

[96]. In the present work, the flexural strength of hybrid RAM is 318 MPa, which is a

higher value than the above literature results and shows the proposed RAM’s better

bearing capability of bending loads. These bending loads are most commonly subjected

loads in any practical applications of RAMs.

Figure 6.4: Flexural testing of E-glass/epoxy/MWCNT/NZF composites

Table 6.20 Details of tensile and flexural properties

Property Tensile Deflection Tensile Flexural Deflection Flexural

Strength at peak Modulus Strength at peak Modulus
(N/mm2) tensile of (N/mm2) bending of
load (mm) elasticity load (mm) elasticity
(N/mm2) (N/mm2)
Value 216 12 573 318 4.25 12291

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6.8.2 Impact strength and hardness
The impact, by description is a large force employed for short time resulting in

a rapid transfer of energy and momentum. When the same force applied gradually, the

effect will be different for materials. Many of the engineering structures are subjected

to impact loads and results in the development of cracks and their propagation causing

the catastrophic failure [25 and 128]. Therefore the determination of the impact strength

of radar absorbing structures is as important as of tensile and flexural strength. It is

defined as the amount of energy the material absorb before it fractures. In impact testing

methods izod and charpy tests are the two varies of pendulum type techniques.

Generally izod impact test is used for testing of the plastics and charpy method is used

for metals. The impact strength of the NMRAS 10 is obtained from izod impact test

using ASTM D256 standard. The sample is loaded as cantilever beam and V-notch is

placed facing the pendulum. The energy absorbed by the RAM is calculated from the

swing height of pendulum after hitting the sample. S.Jogi et al. [350] mentioned that E-

Glass/Kevlar fiber reinforced epoxy composites having high stiffness aerospace

applications exhibited an impact strength of 140 J/m. The fibre reinforced polyester

composite’s impact behavior is determined using the Izod method [349], and the value

of strength in impact is 104 J/m. In the current research, the obtained value of impact

strength of NMRAS 10 is 101 J/m indicating sufficient resistance against the low

velocity impact in service conditions of the radar absorbing material.

The hardness is defined as an ability of a material to resist scratching,

penetration and indentation or collectively to the plastic deformation. The greater value

of hardness indicates its greater resistance to deformation [136, 202 and 289]. It is

frequently specified to provide the information regarding the critical performance.

Hardness testing is vital in material testing, quality control and acceptance of the

190
components in industrial and R &D applications. The relation between the size of the

impression left by the test is related to the hardness in hardness testing equipment like

Rockwell, Brinnel, knop/Vickers, shore durometer and Barcol hardness testing

equipment. The Barcol harness tester is used to determine the hardness of reinforced or

non-reinforced polymer composites. The 6 mm thick E-glass fiber reinforced polymer

composites hardness expressed in Barcol units is 43.28 [335]. The sisal fiber reinforced

epoxy composites with 30 wt% of fiber demonstrated 43.00 barcol unit of hardness

[348]. In the present research, the indentation resistance value of the proposed NMRAS

10 radar absorbing material is obtained from the Barcol hardness tester according

to ASTM D2583 standards and specified as 50. This value is higher than the above

cited literature results. It ensured the structural integrity of NMRAS 10, required for its

application as a radar absorbing structure.

6.9 Summary

This chapter summarises

1. The application of MCDM methods to five alternative RAMs considering the

performance criteria of @15 dB bandwidth, 10 dB bandwidth, maximum reflection

loss and thickness.

2. The selection of NMRAS 10 from the alternative RAMs using TOPSIS, VIKOR

and PROMETHEE-II methods. Calculation of similarity index using Kendall’s

coefficient to check the agreement between the ranks obtained from three methods.

3. Comparison of microwave absorbing properties of NMRAS 10 with results of some

of the reference papers in the literature. Investigation of structural properties of

selected NMRAS 10 including tensile strength, flexural strength, impact strength

191
and hardness. Confirmation of NMRAS 10 as a radar absorbing material with good

microwave absorption as well as mechanical properties

192
Chapter 7 SIMULATION STUDIES OF
MWCNT/NZF RASs USING COMSOL

7.1 Introduction

The numerical simulation studies of EM components are useful in the design,

analysis and optimization stages of development of new and innovative RAMs or

RASs. Out of the various EM simulation soft wares available, COMSOL is used in this

work. It is a multi-physics software platform through which real world designs and

processes are modelled in virtual environment. In the electromagnetic suit of COMSOL

software, RF module with frequency response is used to simulate the electromagnetic

properties of designed RAMs as well as RASs [5-6, 16, 23, 148, 150, 159, 174 and

198].

The main objectives in the design of microwave absorbing material are zero

reflection at the air – absorber interface, strong absorption, broad bandwidth, low

weight and thickness. But it is difficult to achieve simultaneously all the requirements

of RAM. To enhance the performance of microwave absorber and to attain the above

said goals two techniques are used. They are material based and geometry based

techniques. In material based methods, the reflection loss of absorbers are increased by

tailoring material’s permittivity and permeability resulting in high dielectric and

magnetic losses such as utilizing MWCNT, Carbon black, graphene, ferrites,

polyaniline etc. In geometry method, absorbers are constructed in such a way that its

dimensions and geometry enhances the EMW absorption within the structure like

pyramidal, Salisburry, Jaumann and Dallenbach, honey comb and multilayer absorbers

[4, 8 and 343].

193
 In this chapter a new geometry based technique is implemented using the

concept of dielectric resonator in COMSOL simulation software. The dielectric

resonators are consisting of arrays of circular cylinders with dielectric materials [148].

They are used in communication devices as antennas. Here geometry of dielectric

resonator and EM properties of MWCNT/NZF nanocomposite is used to enhance the

microwave absorption properties in the X-band. The MWCNT/NZF RAS are designed

using three types of arrays of geometric elements including cylindrical, conical and

torus and their reflection loss values were evaluated.

7.2 Procedure for Modelling and Analysis

The various steps to be followed in the modelling and analysis using FEM based

COMSOL simulation software are classified as pre-processing, solution and post

processing. The flow chart of the procedure is shown in Figure 7.1. The first and most

significant step of the FEA is pre-processing and also called model preparation. It

involves the modelling of geometry, discretization of the domain into number of

elements. These elements form the building block on which boundary conditions and

external effects are specified. The data input to solver and run the solution programme

for the required output is the next step to the pre-processing. The post processing deals

with conversion process of the output data of computer programme to a visual form.

7.2.1 Pre-processing

The preparation of input data required for finite element analysis is known as

pre-processing. It consists of creating the geometric models, assigning material

properties, mesh generation and specifying the initial and boundary conditions. The

pre-processing of MWCNT/NZF RASs started with selecting 3D model in model

wizard. The radio frequency-electromagnetic waves-frequency domain is the

194
specification of the type of the study conducted. Before the modelling of the RASs with

required geometries, the following assumptions were made in the modelling and

analysis

Figure 7.1: Flow chart of modeling and analysis of RASs using COMSOL

1. Model is homogeneous and has no air bubbles at the interfaces

2. Input EM properties are constant throughout the X-band

3. Sample is free from deformation or shrinkage during the simulation

4. RAS is isolated from the outside environment

5. Temperature is constant throughout the simulation

6. No heat generation while the EM wave propagates through the structure

7.2.1.1 Creating geometric arrays and assigning material properties

195
 The geometric arrays of cylinders, cones and torus were created using the

primitive commands- block, cylinder, cones, torus and transformation command arrays

etc. with specified dimensions. The details of the geometric modelling of cylindrical

RAS were shown in Figure 7.2 and 7.3. Initially a block of 22.8X22.8X1 mm is built

to incorporate the arrays of geometric structures on it. Total 16 geometric entities were

created. By varying the radius from 2 to 2.4 mm in steps of 0.2 mm and height of the

cylinder from 3 to 5 mm in steps of 1 mm, total five cylinder arrayed RASs were

modelled. Similar variation in case of cones considered and resulted in another five

cone arrayed RASs. For torus structures the major radius was taken from 1.5 to 2 mm

and minor radius was 0.5 to 1 mm and both varied in steps of 0.25 mm and obtained

five torus arrayed RASs.

The main aim of the work is to enhance the radar absorption properties by the

combination of dielectric MWCNT and magnetic NZF, the material selected for

cylindrical, conical and torus arrays are composed of NMRAS 10 radar absorbing

material. The bottom plate with 1 mm thickness is the copper plate which is a good

electrical conductor [95, 146, 150, 317 and 344]. The permittivity, permeability and

conductivity values are specified in the material section of model builder wizard

Figure 7.2: Geometric modelling of cylinder arrayed RAS

196
 a b

Figure 7.3: Geometric modelling: a)cone arrayed RAS and b)torus arrayed RAS

7.2.1.2 Mesh generation and boundary conditions

In finite element method, the generation of mesh splits the whole domain into

number of discrete elements. The solution of each element is interpolated to determine

the response of whole system. The tetrahedral elements are used to discretise the

designed MWCNT/NZF radar absorbing material as shown in Figure 7.4. The number

of elements for cylindrical and conical RASs with 2.2 mm radius and 3 mm height are

16,287 and 17,170. For torus structure with major and minor radius 2 mm and 0.5 mm,

the number of elements are 1, 85,811. The maximum element size for all the designs

are 2.28 mm and minimum element size is 0.41 mm. In the EM simulation of RASs in

the frequency domain, two ports are to be specified to propagate the electromagnetic

wave [1, 95 and 146]. The type of ports selected are rectangular wave ports with wave

excitation on and off at the first and second ports respectively.

Figure 7.4: Generated mesh in COMSOL

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7.2.2 Solution and Post processing
The designed RASs with different geometric arrays were solved to obtain the

reflection loss of these microwave absorbing materials. The start and stop frequency

was selected from 8.2 GHz and 12.4 GHz in the study wizard which are the X-band

frequency limits. The response of each RAS was taken for 51 intermediate points. The

computation time is varied for each different geometry with different dimensions. The

entire modelling and analysis is carried out using Intel core i5 processor with 8 GB

RAM. For cylindrical and conical structures (2.2 mm radius and 3 mm height) the

solver time is 6 min 10 s whereas torus structures has taken 1 hr 23 min due to its curved

geometry. The variation of S11 parameter, in other words the reflection loss in dB were

obtained with respect to frequency and exported to excel to compare the performance

of all the structures.

7.3 Validation of simulation and mesh convergence

The major task in the any simulation study is its validation. It can be done by

comparing the result either with analytical or experimental result. In the present work,

the simulation of geometric arrayed structures were validated by performing the

simulation of dielectric cylindrical resonator arrays mentioned in the published work

by Zoubi et al. [148]. In that work, cylindrical arrays with 2.2 mm radius and 5 mm

height was modelled and analysed in the HFSS software. The literature RAS exhibited

12 GHz bandwidth for -10 dB RL and two RL peaks at 8.4 GHz and 17 GHz. The

present COMSOL simulation resulted in 11 GHz bandwidth for -10 dB and two RL

peaks at the same frequency values. The comparison of the results from literature and

present analysis is shown in Figure 7.5. The error obtained in the -10 dB bandwidth

was found to be less than 10%. Therefore the simulation procedure used in the present

work is validated. The next important consideration is the mesh convergence which has

198
to be executed to ensure that the selected number of elements or mesh refinement is

sufficient such that the obtained solution using finite element analysis is accurate to

desired level.

Figure 7.5: Validation of simulation studies

The method of mesh convergence requires plotting the curve of critical result

parameter against the mesh density or number of elements. At the minimum three

convergence runs will be required to draw a curve which can then be used to indicate

when convergence is achieved. If two runs of different densities give the same results,

mesh convergence must already be achieved. While performing mesh convergence, the

solver time also has to be considered. In present work the mesh convergence is

performed to achieve the result in the published Zoubi et al. [148] with five types of

meshes like coarser, coarse, normal, fine and finer, resulting in different number of

elements in the proposed RAS in the ref. The variations obtained in the -10 dB

bandwidth of proposed structure in literature with different meshes/ number of elements

are shown in Figure 7.6. The normal mesh with 17,131 elements and solver time of 6

min 48 s is considered to be the suitable mesh for the present work compared to other

199
mesh refinements as it produced the literature result within the desired accuracy and

computing time.

Figure 7.6: Mesh convergence

7.4 Microwave absorption of MWCNT/NZF nanocomposites with

geometric arrays

The microwave absorption properties of arrayed RASs can be modulated by

changing the geometry parameters like radius and height of the each element. The effect

of these parameters on the bandwidth and absorption strength is determined by

conducting the parametric simulation studies of designed RASs.

7.4.1 Cylinder arrayed RASs

The effect of height and radius of cylinders on the reflection loss values in the

X-band frequency is shown in Figure 7.7. These RASs are designed based on geometry

technique using arrayed structures. In this method, the incident electromagnetic wave

200
couples with arrayed elements at multiple resonance frequencies where electromagnetic

fields are partially restricted and absorbed inside the arrayed structure [344].

Figure 7.7: RL of cylinder arrayed RASs

The increase in the height from 3 to 5 mm with 2.2 mm radius and increase in

radius from 2 to 2.4 mm with 3 mm height shifted the RL peak towards the lower

frequencies due to resonance modes of absorbing material. Similar effect was observed

in research work by Zoubi et al. [148]. Out of the five cylindrical RASs, radius 2 mm

and height 3 mm structure exhibited better performance of -25 dB at 12 GHz and -20

dB, 1 GHz bandwidth. This RAS showed -10 dB RL in the entire X-band frequency

range. Another RAS with radius 2.2 mm and radius 3 mm also exhibited -10 dB RL for

4.2 GHz bandwidth.

7.4.2 Cone arrayed RASs

The variation in the reflection loss of cones arrayed RASs with respect to X-

band frequency is shown in Figure 7.8. The deviation in the radius of the cone from 2

to 2.4 mm with 3 mm height and change in the height from 3 to 5 mm with 2.2 mm

radius of the cone shifted the RL peak towards the lower frequency range [148]. The
201
cone arrayed RAS with 2 mm radius and 3 mm height shown an RL of -42 dB at 8.8

GHz frequency which is highest in the cone arrayed RASs.

Figure 7.8: RL of cone arrayed RASs

Cones with 3 mm height and 2, 2.2 mm radius RAS shown -20 dB RL in the

entire X-band region and also all the cone arrayed RASs exhibited an RL of -13 dB for

4.2 bandwidth corresponding to 95% absorption of electromagnetic wave radiation.

7.4.3 Torus arrayed RASs

The torus arrayed RASs reflection losses were shown in Figure 7.9. The major

radius change from 1.5 mm to 1.75 mm with constant minor radius of 0.5 mm increased

the maximum RL peak from -68 dB to -74 dB and further increase to 2 mm reduces to

-62 dB. Similar variation is observed for the minor radius change from 0.5 mm to 1 mm

with constant major radius of 0.5 mm. It is worthwhile mentioning that all the RASs

with torus arrays exhibited -25 dB RL throughout the X-band. Especially, the structure

with minor radius 0.5 mm and major radius 1.75 mm has shown an RL of -75 dB at 9.2

202
GHz frequency and -30 dB RL corresponding to 99.9% of absorption in the entire X-

band region.

Figure 7.9: RL of torus arrayed RASs

7.5 Summary

1. The implementation of geometry based technique using arrayed structures of

dielectric resonators using COMSOL radio frequency domain.

2. The modelling of three geometric elements arrayed RASs with cylinders, cones

and toruses.

3. Validation and mesh convergence which are the important aspects in the FEA

based simulation analysis.

4. Evaluation of microwave absorption properties of designed RASs with

parametric studies to determine the dimensions of the geometric elements for

optimum performance of RASs.

203
Chapter 8 CONCLUSIONS AND FUTURE SCOPE

8.1 Introduction
The objective of the present work is to determine microwave absorption in terms

of reflection loss of multi-layered RAS composed of MWCNT/NZF in the X-band. The

magnetic nano NZF is prepared using the sol-gel auto combustion method. Three

different kinds of RAMs are fabricated using MWCNT, NZF and a combination of

MWCNT and NZF. The raw materials and RAMs samples are characterized by using

SEM, XRD, EDX, VSM, TGA and VNA. The multi-layered analysis using

transmission line theory resulted in thirty six double layered RAMs. The preferred

double layered RAM is selected using TOPSIS, VIKOR and PROMETHEE-II by

implementing both subjective and objective criteria weights. The tensile strength,

flexural strength, impact strength and hardness values are determined according to the

ASTM standards. The implementation of the proposed hybrid RAM as a band stop filter

is simulated using arrayed structures in COMSOL software. The outcomes and future

scope of the present work are discussed in the subsequent sections.

8.2 Conclusions
The following conclusions and outcomes are drawn from the present work

 The hybrid RAMs fabricated with low aspect ratio MWCNT exhibited

decreased bandwidths and increased thickness compared to hybrid RAMs with

high aspect ratio MWCNT. The bandwidth of -16 dB reflection loss decreased

(by 54% i.e.) from 2.2 GHz to 1 GHz and thickness increased (by 62.5% i.e.)

from 3 mm to 8 mm for low aspect ratio hybrid RAM compared to high aspect

ratio hybrid RAM.

204
 The MRAS 8, consisting of double layered E-glass/epoxy/MWCNT

composites with 3 mm thickness, exhibited 90% absorption for 4 GHz with 2

wt% of MWCNT in the X-band. The MRAS 6 and MRAS 5 shown an RL of -

32 dB and -35 dB at 10.6 GHz and 11.0 GHz corresponding to 99% microwave

absorption. Therefore, these dielectric fibre reinforced RAMs provide good

microwave absorption properties in less weight and thickness than sandwich

structures whose thickness is nearly 10 mm

 The nanocrystalline nickel zinc ferrite is synthesized using urea as a fuel agent

through facile sol-gel auto combustion method. The morphological,

microstructural and magnetic characterization by FESEM, EDX, XRD, TEM,

FTIR and VSM revealed its spherical shape, fine particle size of 26 nm, narrow

particle size distribution, purity, crystallinity and ferromagnetic nature.

 The effect of weight percentages of nickel zinc ferrite, i.e., 10, 20 and 25 % in

E-glass/epoxy/NZF composites on electromagnetic properties is studied. In all

three samples, magnetic losses dominate compared to dielectric losses and the

magnetic losses were increased by 47 % with an increase in weight percentages

of NZF from 10 -25 wt% at 8.2 GHz frequency.

 The double layered E-glass/epoxy/NZF nanocomposite NRAS 5 exhibited an

RL of -10 dB for a bandwidth of 2.4 GHz with a thickness of 4 mm and 25 wt%

of NZF. The contribution of this part of the present work is the proposal of

relatively thin and lightweight radar absorbing materials with magnetic fillers,

which are developed from low cost raw materials and processing methods.

 The NMRAS 10 radar absorbing material with 2 wt% and 20wt% of MWCNT

and NZF exhibited -10 dB for 3.6 GHz bandwidth and -16 dB for 2.2 GHz

205
 bandwidth. This performance is due to the high aspect ratio of MWCNT,

magnetic and dielectric losses provided by MWCNT and NZF and double

layered design of NMRAS 10.

 The thermal stability of E-glass/epoxy/MWCNT/NZF and E-glass/epoxy/NZF

nanocomposites determined by TGA revealed that magnetic RAMs have

temperature resistance up to 300 0C and hybrid RAMs are thermally stable up

to 360 0C. The initial decomposition temperature of neat epoxy composites

enhanced by 10% by the addition of NZF. The MWCNT aspect ratio enhanced

the IPDT of neat epoxy composite by 12% and these polymeric structures could

be used in aircrafts and high speed vehicles where high thermal resistance is

required.

 The tensile strength, flexural strength, impact strength and Barcol hardness

values of NMRAS 10 were investigated as 216 N/mm2, 318 N/mm2, 101 J/m

and 50. These values established the load bearing capabilities of NMRAS 10

along with its good microwave absorption properties.

 The combinative weights were used in the selection of RAM by the MCDM

methods. The rank one attained by NMRAS 10 confirms the synergetic effect

of the combination of dielectric MWCNT and magnetic NZF in radar absorbing

materials. The evaluated Kendall’s coefficient is 0.95 and it indicated the good

agreement of ranks given by the three MCDM methods to five alternative

RAMs.

 The RASs were modelled and analyzed using COMSOL software using three

types of geometric arrayed structures. In cylindrical arrayed radar absorbing

structures, the RAS with 2 mm radius and 3 mm height exhibited -10 dB RL in

206
 the entire X-band, -20 dB for 1 GHz bandwidth and a maximum RL of -25 dB

at 12 GHz frequency. The cone arrayed RAS, with 2 mm radius and 3 mm

height cones, resulted in -20 dB RL in the entire X- band and a maximum RL

of -42 dB at a frequency of 8.8 GHz. The torus arrayed RAS with 0.5 mm minor

radius and 1.75 mm major radius exhibited -30 dB in the entire X-band region

corresponding to 99.99 % absorption of microwaves. Hence these types of RAS

can be used as band stop filters in the X-band frequency range.

8.3 Recommendations for future studies

 In the present work, the effect of the aspect ratio of MWCNT on microwave

absorption properties is studied. Further this can be extended to study the

influence of size and shape of the dielectric materials such as carbon black,

graphene, carbon nanofibers on the microwave absorption properties.

 The microwave absorption properties of RAMs were studied in this work by

considering the normal incidence of the E.M wave. The effect of angle of

incidence varying from 00 to 1800 on microwave absorption properties can be

studied for different types of RAMs

 The effect of the annealing temperature of ferrites on EMW absorption

properties can be studied. The annealing temperature is maintained constant

in the present work during the synthesis of ferrites by the sol-gel auto

combustion method.The EM properties of Co, Zn, etc. elements doped nickel

ferrites in different compositions can be studied.

 The effect of weight percentages and thickness of dielectric and hybrid RAMs

having less than 1mm and effect of thickness of magnetic RAM on

microwave absorbing properties can be studied.

207
 The double layered E-Glass/epoxy/MWCNT/NZF composites RL values are

determined in the present work. This can be extended to multilayer analysis

of hybrid RAMs consisting of MWCNT with CO, Ni, Fe, alloys or ferrites.

 The incorporation of techniques like electroless plating, sputtering, surface

modification of nanofillers and variation of the composites curing pressure

during fabrication can be studied to enhance the microwave absorbing

properties of RAMs.

 In the numerical simulation studies of RAMs and RASs, modeling various

geometric lossy fillers like spheres, tubes can be studied to investigate their

effect on microwave absorption and mechanical properties.

208
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