Plasmonics and Waveguides: Engineering Plasmon-Polaritons in Metallic Nanostructures

Plasmonics and Waveguides
Engineering plasmon-polaritons in metallic nanostructures

Luca Dal Negro
ECE & Photonics Center, Boston University, USA
dalnegro@bu.edu
http://www.bu.edu/nano/
Nanoplasmonics
Plasmonics: engineering charge density oscillations bound at metal-dielectric interfaces
Key Features:
Why metals:
Electron density oscillations coupled to EM waves

Strong field intensity enhancement at metal surfaces
Optical fields nanoscale localized (sub-)
Largely tunable optical properties
Enormous polarizability
Resonant behavior
Classical EM description
Design Parameters
Near-Field
Coupling Coupling
Photonic
Material / Diffractive
Size
Shape
Engineering polarization bound charges in nanomaterials (=Polaritonics)
enables the control of strongly enhanced radiative and non-radiative fields
Hanke et al., Nano Lett., 12 (4)
2037 (2012)
200nm
Example: Plasmon
Resonances
Metallic
Nanostructures
Yan et
al., Opt. Mat. Exp.,in
1, 8,
1548
http://www2.mpipSuh, Nano Lett., 12, 1 269 (2012)
Walsh et al., Nano Lett., 13 (2011)

(2), 786 (2013)
Hanke et al., Nano Lett., 12 (4) 2037
Y. Chu, et. al. Applied Physics Letters 93, 181108
(2012)
(2008).
mainz.mpg.de/groups/bonn/research/menges
Toroghi et al, Appl. Phys. Lett. 100, 183105 (2012)
_bernhard/cleanroom
Example: Surface modes of small particles

Molecular Emission
Localized Surface Plasmons

=
Collective electron oscillations
et al., Sci. Rep., 3, 1505 (2013)
Chen
Field
enhancement
Resonant
Solar
response
Quadrupole plasmon resonance

Enhanced
light-matter
coupling
Collective, in-phase
motion of electrons
3 / spectroscopy
Optical sensing
Nanoscale dnonlinear optics
f a
Field concentrators
NP m
f d light sources
Nanoscale
NPharvesting
2 m
Solar energy
Imaging / optical detection

Singular optics
Half of the electron clouds moves parallel

to the applied field and half moves anti-parallel
Atwater & Polman, Nat. Mat.. 9, 205 (2010)
Sensors
fq a3
NP m
gq
NP 3 / 2 m
particles
Hao, E.; Schatz,
etFor
al.,www.semrock.com
J.larger
Chem. Phys,
120, 357 (2004)
Semrock,
Radiation engineering with plasmonic coupled

COBRA DANE phased-array radar
arrays
34,000 antennas, Siberia's Kamchatka Peninsula
Photonic-plasmonic coupling regimes in arrays

Radiative vs Non-radiative fields: always think of Hertzian dipoles first
Near Field Coupling in Clusters
Near-field of one particle induces additional
polarization in close particles
Transverse field 1/r

Quasi-static near-field coupling
Longitudinal
fields 1/r2, 1/r3
Radiative
jkr
r r jkr
k 2 1 r 3r(re
1
p)
p e
E
(
r
)
(
p
r
)
E (r ) jk
4r r 4 r
Propagating;
Diffraction-limited;
Heisenberg principle for photons
Diffractive Coupling between Clusters

-Propagating scattered light from one
particle can be scattered by another
Transverse;
px x hk x x h
Non-propagative (reactive);
1
Sub-wavelength
localized;
x
x
Large nanoscale
intensity;
Using evanescent (non-propagative) fields the

spatial bandwidth of photons can be dramatically
enhanced.
Principles of Nano-Optics, L. Novotny, .B. Hecht, Cambridge (2006)
Theory of Optical Constants
Why
Why
Why
Why
polished aluminum cooking pan is shiny but opaque transmitted light ?

glass windows are transparent but weakly reflecting ?
all materials behave like metals at high frequencies ?
radio-waves do not escape from the atmosphere while satellite waves do ?
Models are needed to explain the (linear) optical

response of materials
Copyright 2008, Boston University
Optics of conducting media

D
H
J ext
t
B
E
t
B 0
D ext
For monochromatic waves:
E (r , t ) Re E (r )e jt
/ t j
H jD J ext
Assuming:
We can write:
D 0E 0 (1 ) E
J E
H j eff E
Where we defined the: Effective electric permittivity:
eff
, ,

0 j 0 (1 ) j

are generally complex!
Physical meaning
If the imaginary part of the material coefficients or is nonzero, the amplitude
of a plane wave will decrease as it propagates through the medium absorption
Where the complex permittivity is defined as:
0 (1 ) i
2 z
Ec E0 exp
exp i nkz t
Bound charge current density

Free charge current density
Complex phenomenological coefficients of a medium are equivalent to a phase

difference between P and E (or H and B) and are manifested by absorption
Both conductivity and susceptibility contribute to the imaginary part of the permittivity:
Im( ) Im( ) Re
Complex refractive index

Using the ansatz: E E0 f (k r t )
c2k 2
( )
2
c
c
~
k
( ) n ( )
complex dielectric function
Where we can define:
we can obtain the dispersion relation:
n%
( ) n i ( )
Complex refractive index
c
v ph
Re(k ) n( )
vg
k
0
n( )
Snells law refractive index

(real dispersion)
4
( )
( )
0
Absorption coefficient
Intensity extinction
(energy dissipation)
General relations
n% ( )
2
' n
'' 2n
2
(n, ) ( ', '')
'' '
2
'
'' '
2
n%
( ) n i
( ) ' i ''
Or, equivalently:
'
k ( n i )
c
are connected and describe the

intrinsic optical properties of matter
Both the real and imaginary parts of ( )
contribute to the attenuation of the optical
field!
Metal Skin Depth

k
( n i )
c
k ( ) 0
n i 1 i 2
1 1 2

1 22
2 2
E ( r , t ) E0 ( r ) e
E (r , t ) E0 (r )e i ( kz t )
i ( zn / c t ) z /
Useful only when the distances

associated with spatial changes
of the field are large compared
to the mean free path l of the
conduction electrons
Skin depth determines the attenuation length of the field in metals!
For the intensity attenuation:
I I 0 e z
2/
Skin depth data

All the lengths are expressed in nanometers and are measured at RT
Element
Na
Al
Cu
Ag
Au
Hg
(2eV)
38
13
30
24
31
255
(3eV)
42
13
30
29
37
141
(4eV)
48
13
29
82
27
115
lBulk
34
16
42
52
42
11*
measured at 77K
The Drude-Sommerfeld (DS) model

of free electrons lossless metals
Physical picture: Treat the metal as a gas of electrons
E t Re E exp it
d 2r
F eE ma m 2
dt
d 2r
m 2 eE
dt
p t er (t )
Dipole moment:
d 2p
m 2 e2E
P Np 0 E
dt
p t Re p exp it
e2 1
p
E
m 2
Drude dielectric function negligible damping
r
p
Np
Ne 2 1
r 1
1
0E
0m 2
2
p
2
Plasma frequency:
Ne 2
p
0m
Optical response of simple Drude metals

p
Dielectric functions
0
-2
Aluminum
-4
-6
0
-2
-4
-6
-8
-8
-10
n
0
-10
n
5
10
Photon energy (eV)
15
p2
Last Page r 1 2
Only conduction es
contribute to: r
r becomes 1 at high
Metal becomes transparent
r becomes 0 at =p
The dielectric function is negative at optical frequencies!

For most metals, the plasma frequency is in the ultraviolet range (5-15eV)
Drude Model
p 13.8 1015 s 1
1.075 1014 s 1
Real and imaginary part of the dielectric constant for gold according to the Drude-Sommerfeld
free electron model. The blue solid line is the real part, the red, dashed line is the imaginary part.
Note the different scales for real and imaginary part.
General Drude model
(with losses)
Optical response of a collection of free electrons

Drude-Sommerfeld model = Lorentz model without springs
collisionless gas of free electrons moving against A fixed background of positive ions
Lorentz model with clipped springs:
p2
1 2
i
Free electron plasma frequency:
p Ne 2 / m 0
' 1 p
2 2
K 0 (0 0)
Density of free electrons

Fermi velocity
''
vF 1
Effective electron mass

Low T: impurity, imperfections
Collision time
RT: electron-phonon scattering
Electron mean free path

Longitudinal (bulk) waves in metals

D 0 ( ) E
at
p ( p ) 0
D 0 0 ( p )ik E ( ) 0
0
0 if k // E, the wave is longitudinal!
Longitudinal electron waves can be excited at the plasma frequency!
p : Natural frequency of oscillation of the free electron sea

At the plasma frequency electrons undergo longitudinal oscillations.
The quantum quasi-particle associated with these oscillations is called a plasmon
Due to their longitudinal nature, volume plasmons do not couple to transverse
electromagnetic waves, and can only be excited by particle impact.
Physical interpretation of plasma frequency

Equilibrium, neutrality
Non equilibrium, applied field E

E
+
+
+
+
- + +- +
+
+
+ - + + ++
- - + +- -
+-
+
+
+
+
+
+ + + - +
+ - +-
Homogeneous electron density N
+-
Non-homogeneous electron density N N

Induced electric field:
e N
E
0
Continuity equation:
2 N
2 N N
u p 0
2
t N
Nt N
Equation of motion:
u
Plasma oscillations
e
E
Collective oscillations of the electron gas
t
m
Plasma frequency
N (cm-3)
Type of
plasma
1024
5.7 x 1016
33 nm
metals
1022
5.7 x 1015
330 nm
metals
1020
5.7 x 1014
3.3 m
Doped
semiconductors
1018
5.7 x 1013
33 m
Doped
semiconductors
1017
1.8 x 1013
105 m
Doped
semiconductors
1016
5.7 x 1012
330 m
Doped
semiconductors
106
5.7 x 107
33 m
Ionosphere
105
1.8 x 107
105 m
Ionosphere
Opaque
Transparent
Aluminum
Plasma frequencies of metals are
in the VIS and UV
3 eV h p 20 eV
p2
' 1 2
p 2
'' 3
( )
Identical to the high frequency limit

of the Lorentz model!
Opaque
Transparent
The resonant medium: Lorentz model

p ex
P Np
Dipole moment
Polarization density
Lorentz model of materials

There is not a single granule of light which is not
the fruit of an oscillating charge A. Lorentz
Luca Dal Negro, ECE Department, Boston University
m, e
K
The Lorentz model

Lorentz model of materials
m, e
K
Most general classical response model
d 2x
dx
m 2 b Kx eEloc
dt
dt
Driving force
Ansatz:
x xc e
General solution: transient + oscillatory
it
Eloc Ec e
it
Complex representation of the real

time-harmonic quantities
(e / m) Ec
xc 2
0 2 i
0 2 K / m
b/m
The proportionality function between the field

and the electron displacement is complex!
Consequences
If 0 the proportionality factor between F and x is complex
i
x Ae (eE / m)
where:
1
2
1/ 2
tan
0 2 2
1
Max(A) occurs at 0
In-phase response
180 out of phase response
FWHM for ( 0 )
Max(A) 1 /
Collection of oscillators
Induced dipole moment of an oscillator is:
p ex
The polarization of a medium containing N oscillators per unit volume is:
p2
P 2
0E
2
0 i
2
Plasma frequency: p
P Np Nex
Particular example of the constitutive

relation: P 0 E
Ne 2
m 0
p2
1 1 2
0 2 i
L
n 0 for 0
0 L n 1 for 0
n
Dielectric function of Lorentz oscillators

p2
1 1 2
0 2 i
P 0 E
' i ''
' 1
p 2 0 2 2
02 2 2 2
2
''
p 2
02 2 2 2
2
L
Longitudinal Waves in Matter

Longitudinal waves:
( L ) 0 E
1
P
0
1
D0
P 0 E
H ( 0 ) 1 k E 0
B0
Pure polarization waves (not EM!)
D 0 ( ) E
at
Klingshirn, Semiconductor optics

Springer Verlag (2004)
p ( p ) 0
D 0 0 ( p )ik E ( ) 0
0
0 if k // E, the wave is longitudinal!
Polarization mechanisms in dielectrics
Debye relaxation: alignment Lattice vibrations

of permanent dipoles along E vibrational oscillators
against
thermal buffeting
Electronic transitions
electronic oscillators
Stop band (Reststrahlbande)

No wave propagation possible
exponentially decaying wave amplitude
n 0 for 0
0 L n 1 for 0
n
In this range matter is optically thinner than vacuum (n<<1) !!
n1
vacuum
n1 n2
medium
cr
n2
sin cr
n1
For:
n2 0 cr 0
ECE Department, Boston University
Total internal reflection

at normal incidence!!
Important remarks
For metals:
P L
T 0 0
Surface polaritons in metals (called surface-plasmon polaritons)
can be excited in the wide range:
0 P
Metals are ideal materials for broadband engineering of surface-polariton waves
Free and bound electrons in metals: Ag

Silver cannot be explained within the simple Drude model, why?
pe 2
pj 2
1 2
2
i e j j 2 i j
Scattering losses/heat
Free electrons
Radiation damping
Bound electrons
Bound charge effect : 4eV plasma frequency for Ag, 2 eV for Cu
Bound (d electrons) and free charges are competing:

shift (decrease) of plasma frequency
extra reflectance peaks
To describe noble metals (Au,Ag, Cu, etc) in the visible,
more general Lorentz-Drude models are needed!
Mixed excitations in a solid: polaritons

P 0 ( ) 1 E
The electric field in matter is always accompanied by polarization waves
( ) 1
Waves traveling in solids are always a mixture of an electromagnetic

wave and a mechanical polarization wave (as long as ( ) deviates from 1)
Light in matter: mixture of photons and quanta of the polarization field.
The mixed state is quantized in polaritons
Classical Polaritons equation
From:
k
( )
ck
( )
2
Optical response
Material response
Dispersion of waves
The fact that the eigenfrequency 0 of some excitations of a solid
depends on k is called spatial dispersion.
The term dispersion relation means the relation E(k) or (k) for all wave-like
excitations. It can be a simple horizontal-line, a linear or parabolic relation, or something
more complicated. Every excitation which has a wave-like character has a dispersion relation.
The detailed shape of (k) depends on the physical nature of the oscillators and the coupling mechanism.
The term spatial dispersion means that the eigenfrequency 0 of one of the
elementary excitations in a solid depends on k
The term spatial dispersion means that the eigenfrequency 0 of one of the
elementary excitations in a solid depends on k
Bulk plasmon: dispersion relation (Drude metal)

n2
The wave equation is given by:

For a propagating wave solution:
2 r c 2 k 2
p2
Dielectric constant: r 1 2
Dispersion relation for

bulk plasmons
Dispersion relation:
2
r E r, t
2
E r, t
c2
t 2
E r , t Re E r , exp ik r it
p2
1 2 2 p2 c 2 k 2
p2 c 2 k 2
ck
L p
No allowed propagating modes
into the metal (imaginary k)
Note1: Solutions lie above light line
Note2: Metals: p 10 eV; Semiconductors p < 0.5 eV (depending on dopant conc.)
Volume (bulk) Plasmons: Drude dispersion
Bulk Polaritons Dispersion

Using the general Lorentz model (or Kramers-Heisenberg) dielectric function
we can write the polariton equation as:
c2k 2
f
b
2
0 2 2 i
Implicit representation of (k ) for polaritons.
Simple example:
uncoupled oscillators
at vanishing damping
UPB
LPB
Gap
Phonon/Exciton-like
Photon-like
Re k

Plasmonics and Waveguides: Engineering Plasmon-Polaritons in Metallic Nanostructures

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Plasmonics and Waveguides

Engineering plasmon-polaritons in metallic nanostructures

Electron density oscillations coupled to EM waves

Walsh et al., Nano Lett., 13 (2011)

Example: Surface modes of small particles

Localized Surface Plasmons

Quadrupole plasmon resonance

Imaging / optical detection

Half of the electron clouds moves parallel

Radiation engineering with plasmonic coupled

34,000 antennas, Siberia's Kamchatka Peninsula

Photonic-plasmonic coupling regimes in arrays

Transverse field 1/r

Diffractive Coupling between Clusters

Using evanescent (non-propagative) fields the

Principles of Nano-Optics, L. Novotny, .B. Hecht, Cambridge (2006)

Theory of Optical Constants

polished aluminum cooking pan is shiny but opaque transmitted light ?

Models are needed to explain the (linear) optical

Copyright 2008, Boston University

Optics of conducting media

For monochromatic waves:

Where we defined the: Effective electric permittivity:

Bound charge current density

Complex phenomenological coefficients of a medium are equivalent to a phase

Complex refractive index

complex dielectric function

Where we can define:

we can obtain the dispersion relation:

Complex refractive index

Snells law refractive index

(n, ) ( ', '')

are connected and describe the

Metal Skin Depth

Useful only when the distances

Skin depth determines the attenuation length of the field in metals!

For the intensity attenuation:

Skin depth data

The Drude-Sommerfeld (DS) model

Drude dielectric function negligible damping

Optical response of simple Drude metals

The dielectric function is negative at optical frequencies!

Copyright 2008, Boston University

General Drude model

Optical response of a collection of free electrons

Lorentz model with clipped springs:

Free electron plasma frequency:

Density of free electrons

Effective electron mass

RT: electron-phonon scattering

Electron mean free path

Longitudinal (bulk) waves in metals

0 if k // E, the wave is longitudinal!

Longitudinal electron waves can be excited at the plasma frequency!

p : Natural frequency of oscillation of the free electron sea

Physical interpretation of plasma frequency

Non equilibrium, applied field E

Homogeneous electron density N

Non-homogeneous electron density N N

Copyright 2008, Boston University

Identical to the high frequency limit

Copyright 2008, Boston University

The resonant medium: Lorentz model