Plasmons, Polaritons, Polarons, and Excitons

Chapter 14 in Kittell: Be careful he uses CGS

To map onto SI replace 4 with 1/0
We will discuss (,K)--energy and wavelength
dependent
(,0)---describes collective excitation: Plasmons, etc.
(,K)---describes electrostatic screening, e-e, e-P, eD-displacement
impurity
D = E + 4P = E E-field
P-polarization

D = E = 4 ext
E = 4 = 4( ext + ind )
Phys. 555/342: Ch 14A

Dielectric Function for Electron Gas

Plasma Optics
(,k) (,o) ( )

with

d2x
m 2 = eE
dt

mx = eE
2

x e it
E e it
eE
x= 2
m

ex = e E / m
2
ne
P = nex = 2 E
m

Dipole moment

Phys. 555/342: Ch 14A

Dielectric Function for Electron Gas

Plasma Optics
ne 2
P = nex = 2 E
m

D( )
P( )
( ) =
1+ 4
E( )
E( )

4ne 2
( ) = 1+
m 2
Plasma Frequency
2
4ne
2p =
m

2p
( ) = 1+ 2

=p when =0
Phys. 555/342: Ch 14A

Dielectric Function for Electron Gas

Plasma Optics
But the positive background also has a dielectric constant
labeled fi()
2

4ne
p
( ) = ()
=

()
1+

2
2
m

2

4ne
=
m()
2
p

Again---

p =
=0
Phys. 555/342: Ch 14A

Dielectric Function for Electron Gas

Dispersion
EM wave equation

2D 2 2
=c E
2
t

But E e i(K rt ) and D = (,K)E

2
2 2
(,K) = c K
real and >0: For real, K is real and a transverse EM wave propagates with
phase velocity c/1/2
real and <0: For real, K is imaginary and the wave is damped with a
characteristic length 1/|K|
is complex: For real, K is complex and the waves are damped in space.
is infinity: This means the system has a finite response in the absence of an
applied force; thus the poles of (,K) define the frequesncies of the free
oscillations of the medium.
=0: We shall see that longitudinally polarized waves are possible only at the
zeros.
Phys. 555/342: Ch 14A

Transverse Optical Modes in a Plasma

(,K) = c K
2

For < p
For > p

( ) 2 = ()( 2 2p ) = c 2K 2

K2 <0 so K is imaginary
K2 >0 so K is real

E e|K |x

2 = 2p + c 2K 2 /()

This describes a transverse

electromagnetic wave in a
plasma.

Phys. 555/342: Ch 14A

Plasmons

Phys. 555/342: Ch 14A

Transparency of Alkalki Metals in the Ultraviolet

Metal should reflect below the plasma frequency
Metals should transmit above the plasma frequency

The Reflectance of Indium Antimonide with

n=4x1018 cm-1

Phys. 555/342: Ch 14A

Longitudinal Plasma Oscillations

Zeros of dielectric function determine the frequency of
the longitudinal modes of oscillation.

( L ) = 0
2
p
( L ) = 1 2 = 0

There is a free longitudinal oscillation

mode (fig) of an electron gas at the
plasma frequency. This is the low
frequency cut off of the transfer mode

Phys. 555/342: Ch 14A

Longitudinal Plasma Oscillations

The figure shows a longitudinal
plasmon in a thin film with K=0.
The electron gas is displaced by
u.

Electron charge

Positive background

There is an electric field

E=4neu: surface charge -neu

d 2u
nm 2 = eE = 4n 2e 2 u
dt

d 2u
2
+

pu
2
dt

Shift with applied field

2
4ne
2p =
m

For small k we can use previous Eqn.

2 2
F
2
p

3k v
(1+
+ )
10

Surface charge

Phys. 555/342: Ch 14A

Plasma Oscillations
A plasma oscillation is a collective longitudinal excitation of the
conduction electrons. A plasmon is a quantum of plasma
oscillations.

Phys. 555/342: Ch 14A

The Prediction of a Surface Plasmon

Rufus Ritchie

QuickTime and a
TIFF (LZW) decompressor
are needed to see this picture.

Phys. 555/342: Ch 14A

History
Ritchie and Birkhoff had submitted separate abstracts
to a conference at the University of Maryland, but
Rufus could not attend --.Birkhoff offered to present
his paper, which met with some fierce criticism from
Dr. Dennis Gabor (later a Nobel laureate), who said
he had studies the problem and concluded that there
was no such animal as the surface plasmon. Upon
learning of this response, Rufus questioned what he
should do. Colleague David Pines encouraged him
to submit the paper anyway.
It is now one of the most cited papers.

Phys. 555/342: Ch 14A

Ritchies 70th Birthday

The impact of the concept of a surface plasmon: Nuc.
Inst. & Methods B96,448 (1995)

Paper referenced 435

times by 1985 in 1995
it had been referenced
620 times.

Phys. 555/342: Ch 14A

Plasmons

Phys. 555/342: Ch 14A

Surface Plasmons
EM surface waves that exists
at the interface of two media
whose have opposite signs

Plasmons in the bulk: p determined

by the free e- density and mass
Plasmons confined to surfaces: interact with light to
form propagating surface plasmon polaritons (SPP)

Plasmons can be confined in nanoparticles:

resonant SP modes that are localized

Phys. 555/342: Ch 14A

Surface Plasmons

EM surface waves that exists at the interface of two media

whose have opposite signs

Fluctuations of the charge on the metal boundary give rise to

Phys. 555/342: Ch 14A
the SP mode

Surface Plasmons
Dispersion relation and Drude

Surface plasmons

k = ( )
2

2
c2

p2
( ) = 1 2

m ( )d
2
k|| = 2
c m ( ) + d

&

k|| > 0

Can exist only at m < 0

Phys. 555/342: Ch 14A

Surface Plasmons- early uses

When illuminated from
within, the Lycurgus cup
glows red due to
embedded gold
nanoparticles which have
an absorption peak
around 520 nm
Colors in stained glass is
due to metallic
nanoparticles with
different indices and
aspect ratios
Phys. 555/342: Ch 14A

Phys. 555/342: Ch 14A

Phys. 555/342: Ch 14A

Phys. 555/342: Ch 14A

Phys. 555/342: Ch 14A

Photon STM Image of a Chain of

Au nanoparticles [from Krenn et
al, PRL 82, 2590 (1999)]

Individual particles: 100x100x40 nm, separated by 100

nm and deposited on an ITO substrate. Sphere at end
of waveguide is excited using the tip of near-field
scanning optical microscope (NSOM), and wave is
detected using fluorescent nanospheres.
Phys. 555/342: Ch 14A

Kittell Problem 10.1

Phys. 555/342: Ch 14A

Solution 10.1

= kA sin kx e kz , and at the boundary this is equal to Exi. The normal

x
component of D at the boundary, but outside the medium, is ( )kA cos kx, where for a
plasma ( ) = 1 p2/ 2. The boundary condition is kA cos kx = ( )kA cos kx, or
( ) = 1, or p2 = 2 2. This frequency = p 2 is that of a surface plasmon.
1. E x0 =

Phys. 555/342: Ch 14A

Kittell: Problem 10,2

Phys. 555/342: Ch 14A

Kittell, solution 10.2

2. A solution below the interface is of the form () = A cos kx e kz , and above the
interface (+ ) = A cos kx e kz , just as for Prob. (1). The condition that the normal
component of D be continuous across the interface reduces to 1( ) = 2( ), or
1

2p1
2

= 1 +

2p2
2

, so that 2 =

1 2
2
(p1 + p2
).
2

Phys. 555/342: Ch 14A

Kittell, Problem 10.5

Phys. 555/342: Ch 14A

Kittell, solution 10.5

5. md 2r/dt 2 = m2r = eE = 4eP/3 = 4ne 2r/3 . Thus 2 = 4ne 2 3m.

Phys. 555/342: Ch 14A

Quantum treatment of Surface Plasmons

Quantum Calculation
of the induced charge
near a surface as a
result of applying a
constant electric field.

Analog of
classical Surface Charge
Friedel Oscillations: 2kF

4
3
[rsa0 ] = 1/n
3
a0 is Bohr Radii

Phys. 555/342: Ch 14A

A view Equations
4ne 2 1/ 2
P =

n(z,w) induced ch arge

( ) =

( ) induced Total ch arge

( ) 1 E( )
dzn(z, ) =

( ) + 1 2

In Jellium Model

P2
( ) = 1 2

Phys. 555/342: Ch 14A

Physical properties of the simple metals and of Ag calculated from

the free electron model: SP is surface plasmon energy

When there is a difference between theory and Exp.

It means the band structure is important.
Phys. 555/342: Ch 14A

A calculation for finite

Fundimentally different
from the static case.
The magnitude of
oscillations much
larger and the
wavelength is much
longer. The surface
charge peak is not
well defined.
The system is not
responding
adiabatically to the
applied field at these
frequencies.
These long wavelength
oscillations have been
seen experimentally
Phys. 555/342: Ch 14A

A comparison

Phys. 555/342: Ch 14A

Work by Feibelman in
the 1970s showed that
the response of the
surface could be
characterized by the
d() function.

d( ) =

dz z n(z, )
( )

First moment of
induced charge.
Red() develops pole
at ~0.8P
No features at SP
Imd() gives photo
absortion.
Phys. 555/342: Ch 14A

Surface Photoelectric Effect

Phys. 555/342: Ch 14A

New term in excitation matrix

d
|< f | 2 A P i A | i >|2 { (E f E i )}
d

Spatial variation in A

Phys. 555/342: Ch 14A

Variation in A

Phys. 555/342: Ch 14A

A few more Equations from a paper by

Persson and Zaremba
The surface response function g(q,)

g(q, ) =

qz
dz

e
n(z, )

g(q,) determins the amplitude of the reflected component of the

electrostatic potential interacting with the surface. Q is the absolute value
of the parallel componendt of the momentum q||. In the small q limit, we
have.

2( )
( ) 1
g(q, ) =
wd( )
1+
( ) + 1 ( ) + 1

Substitute in Drude dielectric

(q) = SP (1 d( SP )q /2)

Phys. 555/342: Ch 14A

How do you measure dispersion

Phys. 555/342: Ch 14A

Instrument

Phys. 555/342: Ch 14A

Data

Surface plasmon

Phys. 555/342: Ch 14A

Phys. 555/342: Ch 14A

New mode: Multiple Plasmon

Phys. 555/342: Ch 14A

Comparison Exp. Vs. Theory

Phys. 555/342: Ch 14A

MM Energy vs. electron density

Phys. 555/342: Ch 14A