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Advances in
Magnetic Materials
Processing, Properties,
and Performance
Advances in Materials Science and Engineering
Series Editor
Sam Zhang
Advances in Magnetic Materials: Processing, Properties, and Performance,

edited by Sam Zhang and Dongliang Zhao
Aerospace Materials Handbook, edited by Sam Zhang and Dongliang Zhao
Biological and Biomedical Coatings Handbook: Applications, edited by Sam Zhang
Biological and Biomedical Coatings Handbook: Processing and Characterization,
edited by Sam Zhang
Hierarchical Micro/Nanostructured Materials: Fabrication, Properties, and
Applications, Weiping Cai, Guotao Duan, Yue Li
Hydroxyapatite Coatings for Biomedical Applications, edited by Sam Zhang
Nanobiomaterials: Development and Applications, edited by Dong Kee Yi and
Georgia C. Papaefthymiou
Nanostructured and Advanced Materials for Fuel Cells, edited by San Ping Jiang
and Pei Kang Shen
Micro- and Macromechanical Properties of Materials, Yichun Zhou, Li Yang,
and Yongli Huang
Semiconductor Nanocrystals and Metal Nanoparticles: Physical Properties and
Device Applications, edited by Tupei Chen and Yang Liu
Thin Films and Coatings: Toughening and Toughness Characterization,
edited by Sam Zhang
Advances in
Magnetic Materials
Processing, Properties,
and Performance
Edited by
Sam Zhang • Dongliang Zhao
Boca Raton London New York
CRC Press is an imprint of the

Taylor & Francis Group, an informa business
CRC Press
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Contents
Editors ......................................................................................................................vii
Contributors ..............................................................................................................ix
Chapter 1 Magnetic Behavior of Nanostructured Materials .................................1

M. R. Hossain, Animesh Kumar Basak, Alokesh Pramanik, and
Al Mahmudur Rahman
Chapter 2 Elemental Ferromagnetic Nanomaterials: Their Preparation,

Properties, and Applications .............................................................. 67
Suneel Kumar Srivastava and Samarpita Senapati
Chapter 3 Magnetic Materials for Nuclear Magnetic Resonance and

Magnetic Resonance Imaging .......................................................... 131
Elizaveta Motovilova and Shaoying Huang
Chapter 4 Plasma Nanotechnology for Nanophase Magnetic Material

Synthesis........................................................................................... 189
Rajdeep Singh Rawat and Ying Wang
Chapter 5 Compositional Optimization and New Processes for

Nanocrystalline NdFeB-Based Permanent Magnets........................ 293
Zhongwu Liu and Lizhong Zhao
Chapter 6 Layered Two-Phase Magnetoelectric Materials ............................... 373

Zhaofu Du, Sam Zhang, Dongliang Zhao, Tat Joo Teo, and
Rajdeep Singh Rawat
Chapter 7 Rapidly Solidified Rare-Earth Permanent Magnets:

Processing, Properties, and Applications ......................................... 453
Shampa Aich, D. K. Satapathy, and J. E. Shield
Chapter 8 Magnetic Materials Prepared Using Polyacrylamide Gel Route .....509

S. F. Wang, X. T. Zu, and Richard YongQing Fu
v
vi Contents
Chapter 9 Perpendicular Magnetic Anisotropy in Magnetic Thin Films ......... 581

Prabhanjan D. Kulkarni, Somnath Bhattacharyya, and
Prasanta Chowdhury
Chapter 10 Catalytic Application of Magnetic Nanocomposites ....................... 627

Yinghuai Zhu
Chapter 11 Magnetic Domain Walls for Memory and Logic Applications........ 665
Chandrasekhar Murapaka, Indra Purnama, and Wen Siang Lew
Index ...................................................................................................................... 721

Editors
Professor Sam Zhang Shanyong, better known
as Sam Zhang, earned his PhD in ceramics in
1991 from the University of Wisconsin-Madison,
Wisconsin, USA, and is a tenured full professor
(since 2006) at the School of Mechanical and
Aerospace Engineering, Nanyang Technological
University. Professor Zhang was the founding edi-
tor-in-chief for Nanoscience and Nanotechnology
Letters (2008–2015) and principal editor of the
Journal of Materials Research (USA) respon-
sible for the thin films and coating field (since
2003). Professor Zhang has been involved in the
processing and characterization of nanocompos-
ite thin films and coatings for more than 25 years
and has authored/coauthored more than 300 peer-reviewed international journal
papers, 12 books, and 23 book chapters, and guest edited 13 journal volumes special
issues. From the Scopus webpage as of June 29, 2016, Professor Zhang’s total articles
in publication are 298; the sum of the times cited, 6586; h-index, 45.
Professor Dongliang Zhao has been the vice

president at the Central Iron and Steel Research
Institute (CISRI, Beijing, China) since 2012.
CISRI plays a leading role in China’s R&D in
superalloys. Professor Zhao’s research interests
include computational material sciences, mag-
netic materials, energy materials, and superalloys.
He has been the leading principal investigator of
or participated in more than 20 Chinese national
research projects. Professor Zhao has published
50 journal papers and was granted 6 patents. In
2003, Professor Zhao received the title of “Beijing
Outstanding Young Engineer” by the Beijing
City Government. In 2006, he was recognized by
the State Department as one of the National Star
Researchers and in 2008, he was awarded the title of “National Defense Science and
Technology Innovation Leader.”
vii
Contributors
Shampa Aich Shaoying Huang
Department of Metallurgical and Singapore University of Technology and
Materials Engineering Design
Indian Institute of Technology Singapore
Kharagpur
Kharagpur, India Prabhanjan D. Kulkarni
National Aerospace Laboratories
Animesh Kumar Basak Council of Scientific and Industrial
Adelaide Microscopy Research
The University of Adelaide Bengaluru, India
Adelaide, South Australia, Australia
Wen Siang Lew
Somnath Bhattacharyya School of Physical and Mathematical
Indian Institute of Technology Madras Sciences
Chennai, India Nanyang Technological University
Singapore
Prasanta Chowdhury
Zhongwu Liu
National Aerospace Laboratories
School of Materials Science and
Council of Scientific and Industrial
Engineering
Research
South China University of
Bengaluru, India
Technology
Guangzhou, China
Zhaofu Du
Research Institute of Functional Materials Elizaveta Motovilova
Central Iron and Steel Research Institute Singapore University of Technology and
Beijing, China Design
Singapore
Richard YongQing Fu
Faculty of Engineering and Chandrasekhar Murapaka
Environment School of Physical and Mathematical
University of Northumbria Sciences
Newcastle upon Tyne, United Kingdom Nanyang Technological University
Singapore
M. R. Hossain
Department of Materials and Alokesh Pramanik
Metallurgical Engineering Department of Mechanical
Bangladesh University of Engineering Engineering
and Technology Curtin University
Dhaka, Bangladesh Perth, Australia
ix
x Contributors
Indra Purnama S. F. Wang

School of Physical and Mathematical School of Physical Electronics
Sciences University of Electronic Science and
Nanyang Technological University Technology of China
Singapore Chengdu, China
and
Al Mahmudur Rahman Science and Technology on
Institute of Engineering Mechanics Vacuum Technology and Physics
Karlsruhe Institute of Technology Laboratory
(KIT) Lanzhou Institute of Physics
Karlsruhe, Germany Lanzhou, China
Rajdeep Singh Rawat Ying Wang

NSSE, National Institute of Education NSSE, National Institute of Education
Nanyang Technological University Nanyang Technological University
Singapore Singapore
D. K. Satapathy Sam Zhang

Department of Metallurgical and School of Mechanical and Aerospace
Materials Engineering Engineering
Indian Institute of Technology Nanyang Technological University
Kharagpur Singapore
Kharagpur, India
Samarpita Senapati Dongliang Zhao

Department of Chemistry Research Institute of Functional
Indian Institute of Technology Kharagpur Materials
Kharagpur, India Central Iron and Steel Research Institute
Beijing, China
J. E. Shield
Department of Mechanical and Lizhong Zhao
Materials Engineering School of Materials Science and
College of Engineering Engineering
University of Nebraska South China University of Technology
Lincoln, Nebraska Guangzhou, China
Suneel Kumar Srivastava Yinghuai Zhu

Department of Chemistry Institute of Chemical and Engineering
Indian Institute of Technology Kharagpur Sciences
Kharagpur, India Singapore
Tat Joo Teo X. T. Zu

Mechatronics Group School of Physical Electronics
Singapore Institute of Manufacturing University of Electronic Science and
Technology Technology of China
Singapore Chengdu, China
1 Magnetic Behavior of
Nanostructured Materials
M. R. Hossain, Animesh Kumar Basak,
Alokesh Pramanik, and Al Mahmudur Rahman
CONTENTS
Abstract ......................................................................................................................2
1.1 Introduction ......................................................................................................2
1.2 Common Terminology in the World of Magnetism .........................................3
1.2.1 Magnetic Moment .................................................................................3
1.2.1.1 Magnetic Moment in Atom ....................................................5
1.2.1.2 Magnetic Moments in Clusters .............................................. 7
1.2.2 Magnetic Order .....................................................................................8
1.2.2.1 Magnetic Moment in Rare Earth Elements ......................... 11
1.2.2.2 Magnetic Moment in Transition Metal Compounds ............ 11
1.2.2.3 Magnetic Moment in Ferromagnetic Materials ................... 11
1.2.3 Magnetic Anisotropy .......................................................................... 12
1.2.3.1 Crystalline Anisotropy......................................................... 12
1.2.3.2 Shape Anisotropy................................................................. 13
1.2.3.3 Other Anisotropy ................................................................. 15
1.2.4 Coercivity ........................................................................................... 15
1.3 Concept of Nanostructured Magnetic Materials ............................................ 17
1.3.1 Brief History of Nanostructured Magnetic Materials ........................ 18
1.3.2 Common Nanostructured Magnetic Materials ................................... 18
1.3.2.1 Oxides and Carbides Nanoparticles ..................................... 19
1.3.2.2 Metallic Nanoparticles .........................................................20
1.3.2.3 Core-Shell Nanoparticles ..................................................... 22
1.3.3 Different Types of Magnetism ............................................................ 22
1.3.3.1 Ferromagnetism ................................................................... 23
1.3.3.2 Paramagnetism.....................................................................24
1.3.3.3 Diamagnetism ......................................................................25
1.4 Origin of Magnetism ......................................................................................26
1.4.1 Quantum-Mechanical Origin of Magnetism ...................................... 27
1.5 Magnetism in Nanostructured Materials ........................................................ 29
1.5.1 Magnetization Process ........................................................................ 37
1.5.1.1 Domain Walls ...................................................................... 39
1.5.1.2 Coherent Rotation ................................................................ 42
1.5.2 Role of Particle Size on Magnetism ................................................... 43
1
2 Advances in Magnetic Materials
1.6 Fabrication of Magnetic Nanostructured Materials .......................................44

1.6.1 Different Fabrication Processes ..........................................................44
1.6.1.1 Bottom-Up Approach ...........................................................44
1.6.1.2 Top-Down Approach............................................................ 45
1.6.2 Stability of Magnetic Nanostructured Materials ................................ 48
1.7 Characterization of Magnetic Nanostructured Materials ............................... 49
1.8 Application of Magnetic Nanostructured Materials ....................................... 53
1.9 Concluding Remarks ...................................................................................... 56
References ................................................................................................................ 56
ABSTRACT
Over the past couple of decades, nanocrystalline materials, commonly noted as
nanomaterials, are receiving wide attention among scientists due to unusual material
properties at the nanoscale that are not foreseen in the micro-/macroscale. This field
of nanomaterials is still very young, requires a long quest, and upholds prospects
beyond imagination. With this in view, this chapter compiles the advancements of
magnetic behaviors of such nanomaterials. Starting from the origin of magnetism in
nanomaterials, we have systematically addressed their functionality, fabrication, and
characteristics. This chapter ends with concluding remarks and the future prospects
of magnetic nanomaterials.
1.1 INTRODUCTION
The unique properties of materials at the nanometer scale have been the subject of
enormous research interest among researchers over the past decades. Incremental
shifts in “product-performance” using these materials, for example, as fillers in plas-
tics [1], as coatings on surfaces [2], and as ultraviolet protectants in cosmetics [3],
have already been achieved. Nanostructured materials hold even more promise for
the future as they could infuse almost any industry including chemistry, medicine/
medical, plastics, energy, electronics, aerospace, etc. As a result of recent improve-
ment in technologies to produce, characterize, and manipulate these types of materi-
als, this field has seen a huge surge in endowment as well as research. Originating
from the Greek word for dwarf, “nano” signifies one billionth (10−9) of any scale.
The word “nano” has gained great importance in science and evolved as a multidisci-
plinary research topic over the decades. The potential recognition of nanotechnology
and research on nanostructured materials resulted from the famous speech of Nobel
laureate Richard Feynman in 1959, “There’s plenty of room at the bottom…” in
which he emphasizes that there were no fundamental physical reasons why materials
could not be fabricated by maneuvring individual atoms [4]. The term nanotechnol-
ogy was first introduced in 1971 by Norio Taniguchi [5] for ultraprecision machining
and the main breakthrough occurred with the invention of the scanning tunneling
microscope (STM) by Binning and Rohrer in 1981 [6]. The scientific principles and
properties exhibited by materials at the nanometer scale are not normally seen at the
micron scale. Nonetheless, the well-known quantum effects arise in the case where
the size of the system is commensurable with the de Broglie wavelengths of the
Magnetic Behavior of Nanostructured Materials 3
electrons, phonons, and excitations propagating in them. Such fascinating and use-
ful properties manifested by nanostructured materials can be explored for a variety
of structural and nonstructural applications. Atoms and molecules are the essential
building blocks of all materials and the way they are “constructed” with these build-
ing blocks directly dictate their properties. Accordingly, nanotechnology refers to
the maneuvring of individual atoms, molecules, or molecular clusters into structures
to create materials and devices with new or vastly different properties. Conventional
materials are composed of grains varying in size anywhere from 100’s of microm-
eters (µm) up to millimeters (mm) and in contrast, nanostructured materials, grains/
crystals are in the order of 20–30 nm. However, in such cases, a grain of 1 nm size
may contain only three to five atoms, depending on the atomic radii and have a
well-defined effect of its physical properties. For example, the radius of crack-tip
growth and propagation in bulk material is likely to be different from crack prolif-
eration in a nanostructured material where crack and particle size are analogous.
Due to these reasons, the fundamental electronic, magnetic, optical, chemical, and
biological processes are also different at this level. For example, where proteins are
10–1000 nm in size, and cell walls 1–100 nm thick, their behavior on encountering
a nanomaterial may be quite different from that seen in relation to larger-scale mate-
rials. Thus, nanocapsules and nanodevices may present new possibilities for drug
delivery, gene therapy, and medical diagnostics. Fascinatingly, such nanostructured
materials are of the same order of magnitude as the range of the various interactions
that define magnetism/magnetic properties in materials and newer magnetic effects
can be created. Thus, the objective of this present chapter is to explore magnetic
nanostructured materials in terms of their origin, fabrication, characterization, and
functionality.
1.2 COMMON TERMINOLOGY IN THE WORLD OF MAGNETISM

1.2.1 Magnetic MoMent
A magnet’s magnetic moment (µm) is a vector that characterizes the magnet’s overall
magnetic properties. For a bar magnet, the direction of the magnetic moment points
from the magnet’s south pole to its north pole [7] and the magnitude represents how
strong and how far apart these poles are. In SI units, the magnetic moment is A.m2.
A magnet produces its own magnetic field and also responds to external magnetic
fields as well. The strength of the magnetic field is proportional to the magnitude of
its magnetic moment. In addition, when the magnet is put into an external magnetic
field, it is subject to a torque tending to orient the magnetic moment parallel to the
field [8]. The amount of this torque is proportional to the magnetic moment and the
external field as well. According to the positions and orientations of the magnet and
source, a magnet may also experience a force driving it in one direction or another.
The magnetic field parameters at a given point in space are defined to be the mag-
netic field strength (H), the magnetic flux density or magnetic induction (B), and the
magnetization of the material (M) [9]:
B = µ 0 (H + M ) (1.1)
where µ0 = 4π × 10−7 H/m is the permeability of free space (H = Henry, Vs/A). We

can also define the magnetic field parameters as follows:
B = µ 0H(1 + χ) = µH (1.2)
where µ = µ0(1 + χ) is the permeability of the material and χ = M/H is the magnetic
susceptibility of the material. And the magnetic moment, µm, for a given volume V:
M = µ m /V (1.3)
According to the above equations, the well-known B–H curve is shown in Figure
1.1. Based on these curves, a different class of magnetism can be explained as
described hereafter.
If the external field strength increased (in a ferromagnetic solid), then at first
magnetization rises slowly and then more rapidly. Finally, it levels off and reaches a
constant value, for example, saturation magnetization. When H is reduced to zero,
the magnetization retains a positive value, for example, remanent magnetization or
remanence. It is this retained magnetization which has been explored in permanent
magnets. The remanent magnetization can be removed by reversing the magnetic
field strength to a value Hc (coercive field). Without an external magnetic field, orbit-
ing electrons magnetic moments are randomly oriented and thus they mutually can-
cel one another. As a result, the net magnetization is zero as pointed out earlier.
However, when an external field is applied, the individual magnetic vectors tend to
turn into the field direction, which is counteracted by thermal agitation alignment.
Based on that, different magnetic behavior can be explained as follows:
• Diamagnetism occurs due to the external magnetic field that induces a

change in the magnitude of inner atomic currents. Specifically, the external
field accelerates or decelerates the orbiting electrons, so that their magnetic
moment is in the opposite direction from the external magnetic field.
• Antiferromagnetic materials exhibit a spontaneous alignment of moments
below a critical temperature. However, the responsible neighboring atoms in
(a) (b) (c)

Magnetic saturation (Ms) Magnetic saturation (Ms) Magnetic saturation (Ms)
Superparamagnetic Soft magnet Hard magnet
A
A
Magnetization (M)
Magnetization (M)
Magnetization (M)
B B
Coercivity Coercivity
(Hz) (Hz)
External magnetic field (H) External magnetic field (H) External magnetic field (H)
FIGURE 1.1 B–H curve: (a) nonmagnets, (b) soft magnets, and (c) hard magnets. (Adapted
from V. V. Mody, A. Singh, B. Wesley, Eur. J. Nanomed 5(1), (2013), 11–21.)
antiferromagnetics are aligned in an antiparallel fashion. Antiferromagnetic

materials are paramagnetic above Neel temperature (TN).
• Ferrimagnets are similar to antiferromagnets in that two sublattices exist
that couple through a super exchange mechanism to create an antiparal-
lel alignment. However the magnetic moments on the ions of the sublat-
tices are not equal and hence they do not cancel; rather a finite difference
remains to leave a net magnetization. This spontaneous magnetization is
defeated by the thermal energy above the Curie temperature.
1.2.1.1 Magnetic Moment in Atom

A moving electric charge is the source of a magnetic field and a magnetic moment
can be associated with it. At atomic scale, magnetism results from electron motion
[9]. There are two contributions to the magnetic moment from electrons:
• The orbital moment ml, due to the motion of the electron in its orbit in the
form of ml = −µBl, where l is the orbital angular momentum and µB is the
Bohr magneton. The values l = 0, 1, 2, and 3 are attached to electrons in the
s, p, d, and f shells, respectively.
• The spin moment m s = −2 µBS, where S is the spin of purely quantum ori-
gin. It can explain the spinning motion of the electron about its own axis.
The spin is characterized by the value of s, which can only take two pos-
sible values, +1/2 and −1/2.
A different set of electrons rotating about the nucleus is associated with each ele-
ment of the periodic table. In a given electron shell, there are 2l + 1 states available
for each spin state, making a total of 2(2l + 1) states (10 for a d shell, 14 for an f shell)
as shown in Figure 1.2. The distribution of the electrons over the available orbits for
a given shell aims to minimize the energy associated with their mutual electrostatic
repulsion. This energy contains the “exchange term,” which depends on the spin and
is responsible for magnetism in the matter. The electron shells fill up progressively
according to the Hund rules. The first of these rules says that the total spin S associ-
ated with all the electrons in the same electron shell is maximal by taking consider-
ation of Pauli’s exclusion principle. Thus all the electron spins tend to be parallel to
one another. The second Hund rule states that the total orbital angular momentum
L is maximum, with the restriction that the first rule takes precedence. The motion
of the nucleus creates a magnetic field acting on the spin moment. This field is the
I= –3 –2 –1 0 1 2 3
S = +½
S = –½
FIGURE 1.2 Itinerant electron system at dysprosium. (Redrawn based on D. Givord,

Nanomaterials and Nanochemistry, C. Bréchignac, P. Houdy, and M. Lahmani (eds.),
Springer-Verlag, Berlin Heidelberg, Germany, 2007, pp. 101–134.)
source of the spin–orbit coupling between the orbital and spin moments. The energy
of the spin–orbit coupling is given by
E spin −orbit = λLS (1.4)
where λ is the spin–orbit coupling constant. The orbital and spin contributions asso-
ciated with all the electrons in a full (closed) electron shell tend to balance one
another so that the resulting magnetic moment is zero.
In solid state, the mixing of orbitals that result from covalence or the formation
of energy bands often leads to the disappearance of the atomic magnetic moment.
There are only two series of elements in the periodic table that retain magnetism in
solid state due to the internal structure of an unfilled electron shell that is responsible
for preserving magnetic effects in the solid state:
1. The first series (commonly known as rare earth elements) goes from cerium
to lutetium, and corresponds to the progressive filling of the 4f shell. The
electrons, localized in their atomic orbits, are essentially subject to the same
exchange interactions as in an isolated atom and the magnetic moment as
defined by the Hund rules.
2. The second series contains iron, cobalt, and nickel, and corresponds to the
filling up of the 3d shell. In insulating systems such as oxides, the 3d elec-
trons are localized and the magnetic moment is still defined by the Hund
rules. In metals, the 3d electrons are said to be itinerant, forming an energy
band with width of the order of 5 eV. The magnetic moment is no longer
produced strictly on the atomic scale.
Stoner showed that an alternative approach can be used to describe most of the
observed magnetic behavior [9]. The whole set of electrons is considered, distributed
over two half-bands, each containing 5N states, where N is the total number of atoms
(Figure 1.2), and characterized by the value of the electron spins +1/2 (↑) and −1/2
(↓). In the absence of exchange interactions, the minimum energy corresponds to the
equal filling of the two half-bands and the system is nonmagnetic. Under the effect of
exchange interactions, one half-band will be favored because of the tendency for the
electron spins to line up. The state of the system is defined by competition between
these two terms. In Cr, Mn, Fe, Co, and Ni, the minimum energy configuration is
magnetic.
Despite the itinerant nature of the 3d electrons, they remain essentially localized
at each atomic site and at the end of the day many properties of 3d metals can be
described by treating the magnetic moments as atomic. However, the distribution of
moments considered at two different times will not be strictly the same, since the
electrons can hop from one atom to another. The nonintegral values of the magnetic
moments per atom (2.2 µB for Fe, 1.74 µB for Co, 0.60 µB for Ni) basically reflect the
fact that they correspond to an average value taken over all the atoms making up
the given system [9]. A schematic of the orbital and spin magnetic moment is shown
in Figure 1.3.
Orbital magnetic
Total moment
magnetic
moment
Spin moment
FIGURE 1.3 Schematic of orbital and spin magnetic moment. (Redrawn based on from
High-accuracy magnetic property measurement method by separating spin and orbital mag-
netic moments. 04 Mar, 2013 BL08W (High Energy Inelastic Scattering) Japan Synchrotron
Radiation Research Institute (JASRI), University of Hyogo.)
1.2.1.2 Magnetic Moments in Clusters

The first measurements of the magnetic moments of free clusters of 3d ferromag-
netic metals, such as iron and cobalt, were made on clusters consisting of 100–500
atoms (diameter 1–2 nm) [7,8]. These clusters were obtained by laser ablation and
subsequent condensation of vaporized atoms in the inert atmosphere of helium. The
magnetic moments of the clusters were calculated from the extent to which they
are deflected when passed through a region of magnetic field gradient similar to
the Stern-Gerlach experiment [9]. In order to analyze the results, it should be taken
into account that the clusters are superparamagnetic. For iron, the results suggest an
average atomic moment of 2.2 µB, equal to the value in the bulk solid. For cobalt, the
experiments lead to a value of 2.08 µB compared to 1.72 µB in the bulk. The theoreti-
cal band structure of a cluster comprising 15 iron atoms, separated into the succes-
sive contributions of the various atomic layers or shells has been calculated by Pastor
et al. [12] as shown in Figure 1.4. Qualitatively, the energy distribution of the states
in each half-band has two lobes, as in the bulk.
The lower energy lobe is associated with delocalized bonding states, while the
higher energy lobe comes from localized antibonding states. However, the band
width is less than in the clusters. Indeed, the band states are formed from linear
combinations of atomic states. The more states involved, the broader is the energy
distribution of the states. When a magnetic moment is formed, a certain number
of electrons are transferred from one half-band to another, thus the energy loss is
smaller in the case of a narrow band. The narrowing of the d band in clusters is
responsible for the 3d moment to increase. The value of the magnetic moment of
atoms in a cluster is also affected further by secondary mechanisms [9]. There is
a reduction in interatomic distances which leads to an increase in the itinerancy of
the electrons and hence to an increased mixing of orbitals and result in a reduction
of the atomic magnetic moment. On the other hand, the reduced symmetry of the
environment of the atoms causes a reduction in band width that favors an increased
magnetic moment.
Measurements of circular dichroism using x-rays synchrotron facilities make
it possible to examine the spin and orbital moments separately. Apart from the
enhancement of the spin moment, a similar enhancement of the orbital moment has
been detected for small iron clusters [8]. In thin films, Bruno [13] has shown that
the enhancement of the orbital moment and the increase in magneto-crystalline
–2
Fe15(bcc)
Spin
–1 majoritaire
No(ε) (eV–1)
1 Spin
minoritaire
–5 –4 –3 –2 –1 0 1 2 3 4
(ε –ε 0d) (eV)
FIGURE 1.4 Theoretical band structure of a cluster comprising 15 iron atoms. (Adapted
from G. M. Pastor, J. Dorantes-Davila, K. H. Bennemann, Phys. Rev. Lett. 40, 1989,
7642–7451.)
anisotropy which are related to the local reduction of symmetry. However, in

clusters, all moments are coupled in parallel by exchange. The value of the orbital
moment depends on the orientation of the moments relative to the local easy axis of
magnetization. Assuming the clusters to be spherical, the increase in orbital moment
should vanish by symmetry. Two phenomena explain the existence of strong orbital
moments revealed experimentally: First, there is an anisotropic relaxation which
breaks the spherical symmetry of the clusters and second, the cluster atoms are
arranged into successive shells. However, the cancelling effects only come fully into
effect for systems comprising filled (closed) atomic shells.
1.2.2 Magnetic order

The main interactions among electrons in matter are due to electrostatic repulsion.
In quantum mechanics the “exchange term,” results from the indistinguishability of
the electrons. As Heisenberg showed, magnetism then arises naturally as soon as the
Pauli exclusion principle is taken into account. This states that two electrons cannot
occupy the same quantum state defined by the space and spin variables, and thus
requires the wave function for the electron ensemble to be antisymmetric in those
variables. This in turn implies that the interaction energy among electrons depends
on their spin states. The electrons in different atomic sites affect one another by
exchange interactions, a magnetic coupling exists between the atomic moments of
different atoms, and this is the source of magnetic order in a material. The exact
nature of the coupling between moments depends a great deal on the elements that
are present, and also on the crystallographic arrangement of the atoms. When all
(a) (b) (c)
FIGURE 1.5 Schematic of magnetic structures: (a) ferromagnetic, (b) antiferromagnetic

and (c) ferrimagnetic structure. (Drawn based on N. Taniguchi, Precision Engineering, 16(1),
1994, 5–24; V. V. Mody, A. Singh, B. Wesley, Eur. J. Nanomed. 5(1), (2013), 11–21; High-
accuracy magnetic property measurement method by separating spin and orbital magnetic
moments. 04 Mar, 2013 BL08W (High Energy Inelastic Scattering) Japan Synchrotron
Radiation Research Institute (JASRI), University of Hyogo.)
the moments are parallel, the structure is ferromagnetic as shown in Figure 1.5a.
In this case, the moment per unit volume of matter is spontaneous magnetization
(Ms). In an antiferromagnetic arrangement (Figure 1.5b), the moments are organized
into two groups. Within the same group (sublattice), the moments are all parallel to
one another. However, the moments of the two sublattices couple in an antiparallel
manner and the resulting magnetization is zero. Thus in ferrimagnetic systems, the
numbers of atoms or the value of the magnetic moments are not the same in each
sublattice. This time, cancellation is not complete and there remains some spontane-
ous magnetization (Figure 1.5c).
The exchange energy as described earlier can be expressed as
∑J S S
1
E exch = − ij i j (1.5)
2 i , j≠ i
where Jij is the exchange integral, representing the coupling force between spins,
and Si and Sj are the spins carried by atoms i and j. The exchange interactions are
assumed to be very short range. If all the atoms are identical and considering only
nearest neighbors, Jij can be replaced by J, and Si and Sj by S. The exchange energy
per atom then becomes
1
e exch = − zJsS2 (1.6)
2
where z is the number of nearest neighbors of a given atom. When J is positive, that
is when the minimal energy configuration corresponds to parallel coupling between
all spins, it gives rise to ferromagnetism. More generally, the exchange interactions
Jij can vary for one atom I depending on its neighbor’s j and from one atom i to
another. When there are negative terms Jij , they then favor antiparallel coupling
between moments i and j which are required to explain nonferromagnetic struc-
tures. Equations 1.5 and 1.6 assumed a temperature of 0 K. At nonzero temperatures,
thermal vibrations tend to destroy magnetic order. At a certain temperature (Curie
temperature, TC, in ferromagnetic and Neel temperature, TN, in ferromagnetic and
antiferromagnetic materials) a transition occurs from the ordered magnetic state.
The effects of thermal vibrations can be described using the molecular field model.
Let us consider a ferromagnetic material. Since the spin is in fact proportional to the
magnetic moment, valid at 0 K, it can be rewritten as
1
e exch = − µ at H m,0 (1.7)
2
where µat is the atomic magnetic moment, proportional to the spin, and Hm,0 is a ficti-
tious magnetic field representing the exchange interactions and called the molecular
field, first introduced by Weiss:
H m,0 = nMs,0 (1.8)
In this expression, n is the molecular field coefficient and Ms,0 the spontaneous
magnetization at 0 K, that is magnetization at absolute saturation. A central assump-
tion in the molecular field model is that, when the temperature increases, the proper-
ties of the matter remain strictly homogeneous. The molecular field at temperature
T can be expressed as a function of spontaneous magnetization at this temperature:
H m = nMs (1.9)
It can then be shown that the spontaneous magnetization decreases steadily as the
temperature increases (Figure 1.6) and disappears at Curie temperature, TC:
zJS2 nµ at2
Tc = = (1.10)
3k 3k
Spontaneous magnetization (Ms)
Bulk materials
Nanostructured
materials
Temperature (T)
FIGURE 1.6 Schematic of temperature dependence on spontaneous magnetization for dif-

ferent materials. (Drawn based on N. Taniguchi, Precision Engineering, 16(1), 1994, 5–24;
V. V. Mody, A. Singh, B. Wesley, Eur. J. Nanomed. 5(1), (2013), 11–21; High-accuracy
magnetic property measurement method by separating spin and orbital magnetic moments.
04 Mar, 2013 BL08W (High Energy Inelastic Scattering) Japan Synchrotron Radiation
Research Institute (JASRI), University of Hyogo.)
where k is the Boltzmann constant. The value of the Curie temperature provides
a measure of the strength of the exchange interactions. As originally explained by
D. Givord [9], the molecular field model can be utilized to describe the behavior of
antiferromagnetic and ferrimagnetic materials. To go beyond this model, the disor-
der of the moments is considered to be produced at finite temperatures by collective
excitations known as spin waves. As far as magnetic moments are concerned, these
are perfectly analogous to the collective vibrations of atoms known as phonons. For
the same entropy as in the molecular field model, the loss of exchange energy is
lower. When the wavelength λ of a spin wave increases, the angle between consecu-
tive magnetic moments within the wave reduced. In a ferromagnetic material, the
energy ESW of the spin waves can be written as
E SW = D2q (1.11)
where D is the rigidity constant of the spin waves and q = 2π/λ is the wave vector.
1.2.2.1 Magnetic Moment in Rare Earth Elements

In rare earth elements, localized 4f electrons are located in the inner shell that is well
protected from the effects of the environment by the presence of the outer 5s, 5d, and
6s shells. Interactions between 4f electrons located on different atoms are therefore
negligible. In fact, an indirect form of exchange coupling does exist in these systems,
involving electrons in the outer 5d and 5s shells as intermediaries. This coupling,
known as RKKY (Ruderman-Kittel-Kasuya-Yoshida) coupling, is relatively weak
and only extends to 1–2 nm. In contrast, in other exchange coupling mechanisms,
the range of the interactions never exceeds one or two times the interatomic distance.
The magnetic order temperatures are always lower than room temperature. In 3d
transition metal systems, the exchange coupling is related to the itinerant nature of
the electrons. When they hop from atom 1 to atom 2, the electrons conserve their
spin. They then interact with electrons present on atom 2, their spin tending to lie
parallel with these, according to the first Hund rule. The resulting ferromagnetic
coupling force is explained by the intra-atomic nature of the exchange terms. In iron,
cobalt, and nickel, the Curie temperature is much higher than room temperature,
reaching 1380 K in cobalt.
1.2.2.2 Magnetic Moment in Transition Metal Compounds

In insulating transition metal compounds, the exchange mechanism involves a mix-
ture of the 3d and p wave functions of the anions, such as oxygen. The hybridization
of the wave functions depends significantly on crystallographic orientation. Hence,
the mechanism known as superexchange gives rise to the coupling of different signs
and the magnetic arrangements are very often antiferromagnetic (MnO, CoO, NiO)
or ferrimagnetic (γ–Fe2O3, Fe3O4). In some cases, several coupling mechanisms com-
pete with each other and nonaligned magnetic arrangements of moments can exist.
1.2.2.3 Magnetic Moment in Ferromagnetic Materials

The ferromagnetic nature of the bulk solid is conserved in clusters of Fe, Co, or Ni.
This result can be related to the fact that, in the 3d shells of metals, the interaction
mechanism between magnetic moments is insensitive to minor changes in the atomic

environment. In nanoparticles of transition metal oxides, measurements reveal a
reduction in the average magnetization. This happens for magnetite nanoparticles
(γ–Fe2O3), a collinear ferrimagnetic material in the bulk. For an insulating system,
such a reduction in magnetization cannot be attributed to a lower magnetic moment,
since the latter does not depend on the size of the system. In fact, Mössbauer spec-
troscopy on the Fe57 nucleus reveals noncollinear arrangements of the moments
[12]. Such arrangements are characteristic of atoms located in a low-symmetry
environment and subject to magnetic interactions of various signs and supported by
numerical simulation. Noncollinear arrangements of the same origin also occur in
nanoparticles of systems that are antiferromagnetic in the bulk state, such as NiO
[13] and carry a small magnetic moment.
1.2.3 Magnetic anisotropy

If the magnetic susceptibility of a material depends on the direction in which it is
measured, then the situation is known as magnetic anisotropy [13]. When magnetic
anisotropy exists, the total magnetization of a ferromagnet M will prefer to lie along
a special direction widely known as the “easy axis.” The energy associated with this
alignment is “anisotropy energy”:
E a = Ksin 2θ (1.12)
where θ is the angle between M and “easy axis,” and K is the anisotropy constant.
Most materials contain some type of anisotropy affecting magnetization behavior.
The most common forms are: (i) crystal anisotropy, (ii) shape anisotropy, (iii) stress
anisotropy, (iv) externally induced anisotropy, and (v) exchange anisotropy. Among
these, crystalline and shape anisotropy play the most important role on the magnetic
behavior of nanostructured materials.
1.2.3.1 Crystalline Anisotropy

In crystalline anisotropy, the ease of obtaining saturation magnetization is different
for different crystallographic directions. For example, in a single crystal of iron Ms
can most easily be obtained in the [100] direction compared to the [110] direction
and are most difficult to attain for [111] directions as shown in Figure 1.7. The [100]
direction is the easy direction (easy axis). Both iron and nickel are cubic and have
three different axes, whereas cobalt is hexagonal with a single easy axis perpen-
dicular to the hexagonal symmetry (Figure 1.7). The physical origin of crystalline
anisotropy is the coupling of the electron spins which carry the magnetic moment
to the electronic orbit and couple it to the lattice. A polycrystalline sample with no
preferred grain orientation has no net crystal anisotropy due to averaging over all
orientations.
The magnetic anisotropy can be one or two orders of magnitude stronger in mate-
rials composed of 4f elements than in those made from 3d elements as it is much
less sensitive to the background crystalline field. In addition, the spin–orbit cou-
pling force, approximately proportional to the square of the atomic number, is much
(a) (b) (c)

1600 [100] [111]
Parallel axis 500
[110] [111]
M (emu μm–3)
1200 1200 400

[110]
300 [100]
800 800
Basal plane 200
400 400
100
Fe Co Ni
0 0 0
0 200 400 600 0 2000 4000 6000 8000 0 100 200 300
H (Oe)
FIGURE 1.7 Magnetization curves for single crystals of (a) iron, (b) cobalt and (c) nickel
along different directions. (Adapted from K. J. Klabunde, Nanoscale Materials in Chemistry,
Wiley-Interscience, 2001.)
stronger in rare earth elements than in 3d transition metals. Thus both spin–orbit
coupling and the crystalline field influence the overall performance. In rare earth
materials, the spin–orbit coupling dominates the crystalline field, at maximum value
of the orbital moment, aligned with the spin moment. Obviously a strong orbital
moment indicates a highly asymmetric electron orbit. The energy of an orbit placed
in a given environment depends more on its orientation as it becomes more asym-
metric. This is basically why rare earth compounds and alloys often exhibit strong
crystalline anisotropy. A schematic representation of the hard and easy axis with the
corresponding crystallographic structure is shown in Figure 1.8.
For materials made from transition elements, the crystalline field must be consid-
ered before the spin–orbit coupling. Electron orbits adopt shapes that follow from
their surrounding symmetry and the associated orbital moment is often small, for
example, zero for cubic symmetry. The spin–orbit coupling tends to induce an orbital
moment in the direction of the spin moment, but the associated distortion of the elec-
tron orbit is not favorable for the crystalline field. The orbital moment induced by
this mechanism is thus small, for example, a few percent of the spin moment in the
metals Fe, Co, and Ni, and the magnetic anisotropy, which is roughly proportional
to it, is likewise small.
1.2.3.2 Shape Anisotropy

It is easier to induce a magnetization along a long direction of a nonspherical piece
of material than along a short direction as the demagnetizing field is less in the long
direction, because of further apart induced poles. Thus, a smaller applied field will
negate the internal demagnetizing field. For a pro-late spheroid with major axis c
greater than the other two (equal) axes of length a, the shape anisotropy constant is
1
K s = ( N a − N c )M 2 (1.13)
2
where Na and Nc are demagnetization factors. For spheres, Na = Nc as a = c. It can be

shown that 2Na + Nc = 4π; then the limit c ≫ a, that is, a long rod, Ks = 2πM². Thus
a long rod of iron with Ms = 1714 A m−1 would have a shape anisotropy constant of
14
Easy Easy
Hard –1
1
1
–1
–1 –1
m2 m2 –1
m2 0 m2
1
m2 1
1 1 m2 –1
1 1
Easy Hard
6 directions 2 directions 8 directions
FIGURE 1.8 Schematic representation of hard and easy axis with corresponding crystallographic structure. (Adapted from B. D. Cullity, Introduction
to Magnetic Materials, Addison-Wesley Publishing Company, 1972, pp. 214–250.)
Advances in Magnetic Materials
(a) (b) (c) (d)
FIGURE 1.9 Schematic of different forms of shape anisotropy. (Redrawn based on K. M.

Krishnan et al., J. Mater. Sci. 41, 2006, 793–815.)
Ks = 1.85 × 107 erg cm−3. This is significantly greater than the crystal anisotropy so
we see that shape anisotropy can be very important for nonspherical particles. A
schematic of the different forms of shape anisotropy is shown in Figure 1.9.
1.2.3.3 Other Anisotropy

Stress anisotropy results from internal or external stresses that occur due to rapid
cooling, application of external pressure, etc. Anisotropy may also be induced
by annealing in a magnetic field, plastic deformation, or by ion beam irradiation.
Exchange anisotropy occurs when a ferromagnet is in close proximity to an antifer-
romagnet or ferromagnet. Magnetic coupling at the interface of the two materials
can create a preferential direction in the ferromagnetic phase, which takes the form
of a unidirectional anisotropy. This type of anisotropy is most commonly observed
when an antiferromagnetic or ferromagnetic oxide forms around a ferromagnetic
core.
The value of the magnetic anisotropy for nanoparticles can be deduced from the
so-called blocking temperature. In cobalt nanoparticles, the anisotropy obtained is
equal to 3 × 107 J/m3, which are almost two orders of magnitude greater than in the
bulk [15]. In spherical symmetry, even if the magnetic anisotropy of a surface atom
is high, the total anisotropy should disappear due to symmetry. However, the strong
anisotropy in nanoparticles must be associated with anisotropic relaxation and the
fact that the outer atomic shell of the nanoparticles is not filled.
1.2.4 coercivity
Coercivity is the magnetic field strength necessary to demagnetize a ferromagnetic
material that is magnetized to saturation. It is measured in ampere per meter (A/m),
or traditionally in oersted (1 Oe = 79.578 A/m). Let us imagine that a new field is
applied to a sample in the saturated magnetization state, but in the opposite direction
to the initially applied external field.
The magnetization should grow in the opposite direction in order to minimize the
Zeeman energy as shown in Figure 1.10 [9] where the Y axis represents energy and
X axis represents θ, the angle between the applied field and the Z axis.
However, the initial nucleation of a new domain in the saturated state requires the
system to overcome an energy barrier and a moment taking part in this process to go
through a situation in which it lies perpendicular to the easy axis of magnetization.
As the situation is unfavorable, the anisotropy energy is maximum. Thus coercivity
K
Z
E
Barrier
Energy (J)
θ
Angle (θ)
FIGURE 1.10 Relation of coercivity with Zeeman energy. (Redrawn based on E. Kneller,
R. Hawig, IEEE Trans. Mag. 27, 1991, 3588–3592.)
of a material is its capacity to resist the effect of an applied field. When the applied
field is exactly antiparallel to the initial magnetization direction z, the coercive field
Hc is equal to the anisotropy field:
2K
Hc = = HA (1.14)
Ms
As soon as nucleation occurs, magnetic moments reverse in n as known as coher-

ent rotation according to Stoner and Wohlfarth [7]. In general coercive field is a func-
tion of the angle θ between the applied field and the z axis (with the convention that
θ = 0 corresponds to a field antiparallel with the initial direction of the moments):
H c (θ) = H SW (θ) = H A /(sin 2 /3θ + cos2 /3θ)3/ 2 (1.15)
As evident from Equations 1.14 and 1.15, magnetic anisotropy underlies the coer-
civity. However, in reality the coercive field is much weaker than that of the anisot-
ropy field due to the presence of structural defects. As anisotropy is reduced at defect
sites, nucleation is facilitated and accompanied by the formation of a wall that sepa-
rates the nucleus from the rest of the material with opposite magnetization. Complete
reversal of the magnetization takes place by the propagation of the wall through the
material. In this case, the angular variation of the coercive field is very different from
what would correspond to coherent rotation and is expressed as
H c (0 ) (1.16)
H c (θ) ≈
cos θ
where Hc(0) is the coercive field at θ = 0. Thus the projection of the applied field in
the initial magnetization direction plays an active role in the reversal process. As the
coercive field is much weaker than the anisotropy field, the reversible rotation of the
moments toward the applied field can be neglected. Some nanostructured alloys are
heterogeneous, that it, they contain both magnetically soft and hard particles [18].
Due to the exchange coupling between soft and hard particles, the reversal of
magnetization in the soft particles requires a magnetization configuration character-
ized by progressive rotation, similar to what happens in a domain wall. However, this
can only occur over the size of these particles (10–20 nm), well below the equilib-
rium thickness of a domain wall. As already explained, the energy of a confined wall
is greater than the energy of a wall with equilibrium thickness. Due to this reason
the soft phase therefore resists the formation of a confined wall and hence becomes
coercive. The experimental value of the coercive field is in qualitative agreement
with the theoretical value [17,19].
1.3 CONCEPT OF NANOSTRUCTURED MAGNETIC MATERIALS

On October 18, 2011, the European Commission adopted the following definition
of a nanomaterial [20]: “A natural, incidental or manufactured material containing
particles, in an unbound state or as an aggregate or as an agglomerate and where, for
50% or more of the particles in the number size distribution, one or more external
dimensions is in the size range 1–100 nm. In specific cases and where warranted
by concerns for the environment, health, safety or competitiveness the number size
distribution threshold of 50% may be replaced by a threshold between 1 and 50%.”
However, this differs from the definition adopted by the International Organization
for Standardization (ISO): “Material with any external dimension in the nanoscale
or having internal structure in the nanoscale.” Nanoscale is, in turn, defined as size
range from approximately 1–100 nm [21].
Nanostructured materials are not just another step toward miniaturization. This is
mostly due to the fact that, the nanometer scale sits somewhere midway between the
atomic scale and microscale, where quantum phenomena are prevalent compared to
bulk materials. A bulk material should have constant physical properties in contrast
to the nanometer scale. Size-dependent properties, such as quantum confinement in
semiconductor particles, surface plasmon resonance in some metal particles, and
superparamagnetism in magnetic materials are observed. In this level, some material
properties are governed by the laws of atomic physics and do not behave like bulk
materials. Research based on nanostructured materials takes a materials science-
based approach to nanotechnology through a “top-down” or “bottom-up” approach
to fabricate them. Nanostructured materials can be metals, ceramics, polymeric
materials, or composite materials.
Nanostructured magnetic materials are a particular class of nanostructured mate-
rials which can be manipulated by the application of magnetic field. Such particles
commonly consist of magnetic elements in it such as iron, nickel, cobalt, and their
chemical compounds. The magnetic nanoparticles have been the focus of recent
research activity as they possess attractive properties, which could be of potential
use in the field of catalysis including nanomaterial-based catalysts [22], medicine
[23], magnetic resonance imaging [24], magnetic particle imaging [25], data stor-
age [26], environmental remediation [27], nanofluids [28], optical filters [29], defect
sensors [30], and cation sensors [31] to mention a few. One of the most important
magnetic properties at nanometer scale is superparamagnetism which can lead to
particles with much higher magnetic susceptibilities than in traditional paramagnets.
1.3.1 Brief History of nanostructured Magnetic Materials

Nanostructured materials have been used by humans for hundreds of years without
knowing of their existence. For example, the beautiful ruby red color of glass, the
decorative glaze (luster) found on some medieval glass and pottery contain metal-
lic spherical nanoparticles dispersed in a complex way and exhibit characteristic
optical properties. The techniques used to produce these materials were considered
trade secrets at the time, and are not fully understood even now. The development of
nanostructured materials and nanotechnology as a whole has been pushed forward
by the development of sophisticated transmission electron microscopy (TEM) and
scanning tunneling microscopy (STM). Such techniques enable researchers to carry
out the characterization of such materials. Hollow carbon spheres, commonly known
as buckyballs or fullerenes (C60), were discovered in the mid-1980s [32]. The C60
(60 carbon atoms chemically bonded together in a ball-shaped molecule) buckyballs
inspired research that led to the fabrication of carbon nanofibers, with diameters
under 100 nm. Scientists at IBM had managed to position individual xenon atoms on
a nickel surface to spell out the company logo, using scanning tunneling microscopy
probes, as a demonstration of the extraordinary new technology [33]. In 1991, S.
Iijima of NEC in Japan reported the first observation of carbon nanotubes, which are
now produced by a number of companies in commercial quantities [34].
1.3.2 coMMon nanostructured Magnetic Materials

Magnetic nanostructured materials are extremely small particles of materials that
respond to magnetic fields and are classified into three broad categories:
1. Systems with nanometric dimensions such as nanoparticles, nanorods,

nanotubes, etc.
2. Systems with macroscopic dimensions, but made up of crystallites with
nanometric dimensions such as nanostructured/nanopatterned materials,
core/shell nanoparticles, nanorods, nanotubes, etc.
3. A combination of both categories above.
As stated earlier, nanoparticles in general exist on scales larger than the atom but
still smaller than traditional bulk materials. Thus, a combination of both classical
and quantum mechanics must be used to analyze this transitional region of scale and
difference from bulk materials by:
• Intrinsic properties of isolated clusters

• Coercively and remnant magnetization dependence on structure
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Utetheisa pulchella (Linn.). Farafra, 20/4/12.
Noctuidæ
Chloridea nubigera (Herrsch.). Camp IX, Libyan Desert, 5/4/12.
Euxoa spinifera (Hubn.). Kairowin Hattia, Farafra, 12/4/12.
Agrotis ypsilon (Rott.). Bu Gerara, 4/4/12.
Cirphis loreyi (Dup.). Bu Gerara, 3/4/12.
Athetis flava (Oberth.). Meir, Dirut, Egypt, 17/3/12.
Laphigma exixua (Hubn.). Camp IX, 4/4/12; Bu Gerara, 3-4/4/12;
Meir, Dirut, Egypt, 17/3/12.
Phytometra gamma (Linn.). Kairowin Hattia, Farafra, 12/4/12. Camp
XI, Farafra, 6/4/12; Meir, Dirut, Egypt, 17/3/12.
Leucanitis kabylaria (Bang, Haas.). Kairowin Hattia, Farafra, 10-
12/4/12.
Hypoglaucitis benenotata moses (Stdgr.). Kairowin Hattia, Farafra,
12/4/12.
Anumeta hilgerti (Rothsch.). Kairowin Hattia, Farafra, 12/4/12.
Pyralidæ
Ommatopteryx ocellea (Haw.). Camp XII, 17/4/12.
Syria Kingi (Rothsch.). (spec. nov.) Fifteen miles south of Bir
Kairowin, 14/4/12.
Syria variabillis (Rothsch.). Meir, Dirut, Egypt, 17-23/3/12; Camp II,
23/3/12.
Syria Libyca (Rothsch.). (spec. nov.) Kairowin Hattia, Farafra,
12/4/12.
Heterographis adustella (Rag.). Kairowin Hattia, Farafra, 12/4/12.
Heterographis verburii (Butl.). Camp II, 23/3/12.
Heterographis samaritanella (Zell.). Kairowin Hattia, Farafra,
12/4/12.
Heterographis conversella (Led.). Camp II, 23/3/12.
Nomophila noctuella (Schiff). Camp IX, Libyan Desert, 4/4/12; Bu
Gerara, 3-4/4/12; Camp XI, Farafra, 6/4/12; Camp XII, 7/4/12;
Camp IV, 25/3/12; Camp V, 26/3/12; Meir, Dirut, Egypt, 17/3/12.
Pyraustidæ
Cornifrons ulceratalis (Led.). Meir, Dirut, Egypt, 17/3/12; Camp II,
23/3/12.
Noctuelia floralis (Hmpsn.). Camp II, 23/3/12.
II. IDENTIFIED AT SOUTH KENSINGTON
TINEINA
Gelechiadæ
Aproærema mitrella (Wlsm.). Meir, Dirut, Egypt, 17-18/3/12; Camp II,
Libyan Desert, 23/3/12; Negeb er Rumi, Libyan Desert, 4/4/12.
Seven specimens. (Tests J. H. Durrant.)
Phthorimæa eremaula (Meyr). Dakhla Road, Libyan Desert, 26/3/12;
Bu Gerara, Libyan Desert, 2-4/4/12. Three specimens. (Tests J. H.
Durrant.)
Plutellidæ
Plutella maculipennis (Crt.). Meir, Dirut, Egypt, 16-23/3/12; Camp II,
Libyan Desert, 23/3/12; Dakhla Road, Libyan Desert, 26/3/12; Bu
Gerara, Libyan Desert, 3-4/4/12; Negeb er Rumi, Libyan Desert,
4/4/12; Farafra Depression, Libyan Desert, 6/4/12; south of Bir
Kairowin, 10/4/12. Fifty-three specimens. (Tests J. H. Durrant.)
Tineidæ
Trichophaga abruptella (Wlstn.). Meir, Dirut, Egypt, 17-18/3/12. Two
specimens. (Tests J. H. Durrant.)
DIPTERA
Mycetophilidæ
Macrocera (?) nana (Macq.). Meir, Dirut, Egypt, 20-23/3/12. Three
specimens. (Tests F. W. Edwards.)
Chironomidæ
Chironomus tripartitus (Kieff). Meir, Dirut, Egypt, 17-23/3/12. Two
specimens. (Tests F. W. Edwards.)
Syrphidæ
Syrphus corollæ (Fabr.). Bu Gerara, Libyan Desert, 2-4/4/12. Two
specimens. (Tests E. E. Austen.)
Muscidæ
Musca analis (Macq.). Meir, Dirut, Egypt, 16-20/3/12. Four
Musca angustifrons (Thoms.). Meir, Dirut, Egypt, 16-18/3/12. Two
TACHINIDÆ
Sarcophaginæ
Disjunctis nuba (Wied.). Bu Gerara, Libyan Desert, 4/4/12. One
specimen. (Tests E. E. Austen.)
Anthomyidæ
Fannia canicularis (L.). Meir, Dirut, Egypt, 16/3/12. One specimen.
(Tests E. E. Austen.)
Trypetidæ
Urellia stellata (Fuessl.). Abu Harag, Libyan Desert, 26/3/12. One
specimen. (Tests E. E. Austen.)
PLANIPENNIA
Chrysopidæ
Chrysopa vulgaris (Schneider). Meir, Dirut, Egypt, 17/3/12; Camp II,
Libyan Desert, 23/3/12; Dakhla Road, Libyan Desert, 26/3/12; Abu
Harag, Libyan Desert, 26/3/12; Bu Gerara, Libyan Desert, 2-
3/4/12; Negeb er Rumi, Libyan Desert, 4/4/12. Twenty-five
specimens. (Tests H. Campion.)
HEMIPTERA
Reduviidæ
Reduvius palliles (Klug). Meir, Dirut, Egypt, 18/3/12. One specimen.
(Tests C. J. Gahan.)
Jassidæ
Chlorita flavescens (Fabr.). Meir, Dirut, Egypt, 20/3/12. Three
specimens. (Tests F. Laing.)
COLEOPTERA
Carabidæ
Stenolophus marginatus (Dej.). Camp II, Libyan Desert, 23/3/12.
One specimen. (Tests G. J. Arrow.)
Dermestidæ
Dermestes frischi (Kug.). Bu Gerara, Libyan Desert, 2/4/12. One
specimen. (Tests G. J. Arrow.)
Scarabæidæ
Aphodius hydrochæris (F.). Meir, Dirut, Egypt, 17/3/12. One
specimen. (Tests G. J. Arrow.)
Aphodius granulifrons (Fairm.). Camp II, Libyan Desert, 23/3/12.
One specimen. (Tests G. J. Arrow.)
Aphodius sp (?). Meir, Dirut, Egypt, 20/3/12. One specimen. (Tests
G. J. Arrow.)
Tenebrionidæ
Ocnera hispida (Forsk.). Meir, Dirut, Egypt, 20/3/12. One specimen.
(Tests K. G. Blair.)
ORTHOPTERA
Gryllidæ
Gryllotalpa gryllotalpa (L.). Meir, Dirut, Egypt, 17-21/3/12. Two
specimens. (Tests B. Uvarov.)
APPENDIX III
ROCK INSCRIPTIONS FROM THE LIBYAN DESERT
T HE graffiti shown in the accompanying plates were collected in

the Libyan Desert. The majority of them occurred on the Gubary
road, between the oases of Kharga and Dakhla, or in the hattia
through which this road runs, immediately before entering the oasis
of Dakhla, in its south-east corner.
In many places these rock scribings were extraordinarily
numerous. It is no exaggeration to say that at some of the
recognised halting-places on the Gubary road, where it is the custom
for caravans to rest during the midday heat, or at the end of the
day’s journey, the rocks are so thickly covered with graffiti that it is
almost impossible to walk without treading on them.
The collection does not pretend to be in any way a complete one,
for the signs were mostly copied during a hurried journey in the hot
weather of 1909; there are consequently a considerable number that
have been overlooked.
Unfortunately most of them are cut on the flat horizontal stones by
the roadside; so it was impossible to tell which was their right way
up, as that would obviously depend upon the position with regard to
them occupied at the time by the man who cut them. Some of them,
however, were on more or less vertical surfaces, so that there could
be no doubt as to their correct positions.
Where any of the others have been compared with signs
previously reported from a different locality, from which they differed
only by their position, the angle through which they have to be
turned, to make their position correspond with the signs with which
they are compared, is intended to be taken in a clockwise direction.
Those scribings that did not occur on the Gubary road, or in the
hattia, were found in the following localities:—
Nos. 230-238 in the northern part of Kharga Oasis, near ’Ain el

Hagar. They were mostly taken from the mouth of a shaft, cut
vertically into a horizontal tunnel, excavated through the rock below
to act as an infiltration gallery, to bring the water from the subsoil
through which it ran to the surface at a lower level.
(Large-size)
No. 219 was found on a loose block of stone at the foot of a
ruined mud tower in Dakhla Oasis, near Bir ’Ain Sheykh Mufta, about
three kilometres to the south-east of Smint el Kharab.
Nos. 221-228 occurred cut on a small stone ruin known as Qasr el
Kadabya, about five kilometres to the south of the village of Tenida,
in Dakhla Oasis.
No. 224 was seen, at the foot of the wall by a doorway, in a small
stone building at the well of ’Ain Amur, on the more northerly road
from Kharga to Dakhla oases.
In addition to the graffiti shown in the plates, a large number of
rough drawings were seen, which want of time, unfortunately, did not
allow me to copy. Many of them were of subjects that did not admit
of reproduction. Among the remainder were hunting and battle
scenes, drawings of a few boats, or ships—one of which was
obviously intended to represent a dahabya—and, in addition to
numerous pictures of camels, those of horses, mules or donkeys
were unexpectedly numerous, considering the small use that is
made of these beasts in that part of the desert.
Among the animals shown in the hunting scenes were several
ostriches, which, though found in the Sudan, are quite unknown at
the present time in the district where the graffiti were seen. In
addition, horned game were represented in a few places; but it was
impossible to determine the species which were intended to be
represented.
In the battle scenes, the men were armed with bows, shields,
spears and swords. I saw no guns to indicate modern drawings, or
shangamangers that might have pointed to a Sudan origin.
The figures in every case were cut on the surface of the Nubian
sandstone, a substance that is easily scratched with a knife. A
portion of some of the figures given in the plates is shown by means
of a dotted line, intended to show that the part thus outlined is
uncertain, owing to the rock having been chipped, or to some other
cause.
The Gubary road, where most of the graffiti were found, runs near
the foot of a scarp that shelters it to a great extent from the strongly
predominant northerly winds. But considering the amount of erosion
that takes place during the frequent sandstorms from this quarter,
after making all allowance for the sheltered position of the rocks
upon which these inscriptions occur, their sharp-cut appearance was
remarkable, seeming to indicate that they do not date from a very
remote period.
Nos. 217 and 218, however, were an exception. These two
inscriptions were cut one above the other, about five feet above
ground level, on a vertical surface facing about north-west. The rock
at this point may perhaps have been unusually soft, but both
inscriptions showed most distinct signs of weathering.
(Large-size)
No. 217 appears to be of special interest, as it seems to be written

partly in primitive Arabic characters and partly in some script, such
as Tifinagh, making use of dotted letters. Inscriptions of this bilingual
character have also been found in the Twat group of oases, in the
Western Sahara, at Ulad Mahmud, in the Gerara District.[26]
The uncertainty as to the correct position of most of these graffiti,
combined with the simple forms that so many of them show and the
rough manner in which they have been drawn, renders comparisons
with other drawings perhaps dangerous, and in any case requires
more expert knowledge than that possessed by the present writer.
But the following notes upon them may perhaps be of interest.
Many of the drawings are unquestionably tribal camel brands, as
an Arab can often be seen cutting his wasm, or brand, on the ground
during a halt, in the same manner as a white man will write his
name.
These wasms are probably of great antiquity, and are said by the
Arabs who use them to date from pre-Mohammedan times. They are
used by the bedawin in a manner analogous to the heraldry of
medieval Europe. Each tribe has its own brand, the junior branches
and offshoots of the clan adopting the original wasm with a
difference, recalling the “marks of cadency” in heraldry.
I was able, with the assistance of my men, to identify the following
brands:—
The circle seen in No. 27 is a wasm of the Hamamla tribe shown
in No. 80 and, with the added stroke, may constitute the brand of
one of its subdivisions.
No. 29 is the wasm of the Khana tribe.
No. 37 of the Jebsia.
No. 43 that of the Zowia. It is curious that this, one of the most
fanatical tribes that have been converted to the tenets of the
Senussia, should make use of the emblem of Christianity as their
badge.
No. 44 may be the brand of the Zoazi tribe that appears in No.
168, and also perhaps in No. 114.
No. 48, in the position shown, is the wasm of the Ulad ben Miriam,
or, if turned as it appears in No. 158, of a Maghrabi tribe known as
the Malif.
(Large-size)
No. 75 was said to be the brand of another Maghrabi tribe, the

name of which I was not able to learn.
No 85 is the mark of the Amaim, which may be also represented
by Nos. 157 and 174.
No. 86, if turned through 180 degrees, would be the wasm of an
Arab tribe from Moab, whose name I could not ascertain.
No. 87 may perhaps be inverted and intended to be the brand of
the Reshaida—a dotted circle surmounted by a cross. Possibly No.
170, though the circle is represented by a square and the figure is
also inverted, may also stand for this wasm.
The Reshaida are an offshoot of the Awazim, whose brand—a
circle and cross, without the “cadency mark” of the dot—appears in
No. 166, with a line added to it on the left-hand side. Reference will
be made to this additional line below. Possibly Nos. 98 and 124 are
also meant for this Awazim brand.
No. 109 is the wasm of the Orfilli tribe.
No. 156 that of the Hassun, said to be an offshoot of a tribe,
whose name I could not ascertain, that have the mark Y for their
brand.
Nos. 172 and 173 are both brands of the well-known Bisharin
tribe.
No. 177 is the mark of the Harb tribe.
No. 179 of the Hawerti tribe.
No. 234 was said by my men to be the brand of a tribe sprung
from another clan whose wasm may be shown in Nos. 73 and 112,
but they were ignorant of the names of both of the tribes.
Many of the other marks shown in the plates are probably derived
from these wasms. The bedawin Arabs are nearly always illiterate,
but are accustomed to communicate with each other by marks
scratched on the ground in the same way that gypsies make use of a
“patteran.” See p. 180 ante.
Such marks, for instance, as No. 50, derived from the Malif wasm,
and 171 and 183, from the brand, are very possibly produced in
this way.
Many of the simpler signs occurred repeatedly, and in addition the
group shown in No. 2 was seen twice, and that in No. 14 several
times, while the combination No. 25 in one place was repeated no
less than thirty-three times in three horizontal lines. Similar marks to
those No. 95 occurred in several places, generally in groups of three,
placed as shown in the plate.
No. 18, the seal of Solomon, is not uncommonly seen in the rock
inscriptions of the Western Sahara. It takes several forms, each of
which may have a dot in the centre, thus: . Its commonest form
seems to be that shown in No. 18, but sometimes one of the
triangles of which it is composed is drawn with a heavier line than
the other, thus: . It is also represented in at least one case-on the
Col de Zanaga, in the Figuig district—surrounded by a waved line
producing a kind of rosette . In addition to these forms, the false
seal of Solomon, or five-pointed star, constructed by a continuous
line is also seen in this district, but I did not happen to come
across it in the Libyan Desert. These signs are all much used by the
native magicians.
(Large-size)
No. 88 was apparently the tracing of a leathern sandal and was
lifesize. The outline of both shod and unshod feet, sometimes the
right foot being traced and at others the left, were of not infrequent
occurrence. They are also found in the Western Sahara at Qasr el
Jaj Ahmer, in the Geryville district, and at Guebar Rashim. The
outlines of hands also occur; but I did not see any of the latter in the
Libyan Desert.
Of the other signs, the mark which occurs, in combination with

others, in Nos. 14 and 244, has also been found on the temple of
Soleb, in the midst of an inscription. The sign , No. 74, also
appears here.[27]
Nos. 42, 43 and 49 were reported by the late Mr. Oric Bates from
Marmarica.[28] So, too, were Nos. 63 and 71, if turned through 180
degrees. The small circle that appears as No. 80, and in combination
with other signs in Nos. 9, 27, and in several of the groups shown in
the plates, and also No. 162, if turned through a right angle, also
figure in this collection. Among which, too, is the sign which may
be identical with the mark in the inscription given as No. 219.
In some of the inscriptions found at the Gara esh Shorfa, in the
Aulef district of Tidikelt in the Twat group of oases, the vowel dot
(tagherit) of the Libyco-Berber script is often enclosed by a line that
forms a kind of loop round it, recalling the cartouche frequently used
in modern Tifinagh writing to surround the different words of a
sentence; the is also sometimes enclosed in the same manner,
the letters when thus treated having the following appearance: ,
. The right-hand signs of No. 63 and No. 132, No. 146 and
several other of the graffiti shown in the plates may perhaps be
examples of this practice, which also is very possibly illustrated by
the sign that occurs in No. 219. The cartouche treatment
appears in No. 245.
Some of the more complicated signs may only be idle scratchings;
drawings, for instance, such as No. 34 are often to be seen upon
blotting pads, being made by some writer during the intervals of his
composition. But such signs as Nos. 16, 142, 148, 149 and 153
recall the curious ligatured monograms sometimes used by the
modern Tawarek in their writings, or the cryptograms, mentioned by
Duveyrier and H. Barth, that the Tawarek women sometimes amuse
themselves by inventing, that can only be deciphered by those to
whom they have imparted the key.[29]
The circles in Nos. 203, 211 and 212 represent small cups about
two inches in diameter and were used perhaps for some game such
as harubga, or possibly for divination in the manner described by
Mohammed et Tounsi.[30] Somewhat similar groups of cups have
been found in the Twat Oasis group at ’Ain Guettara, and also in the
Geryville district, at El Jaj Mohammed and Shellala Dahrania.
Nos. 224—the left-hand portion—242 and 243 probably represent
human beings. In 224 the five fingers of two hands and the long hair
in the star like a mark above them occur in several other undoubted
drawings of figures that were seen, but are not shown in the plates. It
is, however, doubtful whether it is the feet or the hands that are
represented in Nos. 242 and 243. Among the figures that are not
given in the plates, several appeared in which the hair was
represented by dots instead of the lines in No. 224.
Rough drawings of camels were often seen. They are shown in
Nos. 193 and 196, and possibly also Nos. 194, 195 and 131 are
intended to show them. Nos. 193 and 195 may perhaps represent
camels carrying a travelling tent, such as are used by wealthy
women, and sometimes also by men on a journey. No. 193 may
possibly represent a beast with two humps, though these, of course,
are never seen in North Africa. No. 196 apparently carries a rider,
mounted on a riding saddle. Among other creatures appearing in the
plates, No. 210 is presumably a man being swallowed by a
crocodile.
Rough drawings of camels, of a very similar type to those here
reproduced, have been found by Lieut.-Col. Tilho in the oasis of
Harda, in Borku; and I came across others myself in a cave, near
Marsa Matru, on the North Egyptian coast. The latter were found in
conjunction with drawings of a cannon being fired and of a paddle-
wheel steamer, which appeared to be contemporaneous, so
evidently they were of a comparatively recent date.
The drawings of ostriches and the fragments of their shells which
are often to be found in the Libyan Desert, even in the
neighbourhood of the Egyptian oases, has been held to show that
they once existed wild in this part of the desert. But the argument is
by no means conclusive; ostrich eggs used frequently to be brought
from the Sudan by the old slave-trading caravans, who used them as
food, and the drawings no more show that ostriches inhabited this
part than the pictures of boats show that dahaybas once sailed over
the desert in the neighbourhood, say, of Dakhla Oasis. The
occurrence of these, and of drawings of antelopes and other wild
animals, merely show that some of the travellers who used these
roads came from districts where the creatures they represented
could be seen.

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Advances in magnetic materials :

processing, properties, and

Biota Grow 2C gather 2C cook Loucas

Advances in Materials Processing Yafang Han

Advances in Materials and Pavement Performance

Science and Principles of Biodegradable and

Magnetic Properties of Paramagnetic Compounds Magnetic

Magnetic Properties of Paramagnetic Compounds Magnetic

Magnetic Properties of Paramagnetic Compounds Magnetic

Magnetic Properties of Paramagnetic Compounds Magnetic

Advances in Magnetic Materials: Processing, Properties, and Performance,

Boca Raton London New York

CRC Press is an imprint of the

No claim to original U.S. Government works

Printed on acid-free paper

International Standard Book Number-13: 978-1-4987-0671-1 (Hardback)

Chapter 1 Magnetic Behavior of Nanostructured Materials .................................1

Chapter 2 Elemental Ferromagnetic Nanomaterials: Their Preparation,

Chapter 3 Magnetic Materials for Nuclear Magnetic Resonance and

Chapter 4 Plasma Nanotechnology for Nanophase Magnetic Material

Chapter 5 Compositional Optimization and New Processes for

Chapter 6 Layered Two-Phase Magnetoelectric Materials ............................... 373

Chapter 7 Rapidly Solidified Rare-Earth Permanent Magnets:

Chapter 8 Magnetic Materials Prepared Using Polyacrylamide Gel Route .....509

Chapter 9 Perpendicular Magnetic Anisotropy in Magnetic Thin Films ......... 581

Chapter 10 Catalytic Application of Magnetic Nanocomposites ....................... 627

Index ...................................................................................................................... 721

Professor Dongliang Zhao has been the vice

Indra Purnama S. F. Wang

Rajdeep Singh Rawat Ying Wang

D. K. Satapathy Sam Zhang

Samarpita Senapati Dongliang Zhao

Suneel Kumar Srivastava Yinghuai Zhu

Tat Joo Teo X. T. Zu

1.6 Fabrication of Magnetic Nanostructured Materials .......................................44

1.2 COMMON TERMINOLOGY IN THE WORLD OF MAGNETISM

where µ0 = 4π × 10−7 H/m is the permeability of free space (H = Henry, Vs/A). We

• Diamagnetism occurs due to the external magnetic field that induces a

(a) (b) (c)

antiferromagnetics are aligned in an antiparallel fashion. Antiferromagnetic

1.2.1.1 Magnetic Moment in Atom

FIGURE 1.2 Itinerant electron system at dysprosium. (Redrawn based on D. Givord,

E spin −orbit = λLS (1.4)

1.2.1.2 Magnetic Moments in Clusters

anisotropy which are related to the local reduction of symmetry. However, in

1.2.2 Magnetic order

(a) (b) (c)

FIGURE 1.5 Schematic of magnetic structures: (a) ferromagnetic, (b) antiferromagnetic

H m,0 = nMs,0 (1.8)

FIGURE 1.6 Schematic of temperature dependence on spontaneous magnetization for dif-

1.2.2.1 Magnetic Moment in Rare Earth Elements

1.2.2.2 Magnetic Moment in Transition Metal Compounds

1.2.2.3 Magnetic Moment in Ferromagnetic Materials

mechanism between magnetic moments is insensitive to minor changes in the atomic

1.2.3 Magnetic anisotropy

1.2.3.1 Crystalline Anisotropy

(a) (b) (c)

1200 1200 400

1.2.3.2 Shape Anisotropy

where Na and Nc are demagnetization factors. For spheres, Na = Nc as a = c. It can be

(a) (b) (c) (d)

FIGURE 1.9 Schematic of different forms of shape anisotropy. (Redrawn based on K. M.

1.2.3.3 Other Anisotropy