Surface Plasmon Polaritons (SPPs)

Introduction and basic properties

- Overview
- Light-matter interaction
- SPP dispersion and properties

Standard textbook:
- Heinz Raether, Surface Plasmons on Smooth and Rough Surfaces and on Gratings
Springer Tracts in Modern Physics, Vol. 111, Springer Berlin 1988
Overview articles on Plasmonics:
- A. Zayats, I. Smolyaninov, Journal of Optics A: Pure and Applied Optics 5, S16 (2003)
- A. Zayats, et. al., Physics Reports 408, 131-414 (2005)
- W.L.Barnes et. al., Nature 424, 825 (2003)

Elementary excitations and polaritons

Elementary excitations:
Phonons (lattice vibrations)
Plasmons (collective electron oscillations)
Excitions (bound state between an excited electron and a hole)
Polaritons:
Commonly called coupled state between an elementary excitation and a photon
= light-matter interaction
Plasmon polariton: coupled state between a plasmon and a photon.
Phonon polariton: coupled state between a phonon and a photon.

Plasmons
free electrons in metal are treated as an electron liquid of high density

n 10 23 cm 3

longitudinal density fluctuations (plasma oscillations) at eigenfrequency p

quanta of volume plasmons have energy

4ne 2
h p = h
m0

, in the order 10eV

Volume plasmon polaritons

propagate through the volume for frequencies

> p

Surface plasmon polaritons

Maxells theory shows that EM surface waves can propagate also along a metallic
surface with a broad spectrum of eigen frequencies
from = 0 up to

= p

Particle (localized) plasmon polaritons

Plasmon resonance positions in vacuum

Bulk
metal

+ + + +

=0
-

Metal
surface

Metal sphere
localized SPPs

++ -- ++ -- ++ --

= 1
drude
model

+
-

+
-

= 2

drude
model

Surface Plasmon Photonics

Optical technology using
- propagating surface plasmon polaritons
- localized plasmon polaritons

Also called:
Plasmonics
Plasmon photonics
Plasmon optics

Topics include:
Localized resonances/
local field enhancement

- nanoscopic particles
- near-field tips

Propagation and guiding

- photonic devices
- near-field probes

Enhanced transmission

- aperture probes
- filters

Negative index of refraction

and metamaterials

- perfect lens

SERS/TERS

- surface/tip enhanced Raman scattering

Molecules and
quantum dots

- enhanced fluoresence

Nanophotonics using plasmonic circuits

Nanoscale plasmon waveguides
Proposal by Takahara et. al. 1997

h
Metal nanowire
Diameter <<

Proposal by Quinten et. al. 1998

h
Chain of metal nanoparticles
Diameter and spacing <<
Atwater et.al., MRS Bulletin 30, No. 5 (2005)

First experimental observation by

Maier et. al. 2003

Subwavelength-scale plasmon waveguides

Krenn, Aussenegg, Physik Journal 1 (2002) Nr. 3

Some applications of plasmon resonant nanoparticles

SNOM probes

Sensors

Surface enhanced
Raman scattering (SERS)

Nanoscopic waveguides for light

S.A. Maier et.al., Nature Materials 2, 229 (2003)

T. Kalkbrenner et.al., J. Microsc. 202, 72 (2001)

Light-matter interactions in solids

EM waves in matter
Lorenz oscillator
Isolators, Phonon polaritons
Metals, Plasmon polaritons

Literature:
- C.F.Bohren, D.R.Huffman, Absorption and scattering of light by small particles
- K.Kopitzki, Einfhrung in die Festkrperphysik
- C.Kittel, Einfhrung in die Festkrperphysik

EM-waves in matter (linear media) - definitions

Polarization

P = 0 E with suszeptibility

Complex refractive index

N = n + i =

Complex dielectric function

Electric displacement

= + i = 1 +

D = 0 E + P = 0 (1 + )E = 0E
Relationship between N and

= n2 + 2
= 2n

EM-waves in matter (linear media) - dispersion

E = E0 e

i( kr t)

wavevector k =

frequency = 2 f

i kr t)

B = B0 e (

Dispersion in transparent media without absorption:

k=

k and are real

c
k
n

>0

Dispersion generally:

(k k) =

2
c

() and thus k = k + ik are complex numbers!

E = E0 ei (kr t ) = E0 ei (k r t )e k r
propagating wave

exponential decay of amplitude

Harmonic oscillator (Lorentz) model

-

0
+

m&x& + bx& + Kx = eE = eE0 eit

x=

em
i eE
=
E
Ae
02 2 i
m

p = ex = 0E
P = Np = 0 E

p2
= 1+ = 1+ 2
0 2 i

02 = K m
=b m
2p = Ne 2 / m 0 plasma frequency

One-oscillator (Lorentz) model

N = n + i =

2
(
n 1) + 2
R=
(n + 1)2 + 2

from Bohren/Huffman

Weak and strong molecular vibrations

weak oscillator: > 1

strong oscillator: < 0

25

25

eps''

eps'

eps'

eps''

1,6

0,8

20

20

1,2

0,6

15

15

0,8

0,4

10

10

0,4

0,2

-0,2

-5

-5

-0,4

-10

0
-0,4
-0,8

860

880

900

920

940

860

880

900

920

940

wavenumber / cm -1

wavenumber / cm -1

caused by: molecular vibrations

crystal lattice vibrations

SiC, Xonotlit, Calcite, Si3N4

examples: PMMA, PS, proteins

-10

Optical properties of polar crystals

note:
lattice has transversal T and longitudinal L
oscillations but only transversal phonons
can be excited by light

N = n + i =

(k k ) =

2
c2

A n = 0, =

B n = , = 0

A k =i

E = E0 ei (kr t )

=0

B k=

2
(
n 1) + 2
R=
(n + 1)2 + 2

A: total reflection
B: transmission and reflection

SiC - single oscillator model

>0

General dispersion for nonconductor

0 = 0
permanent dipoles
e.g. water

resonances
restoring forces

0 > 0
phonons
molecular vibrations

Dispersion in polar crystals - phonon polaritons

Dispersion relation for = 0
2
2

L
k 2 = 2 = 2 ( s ) 2
c
c
T 2

=0
between TO and LO
there is no solution for
real values and k

frequency gap:

E e it e kr
no propagation

reflection

strong coupling of mechanical and

electromagnetic waves, polariton like
photon like

Metals - drude model

- Intraband transitions
- longitudinal plasma oscillations
- 0 = 0 i.e. no restoring force
- P = plasma frequency

p2
= 1+ 2
0 2 i

k =i

=0

E = E0 ei (kr t )

n = 0, =

k=

n = , = 0

0 = 0

= 1

p2
2 i
total reflection

p2
1 2
= 1 2
+ 2

transmission

p2

p2
p2
=

( 2 + 2 ) 3

>> = 1/ (1/ collision time)

collisions usually by electron-phonon scattering
generally:
> 0 leads to damping of transmitted wave n > 0, > 0

Aluminium

T = 0

L = P

Free and bound electrons in metals

Bound electrons contribute like a Lorenz oscillator

metal = drude + bound

bound
where

drude
drude

bound

p2 ,d
= 1 2
i d

p2 , j
= 2
2
j 0 i j

Metals - plasmon polaritons

Plasmon polariton dispersion ( = 0)

2 = p2 + c 2 k 2

= ck
E e it e kr
no propagation

k
reflection

Dielectric function of metals and polar crystals

Metal
collective free electron oscillations (plasmons)
no restoring force

Polar crystal
strong lattice vibrations (phonons)

Reststrahlenband

plasma frequency
(longitudinal oscillation)

transversal optical
phonon frequency, TO

longitudinal optical
phonon frequency, LO

Surface Plasmon Polaritons (SPPs)

Introduction and basic properties
- Overview
- Light-matter interaction
- SPP dispersion and properties

Standard textbook:
- Heinz Raether, Surface Plasmons on Smooth and Rough Surfaces and on Gratings
Springer Tracts in Modern Physics, Vol. 111, Springer Berlin 1988
Overview articles on Plasmonics:
- A. Zayats, I. Smolyaninov, Journal of Optics A: Pure and Applied Optics 5, S16 (2003)
- A. Zayats, et. al., Physics Reports 408, 131-414 (2005)
- W.L.Barnes et. al., Nature 424, 825 (2003)

Surface polaritons (SPs)

Coupled state between photons and elementary excitations at the interface between a
material with < 0 and a dielectric.
- radiative surface polaritons are coupled with propagating EM waves.
- nonradiative surface polaritons do not couple with propagating EM waves.
- for perfectly flat surfaces SPs are always nonradiative!
- mixed transversal and longitudinal EM field.
In contrast to TIR the surface polariton field on both sides of the interface are evanescent.

dielectric

ESP = E0 ei (k x x k z z t )

d ( ) > 0 z

k x = k x + ik x

surface wave

E (z )

++ -- ++ -- ++ --

( ) < 0

E (z ) e

Im k z z

k x =

SP

SP fields
Ez

Ez

Hy

++

Ex

Hy

++ -- ++ -- ++ -++ -- ++ -- ++ -++ -- ++ -- ++ -++ -- ++ -- ++ --

Ex

--

kx

Ex
i (k x x + k z z t )
E = 0 e
E
z

dielectric:
metal/polar crystal:

i ( k xd x + k zd z t )

e
ei (k xm x k zm z t )

0
i (k x x + k z z t )
H = H y e
0

Derivation of SPP dispersion boundary conditions

Ey = 0

Ez

Hy

++

Ex

Hx = Hz = 0
--

z
x

dielectric

d ( )

longitudinal surface wave

z>0
z<0

++ -- ++ -- ++ --

metal

z
x

m ( )

Boundary
bonditions (z=0)

H d = (0, H yd ,0)ei (k xd x + k zd z t )
E d = (E xd ,0, E zd )ei (k xd x + k zd z t )

m E zm = d E zd
E xm = E xd

H m = (0, H ym ,0)ei (k xm x k zm z t )
E m = (E xm ,0, E zm )ei (k xm x k zm z t )

H ym = H yd

k xm = k xd = k x

Derivation of SPP dispersion

1
curl H =
E
c t

Maxwell eq.:

Ex
x 0

1
y H y = t 0
c
0
Ez
z
zH y
Ex

0 = 0
c
H
Ez
x y
Diel.:

Metal:

e
e

i ( k x x + k zd z t )
i ( k x x k zm z t )

x-component:
Metal:

z H ym = + k zm H ym
+ k zm H y = m

Diel.:

Ex

z H yd = k zd H yd
+ k zd H y = + d

Ex

z-component:
Metal:

Diel.:

+ k x H y = m

+ k x H y = d

E zm

E zd

Derivation of SPP dispersion

x-component:
Metal

I:

k zm H y = m

Diel.

II:

k zd H y = d

I / II:

Ex

Ex

m
k zm
=
k zd
d

k zd

k zm

=0

Dispersion relation of SPPs

generally:

k x2 + k y2 + k z2 = k 2

dielectric:

k + k = d

metal:

k +k

2
x

2
zd

c2

at interface metal/dielectric:

k xd = k xm

m d
k x2 =
c m + d

2
x

2
zm

= m

2
c2

2
c2

k zd

k zm

=0

d

k zd2 =
c ( m + d )
2

m

=
c ( m + d )
2

2
zm

Re( m ) < 0 and m > d real k x

kzd and k zm are imaginary

Dispersion relation of SPPs

ESP = E0 ei (k x x k z z t )

m d
k x2 =
c m + d
2

k zd2 =
c ( m + d )
2

2
zm

photon
in air

= ck x

2
d

SP = p

m2

=
c ( m + d )

1
1+ d

d
surface plasmon polariton

m + d
ck x
m d
kx

Re( m ) < 0 and m > d real k x

kzd and k zm are imaginary

Volume vs. surface plasmon polariton

= ck x
photon
in air

2 = p2 + c 2 k x2

plasmon
polariton

volume plasmon
with damping

SP = p

1
1+ d

surface plasmon polariton

m + d
ck x
m d

kx

surface plasmons
non-propagating
collective oscillations
of electron plasma
near the surface

SP dispersion - plasmon vs. phonon

photon
in air

= ck x

+1

photon
in air

LO

1
surface plasmon
polariton

TO

surface phonon
polariton

kx

kx

Plasmon polaritons:

Phonon polaritons:

Light-electron coupling in

metals

semiconductors

Light-phonon coupling in polar crystals

SiC, SiO2

III-V, II-VI-semiconductors

SP propagation length
metal/air
interface

k x = k x + ik x =

m +1

d =1
m = 1
= 0.2

E( x ) = E 0 e

ik x x

= E0e

ik x x k x x

propagating term exponential decay

in x-direction

1
Lx =
2k x
Example silver:

propagation
length
intensity !

= 514.5 nm : Lx = 22 m
= 1060 nm : Lx = 500 m

10
7.5
5
2.5
-2.5
-5
-7.5
-10

p2

Drude
model

+ i
2

m
0.4

0.6

0.8

m
SP =

Lx (vac )

p
2

= 1

200
100
50
20
10
5
2
1
0.2

0.4

0.6

0.8

SPP field perpendicular to surface

dielectric

d ( )

kx

E( z ) = E 0 e
Ez

Im k z z

Lz =

1
Im k z

z-decay length
(skin depth):

metal

m ( )

z
x

Examples:
silver:

= 600 nm : Lz ,m = 390 nm and Lz ,m = 24 nm

gold:

= 600 nm : Lz ,m = 280 nm and Lz ,m = 31 nm

SPPs have transversal and longitudinal el. fields

Ez

Hy

++

Ex

--

x
El. field E z = i

SP

kx
Ex
kz

m
E zd
=i
d
Ex
At large

The mag. field H is

parallel to surface
and perpendicular to
propagation

E zm
d
= i
Ex
m

values,

the el. field in air/diel. has a strong

transvers Ez component compared to the
longitudinal component Ex
In the metal Ez is small against Ex

At large kx, i.e. close to = - d,

both components become equal

E z = iE x

(air: +i, metal: -i)

Dispersion and excitation of SPPs

in a dielectric k of the photon is increased

photon in air

k of photon in dielectric can equal k of SPP

photon in
dielectric
SPP can be excited by p-polarized light
(SPP has longitudinal component)

SPP dispersion

kx

Kretschmann configuration
kx

k of photon in air is always < k of SPP

no excitation of SPP is possible

z
thin metal film
dielectric
E

0
R

Methods of SPP excitation

nprism > nL !!

Excitation by ATR
Kretschmann configuration

d
m
0
E

kx

Otto configuration

m
d
0

z
x

0
R

total reflection at prism/metal interface

-> evanescent field in metal
-> excites surface plasmon polariton at
interface metal/dielectric medium
metal thickness < skin depth

kx

z
x

0
R

total reflection at prism/dielectric medium

-> evanescent field excites surface plasmon
at interface dielectric medium/metal
usful for surfaces that should not be damaged
or for surface phonon polaritons on thick crystals
distance metal prism of about

ATR: Attenuated Total Reflection

Excitation by ATR
SPP excitation requires

kphoton,x = kSP,x

kSP,x

kSP,x

m
0

kphoton,x

z
x

kphoton,x < kSP,x

no SPP excitation

kphoton,x

kphoton,x = kSP,x
SPP excitation

Excitation by Kretschmann configuration

z
x

d
m
0

k=

kx =

k=

0 sin ( 0 )

= c / k x 0 sin ( 0 )

= ck

photon in
dielectric

photon
in air

SPP dispersion

kx =

m +1

k x0

0
k x0

=c

m +1
c
=
m
0 sin ( 0 )

Resonance
condition

kx

Kretschmann configuration angle scan

illumination freq. 0= const.

s-polarized
-> no excitation of SPPs

R
R

p-polarized

photon
in air

0
kx