Week07 Plasmonics I

9/8/2023
EEE 6505 – Nanophotonics and Plasmonics
EEE Plasmonics I
6505
Week 09
Lecture 06
Dr. Sajid Muhaimin Choudhury, Assistant Professor

Department of Electrical and Electronics Engineering
Bangladesh University of Engineering and Technology
Recap so far
Light interaction with small objects (d < )
• Insulators (Rayleigh Scattering, blue sky..)
• Semiconductors (Size dependent absorption, fluorescence..)
• Metals…Resonant absorption at sp
Microparticles
• Particles with d   (-independent scattering, white clouds)
• Particles with d >>  (Intuitive ray-picture useful)
Dielectric photonic crystal
• Molding the flow of light

© 2008 by Princeton U Press Photonic Crystals: Molding Flow of Lights
EEE 6505 – Nanophotonics and Plasmonics Dr. Sajid Muhaimin Choudhury 2
Department of EEE, BUET
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EEE 415 - Week 01 1

9/8/2023
Introduction: Plasmonics
• Plasmonics = Field dealing with the resonant interaction of light with
conduction electrons in metals

3
What is Plasmon?
• Plasma oscillations, also known as Langmuir waves, are
rapid oscillations of the electron density in conducting media such as
plasmas or metals in the ultraviolet region.
• In physics, a plasmon is a quantum of plasma oscillation. Just as light (an
optical oscillation) consists of photons, the plasma oscillation consists of
plasmons.
• The plasmon can be considered as a quasiparticle since it arises from the
quantization of plasma oscillations, just like phonons are quantizations of
mechanical vibrations. Thus, plasmons are collective (a discrete number)
oscillations of the free electron gas density.
• Since plasmons are the quantization of classical plasma oscillations, most
of their properties can be derived directly from Maxwell's equations.
https://en.wikipedia.org/wiki/Plasmon
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Plasmon-Polaritons
What is a plasmon ?
• Compare electron gas in a metal and real gas of molecules
• Metals are expected to allow for electron density waves: plasmons
Bulk plasmon
• Metals allow for EM wave propagation above the plasma frequency
They become transparent!
Surface plasmon z
E Strong local field
Dielectric
Metal I
H
Note: This is a TM wave
• Sometimes called a surface plasmon-polariton (strong coupling to EM field)

5
Local Field Intensity Depends on Wavelength

z
z
D << o
I I
Long wavelength Short wavelength
Characteristics plasmon-polariton • Strong localization of the EM field

• High local field intensities easy to obtain

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Applications
Technological applications in
• Sub-diffraction limited optics
• Bio and Chemical sensing
• Surface-enhances spectroscopy
• Solar energy harvesting
• Medicine (therapy, drug-delivery, imaging)
• Information processing (Waveguiding,
Optoelectronics, Integrated Circuits)
• Catalysis and sustainability
• Novel optical media (transparency, anisotropy,
chiral, nonlinear)
7
Discovery of Plasmon
David Pines and David Bohm, A collective description of electron
interactions: II. Collective vs individual particle aspects of the
interactions, Phys. Rev. 1952, 85, 338
Theory: Introduced the concept of “Plasmon” (bulk)
Hiroshi Watanabe, Experimental evidence for the collective nature of
the characteristic energy loss of electrons in solid studies on the
dispersion relation of plasma frequency, J. Phys. Soc. Japan 1956
Exp: Evidence supporting a “collective plasma” (bulk)
Rufus H. Ritchie, Plasma losses by fast electrons in thin films, Phys.
Rev. 1957, 106, 874
Theory: Predicted existence of “Surface Plasmon”
Cedruc J. Powell and John B Swan, Origin of the characteristic
electron energy losses in aluminium, Phys. Rev. 1959, 115, 869
Exp: Observation of the Surface Plasmons
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Materials for Plasmonics

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Electronic Band Structure of Metal

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Light Interaction with Matter: Maxwell’s Equations

Maxwell’s Equations
Divergence equations Curl equations
B
Gauss Law  D  f  E   Faraday’s Law
t
D Ampere’s Law
Gauss Law for magnetism  B  0  H  J
t
D = Electric flux density B = Magnetic flux density
E = Electric field vector H = Magnetic field vector

 = charge density J = current density

11
Relation between Field and Flux
Electromagnetic Properties of a Medium is dependent on the Polarization, P and

Magnetization, M of a medium
D(r,t) = ε0(r) E(r,t) + P(r, t)
B(r,t) = μ0(r) H(r,t) + M(r, t)

ε0 is permittivity of the medium, μ0 is the permeability of the medium
For linear source-free medium D = ε0ε E [P = ε0χeE]

B = μ0 μ H [ M = χmH ]
jc = σE © 2008 by Princeton U Press Photonic Crystals: Molding Flow of Lights
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The dielectric permittivity ε governs the behavior of matter under an

external electric field.
ε(ω) = ε1(ω) + iε2(ω) and σ(ω) = σ1(ω) + iσ2(ω) are complex functions of
iσ(ω)
angular frequency and linked by ε(ω)=1+
ε0ω
Experimentally, dielectric permittivity is determined via the complex
refractive index 𝑛(ω) = n(ω) + iκ(ω), where 𝑛 = ε
ε1=n2 - κ2 and ε2=2nκ
n = refractive index  Speed of EM wave in medium
κ = extinction coefficient  absorption of EM waves in the medium

13
Dielectric Function of Free electron Gas

The optical properties of metal can be described by a free electron
model: free conduction electrons constitutes a plasma – a gas of
charged particles that react collectively to EM fields.
Can be described as a
harmonic oscillator
(Drude-Sommerfeld)
The electrons displaced by the external field, experience a restoring

force and start to oscillate
From the simple picture, we can write an equation of motion for time-
𝐫 𝐫
harmonic field me + meΓ = 𝑒𝐄𝟎𝑒
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Drude Somerfield Theory

𝐫 𝐫
The equation of motion for the free electron me + meΓ = 𝑒𝐄𝟎𝑒
Yields solution in form 𝐫(t) = − 𝐄(t)
ω) (ω
The displaced electrons contribute to macroscopic polarization P=ner
ω
𝐏=− 𝐄 which leads to 𝐃 = ε0 1 − 𝐄
(ω ω) (ω ω)
where ωp = is the bulk plasma frequency of the free electrons

ε0
Since D = ε0ε E we define Drude dielectric permittivity as

ω
εdrude(ω) = 1 − 2
ω + 𝑖Γω
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Electronic Band Structure
The parabolic sp bands explain why free electron gas

description works well for most metals
EEE 6505 – Nanophotonics and Plasmonics © 2008 by Princeton U Press Photonic Crystals: Molding Flow of Lights
Dr. Sajid Muhaimin Choudhury 16
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Drude Somerfield Theory

The free electron model is an ideal model where ε → 1 at ω ≫ ωp
Extension need for nobel metals (Au, Ag, Al) at ω > ωp
In this region response is dominated by
the s-electrons. The filled d-bands close
to the Fermi level generate a highly
polarized environment with the positive
ion background: P∞=ε0(ε∞−1)E
Drude permittivity now reads
ω
εdrude(ω) = ε∞ − 2
ω + 𝑖Γω
The collision frequency (damping) Γ = 𝑣𝐹/𝑙 is expressed as a
function of Fermi velocity 𝑣𝐹 and electron mean free path 𝑙.

17
Interband Transitions
Effects of the interband (sp → d) transitions: Example of silver
In the bulk, the mutual polarization of Ag 5s and 4d electrons causes a
renormalization/screening of the bulk plasma frequency
from ωp=9.2 eV (unscreened)
to ωp∗ ≈ 3.76 eV (actually observed)
Correspondingly, the surface plasmon frequency is also screened

from ωs = 6.5 eV (unscreened)
to ωs∗ ≈ 3.64 eV (actually observed)
Liebsc, Phys Rev Lett 1993, 71, 145

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Interband Transition: Lorentz Model

At high frequencies (visible) the response of
the bound valence electrons (d band) limits the
validity of the Drude-Sommerfeld model
For d-(bound/valence electrons)
𝜕 2𝐫 𝜕𝐫
m 2 + m𝛾 + 𝛼𝐫 = 𝑒𝐄𝟎𝑒
𝜕𝑡 𝜕𝑡 Restoring Force
ω= 𝑛𝑒2/𝑚ε0
ω
Leads to εinterband(ω) = 1+
(ω −ω ) ω
Drude-Lorentz model
ω ω
ε (ω) = 1 − +
ω ω (ω −ω ) ω © 2008 by Princeton U Press Photonic Crystals: Molding Flow of Lights
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Surface Plasmon Polariton: EM Wave at Interface

By definition, Surface Plasmon Polaritons (SPP) are quanta of surface-charge-
density oscillations. Classically, they are solutions of Maxwell’s equations
under certain boundary conditions
SPP = charge oscillations in the metal (surface plasmon) and EM
wave in the dielectric (polariton)
ε ,μ ε ,μ
Let’s consider a planar interface 2 2
ε
𝑑
, μ
𝑑
ε1, μ1 𝑚 𝑚
At z=0 between ε1(ω) and ε2(ω)
Homogenous solutions (eigenmodes; solutions in the absence of
external excitation) of Maxwell’s equations are solutions of the wave equation
ω
  E(r, ω) - ε (r, ω) E(r, ω) = 0

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Surface Plasmon Polariton: EM Wave at Interface

Solving the wave equation separately in each region and applying proper
boundary conditions lead to sets of self-consistent solutions with p- and s-
polarized modes.
TM or p-polarized TE or s-polarized
However, surface-bound EM modes
do not exist for s-polarized excitations E
E
Solution for TM-modes: H
H
𝐸 ε2, μ2 k ε𝑑 , μ𝑑 k
ε1, μ1 ε𝑚, μ𝑚
𝐸j= 0 e ( )
e ( 𝑗 = 1,2 )
𝐸
The wave vector parallel to the interface 𝑘𝑥 is conserved, leading to
𝑘 + 𝑘 = 𝜀𝑗𝑘2

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Surface Plasmon Polariton Dispersion Relation

Field must satisfy Gauss law (∇. 𝐃 = 0): 𝑘𝑥𝐸𝑥𝑗 + 𝑘𝑧𝑗𝐸𝑧𝑗 = 0
The boundary conditions (i.e., 𝐄∥ and 𝐃⊥ are continuous) lead to
𝐸𝑥1 − 𝐸𝑥2 = 0 and 𝜀1𝐸𝑧1 − 𝜀2𝐸𝑧2 = 0
For non-trivial solution of the 4 equations,
1 0 1 0 
0 1 0  2 
det   kx  1k z 2   2 k z1   0
 kx k z1 0 0 
 
 0=
Which leads to 𝑘𝑧1 0 𝑘 k xfor k𝑘z 2 ≠
𝑧2 𝑥  0

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Surface Plasmon Polariton Dispersion Relation

Using 𝑘 + 𝑘 = 𝜀𝑗𝑘2 and 𝑘𝑧1 = 𝑘𝑧2 we obtain the SPP dispersion relation
2
1 2 2 1 2
2
1 2 1 2
2
,
1 2

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Surface Plasmon Polariton: Condition of Existance

From the dispersion relations:
propagating interface EM waves
exists for the following conditions:
𝜀1 × 𝜀2 < 0, 𝜀1 + 𝜀2 < 0
(i.e. 𝑘𝑥 is real and 𝑘𝑧 is purely imaginary)
So, real part of one of the dielectric permittivity must be negative:
metal

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Dispersion Relation Surface-Plasmon Polaritons

Relations between k vectors z kzd d  1
k zm k
• Condition for SP’s to exist:  zd
Example
m d kzm  m  1
z Air
• Relation for kx (Continuity E//, H//) : kxm  kxd Example
SiO2
true at any boundary

k x2  k zi2   i  
2
• For any EM wave:

c
 Dispersion relation

2
• Both in the metal and dielectric: k sp  k x   i    k zi
2
c 𝜔 𝜀 𝜀
𝑘 =
kzm kzd 𝑐 𝜀 +𝜀

m d
25
Plot of the dispersion relation

𝜔 𝜀 𝜀
• Last page: 𝑘 =
𝑐 𝜀 +𝜀
r
• Plot dielectric constants d dielectric
metal
p 
 d
 sp
𝜔 𝜀 𝜀 𝜔 k   d
• Low : 𝑘 = lim ≈ 𝜀 c
𝑐 → 𝜀 +𝜀 𝑐 
sp
• At  = sp (when m = -d): kx  
• Note: Solution lies below the light line k

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Surface Plasmon Polariton: Dispersion Diagram
Radiative modes
𝑘𝑥 real, 𝑘𝑧 imaginary 𝑘𝑥 real, 𝑘𝑧 real
𝜔 Light Cone
𝜔 = 𝑐𝑘𝑥
Plasmon Polariton
𝜔 = 𝑐𝑘𝑥/n
𝜔= 𝜔 + 𝑐𝑘𝑥 2
𝜔𝑝 Bulk Plasmon
𝜔𝑝 Surface Plasmon
Bound modes
2
Surface Plasmon Polariton
(𝜀 +𝜀 )
𝜔= 𝑐𝑘𝑥
𝜀 𝜀
𝑘𝑥
 p2 2 p
 = sp when:  m  1 2   d 2   p2    d 2   p
2 
 1  d 1  d
Red (SPP) and Blue (free electron) do not cross the light line
Cannot directly excited w/EM waves (momentum mismatch)
27
Excitation Surface-Plasmon Polaritons (SPPs) with Light

Problem SPP modes lie below the light line
• No coupling of SPP modes to far field and vice versa (reciprocity theorem)
• Need a “trick” to excite modes below the light line
Trick 1: Excitation from a high index medium
• Excitation SPP at a metal/air interface from a high index medium n = nh
 c  c

k k nh
sp
e
kh  ksp
k Air k sp kh k
• SPP at metal/air interface can be excited from a high index medium!
EEE 6505 •– How does this work

Nanophotonics in practice ?
and Plasmonics © 2008 by Princeton U Press Photonic Crystals: Molding Flow of Lights
Dr. Sajid Muhaimin Choudhury 28
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Excitation Surface-Plasmon Polaritons (SPPs) with Light

Kretchmann geometry (Trick 1) From dispersion relation
ksp
• Makes use of SiO2 prism k//,SiO2


• Create evanescent wave by TIR
kSiO2
• Strong coupling when k//,SiO2 to ksp E
H
• Reflected wave reduced in intensity

c
  c
k n
k
sp
e
Note: we are matching energy and momentum k Air ksp kSiO2 k

29
Surface-Plasmon is Excited at the Metal/Air Interface

Kretchmann geometry
k sp , A ir
• Makes use of SiO2 prism
ksp,SiO2
 • Enables excitation surface plasmons at the Air/Metal
k S i O2 interface
E
H • Surface plasmons at the metal/glass
interface can not be excited!
 Light line air Light line glass

 sp , A IR Surface plasmon Metal/Air interface
sp,SiO 2
e Surface plasmon Metal/Glass interface
k //,SiO2   d
 sin   k
sp
c
kAir k ksp,SiO2 k
k s p , A irS i O 2 © 2008 by Princeton U Press Photonic Crystals: Molding Flow of Lights
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Quantitative Description of the Coupling to SPP’s

Calculation of reflection coefficient
2 d
• Solve Maxwell’s equations for 1
• Assume plane polarized light 0
• Find case of no reflection E

H D
r01p  r12p exp 2ik z1d 

2 2
Ep
• Solution (e.g. transfer matrix theory!) R  rp 
E0 1 r01p r12p exp 2ikz1d 
Plane polarized light

k k  k k 
p
where rik are the amplitude reflection coefficients rikp   zi  zk   zi  zk 

 i  k 

 i k 
Also known as Fresnel coefficients (p 95 optics, by Hecht)
Notes: Light intensity reflected from the back surface depends on the film thickness
There exists a film thickness for perfect coupling (destructive interference between two refl. beams)
When light coupled in perfectly, all the EM energy dissipated in the film)
31
Dependence on Film Thickness
Critical angle

R E
H
laser detector
• Width resonance related to damping of the SPP

• Light escapes prism below critical angle for total internal reflection
• Technique can be used to determine the thickness of metallic thin films
© 2008 by Princeton U Raether,
Press Photonic“Surface plasmons”
Crystals: Molding Flow of Lights
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Surface Plasmon Polariton: Reflectivity Measurement

Different air gap between Different thickness of a
The gold film and the glass Gold film on glass
g=200 nm: SPP radiation damping d=20 nm (<skin depth): SPP field couples
SPP field couples back to glass back to glass
g=1000 nm: SPP not efficiently excited d=80 nm (>skin depth): SPP not efficiently excited
λ=632.8nm Novotny, Principles of Nano-Optics
33
FDTD Simulation: Kretschmann

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35
Interband Transitions

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Excitation Surface-Plasmon Polaritons with Gratings (trick 2)

Grating coupling geometry (trick 2)
• Bloch: Periodic dielectric constant couples waves for which the k-vectors
differ by a reciprocal lattice vector G
• Strong coupling occurs when k//,SiO2  k sp  mG

E
k//,SiO2

 ke   d sin  H
where: ke
c 
   m d 
1/ 2
k//,SiO2 ksp P
ksp   
c  m  d 
G  2 P   c
k
sp
• Graphic representation
e
2 2 k//
 k //,SiO2
© 2008 by Princeton
P U Press Photonic Crystals: Molding Flow of Lights
EEE 6505 – Nanophotonics and
P Plasmonics Dr. Sajid Muhaimin Choudhury 37
37
Excitation Surface-Plasmon Polaritons with Dots (Trick 3)

Dipolar radiation pattern
d = 200nm
h = 60nm
E
700 nm
E-fields
• Strong coupling: k//,SiO2  k sp  kdot Radiation

Spatial Fourier transform of the dot contains
significant contributions of kdot values upto 2/d • Dipole radiation in direction of charge oscillation!
H. Ditlbacher, Appl. Phys. Lett. 80, 404 (2002) • Reason: Plasmon wave is longitudinal
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Other Excitation Geometries
• Radiation pattern more directional
• Divergence angle determined by spot size

200nm 700nm
60nm
• Illumination whole line radiation  to line
• Pattern results from interference 2 dipoles
H. Ditlbacher, Appl. Phys. Lett. 80, 404 (2002)

39
Excitation Surface-Plasmon Polaritons from a Scattering Particle

Atomic Force Microscopy Image Near-field Optical Microscopy Image
200 nm 7.5 7.5
100 nm
5.0 5.0
0 nm
Scatter site
2.5 2.5
0 0
0 2.5 5.0 7.5 0 2.5 5.0 7.5
Distance (m) Distance (m)
Excitation direction
• Scattering site created by local metal ablation • Scattering site brakes translational symmetry
with a 248 nm Excimer laser (P=200 GW/m2)
• Enables coupling to SPP at non-resonant angles
I.I. Smolyaninov, Phys. Rev. Lett. 3877 (1996)

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Excitation SPPs on stripes with d < 

Excitation using a launch pad
Atomic Force Microscopy image
200 nm
Al
Near Field Optical Microscopy image
End stripe
Note oscillations

EEE 6505 – Nanophotonics and Plasmonics Dr. Sajid
J.R. Krenn et al., Europhys.Lett. Muhaimin
60, 663-669 Choudhury
(2002) 41
41
Excitation SPPs on stripes with d < 
Atomic Force Microscopy image

Intensity (a.u.)
Near Field Optical Microscopy image
Distance (m)
End stripe
Note oscillations

EEE 6505 –O
Note: Nanophotonics and Plasmonics
scillations are due to backreflection Dr. Sajid Muhaimin Choudhury 42
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2D Metallo-dielectric Photonic Crystals

Full photonic bandgap for SPPs Scanning Electron Microscopy image (tilted)
• Hexagonal array of metallic dots

metal
glass
300 nm
300 nm
S.C. Kitson, Phys Rev Lett. 77, 2670 (1996)
  c
k
• Array causes coupling between waves sp
for which:
ksp = /P or sp=2/ksp= 2P Gap e Gap
• Gap opens up at the zone boundary 2   2

EEE 6505 – Nanophotonics and Plasmonics  k// Molding Flow of Lights
© 2008 by Princeton U Press Photonic Crystals:
P P P Dr. PSajid Muhaimin Choudhury 43
43
Guiding SPPs in 2D metallo-dielectric Photonic Crystals

Guiding along line defects in hexagonal arrays of metallic dots (period 400 nm)
• Scanning electron microscopy images
Linear guides Close-up Y-Splitter
• SPP is confined to the plane

• Full photonic bandgap confines SPP to the line defect created in the array

EEE 6505 – Nanophotonics and Plasmonics S.I. Bozhevolnyi, PhysDr.
RevSajid
Lett.Muhaimin Choudhury
86, 3008 (2001) 44
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Guiding SPPs in 2D metallo-dielectric Photonic Crystals

First results
• Scanning electron microscopy images
Atomic Force Microscopy image Near-field Optical Microscopy image
Dot spacing: d = 380 nm

Excitation: e = 725 nm
SPP: sp = 760 nm = 2d
EEE 6505 – Nanophotonics and Plasmonics S.I. Bozhevolnyi, PhysDr.
RevSajid
Lett.Muhaimin Choudhury
86, 3008 (2001) 45
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Surface and Bulk Plasmon in EELS
ωp ωs

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SPP Applications

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SPP Applications

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Key Physical Quantities: Common Plasmonic Materials

49
EEE Plasmonics II
Localized Surface Plasmon
6505
Week 09
Lecture 06
Dr. Sajid Muhaimin Choudhury, Assistant Professor

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LOCALIZED SURFACE
PLASMON
51
Dr. Sajid Muhaimin Choudhury
51
EEE 415 - Week 01 26

Week07 Plasmonics I

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9/8/2023

EEE 6505 – Nanophotonics and Plasmonics

Dr. Sajid Muhaimin Choudhury, Assistant Professor

• Particles with d >>  (Intuitive ray-picture useful)

Dielectric photonic crystal

• Molding the flow of light

EEE 415 - Week 01 1

© 2008 by Princeton U Press Photonic Crystals: Molding Flow of Lights

EEE 415 - Week 01 2

• Metals are expected to allow for electron density waves: plasmons

• Sometimes called a surface plasmon-polariton (strong coupling to EM field)

Local Field Intensity Depends on Wavelength

Characteristics plasmon-polariton • Strong localization of the EM field

© 2008 by Princeton U Press Photonic Crystals: Molding Flow of Lights

EEE 415 - Week 01 3

EEE 415 - Week 01 4

Materials for Plasmonics

© 2008 by Princeton U Press Photonic Crystals: Molding Flow of Lights

Electronic Band Structure of Metal

© 2008 by Princeton U Press Photonic Crystals: Molding Flow of Lights

EEE 415 - Week 01 5

Light Interaction with Matter: Maxwell’s Equations

D = Electric flux density B = Magnetic flux density

E = Electric field vector H = Magnetic field vector

© 2008 by Princeton U Press Photonic Crystals: Molding Flow of Lights

Relation between Field and Flux

Electromagnetic Properties of a Medium is dependent on the Polarization, P and

D(r,t) = ε0(r) E(r,t) + P(r, t)

B(r,t) = μ0(r) H(r,t) + M(r, t)

For linear source-free medium D = ε0ε E [P = ε0χeE]

EEE 415 - Week 01 6

The dielectric permittivity ε governs the behavior of matter under an

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Dielectric Function of Free electron Gas

The electrons displaced by the external field, experience a restoring

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Drude Somerfield Theory

where ωp = is the bulk plasma frequency of the free electrons

Since D = ε0ε E we define Drude dielectric permittivity as

Electronic Band Structure

The parabolic sp bands explain why free electron gas

EEE 415 - Week 01 8

Drude Somerfield Theory

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Correspondingly, the surface plasmon frequency is also screened

Liebsc, Phys Rev Lett 1993, 71, 145

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Interband Transition: Lorentz Model

Surface Plasmon Polariton: EM Wave at Interface

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EEE 415 - Week 01 10

Surface Plasmon Polariton: EM Wave at Interface

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Surface Plasmon Polariton Dispersion Relation

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Surface Plasmon Polariton Dispersion Relation

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Surface Plasmon Polariton: Condition of Existance

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Dispersion Relation Surface-Plasmon Polaritons