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Excitons and Optical Absorption
Excitons and Optical Absorption
+
=
Where and are the destruction and creation operators for conduction
band states, and and are the destruction and creation operators for
the valence band states
k
c
+
k
c
k
b
+
k
b
= + = =
r
g v c
m
k
E k E k E E E
2
2 2
initial final
k
2
ECE 407 Spring 2009 Farhan Rana Cornell University
Optical Transition Rate
The transition rate (per unit volume per second) is given by the Fermis golden rule:
( ) e o
t
=
| | initial final
2
initial final
states
final ll
1 2
E E V
V
R
A
The perturbation due to the radiation field is approximately (neglecting the
photon wavevector in comparison to the electron wavevector) :
= =
+
+
+
|
k
k k
vc
o
k
k k
cv
o
c b n P
m
A e
V b c n P
m
A e
V
n P
m
A e
b c n P
m
A e
c b
b c n P
m
A e
c b V
cv
o
k k
cv
o
k k
k
k k
cv
o
k k
.
2
0 .
2
0
0 .
2
0
'
' '
final final
=
=
=
+ +
+ +
|
The optical matrix element is then:
( ) ( ) ( ) e o
t
|
.
|
\
|
=
|
k E k E
V
n P
m
A e
R
v c
k
cv
o
2
.
2
2
2
2
Also added a
factor of 2 for
the spin
ECE 407 Spring 2009 Farhan Rana Cornell University
Two-Band Model for Interacting Electrons
e
The Hamiltonian is now assumed to include coulomb interaction between electrons:
( ) ( ) ( )
( ) ( ) + +
+ + =
+
+
+
+
+
+
+
+
+
+ +
q k k
k k q k q k
q k k
k k q k q k
q k k
k k q k q k k k
k
v
k k
k
c
b b b b q V
V
c c c c q V
V
c b b c q V
V
b b k E c c k E H
, ' ,
' '
, ' ,
' '
, ' ,
' '
2
1
2
1
1
( ) = =
2
2
q
e
q V
s
c
+
+
+ +
q k k
k k q k q k k k
k
v
k k
k
c
c b b c q V
V
b b k E c c k E H
, ' ,
' '
1
3
ECE 407 Spring 2009 Farhan Rana Cornell University
e
Problem:
In the presence of coulomb interaction between electrons,
the assumed final state:
is not an eigenstate of the Hamiltonian:
0
final
k
k
b c
+
=
final final final
E H =
( ) ( ) ( ) + + =
+
+
+
+ +
q k k
k k q k q k k k
k
v
k k
k
c
c b b c q V
V
b b k E c c k E H
, ' ,
' '
1
+ =
+
+
+
q
q k q k
v c
b c q V
V
k E k E E H
So what do we do??
Two-Band Model for Interacting Electrons
ECE 407 Spring 2009 Farhan Rana Cornell University
e
( ) ( ) ( ) + + =
+
+
+
+ +
q k k
k k q k q k k k
k
v
k k
k
c
c b b c q V
V
b b k E c c k E H
, ' ,
' '
1
( ) =
+
k
k k
b c k A
V
0
1
final
,
initial final
0
1
0
Lets see if this could be an eigenstate:
If we want the above to equal:
( ) = =
+
k
k k
b c k A
V
E E H
0
1
final initial
1
( ) 1
1
1
2
final final
= =
k
k A
V
Superposition
4
ECE 407 Spring 2009 Farhan Rana Cornell University
The Exciton State
( ) ( ) | |
r
g v c
m
k
E k E k E
2
2 2
+ =
Note that:
The easiest way to solve the above equation is to inverse Fourier transform it:
( ) ( ) ( ) ( ) r A E E E r A r V
m
g r
r
=
(
V
initial final
2
2
2
( )
r
e
r V
s
tc 4
2
=
The above equation looks like the Schrodinger equation of a hydrogen atom (in
relative coordinates) with an attractive coulomb potential. The bound solutions are
hydrogenic wavefunctions and the corresponding energies are:
{ ..... 3 , 2 , 1
2
initial final
= + = n
n
E
E E E
o
g
2
2
2
4
2
|
|
.
|
\
|
=
s
r
o
e m
E
tc
r
s
o
m
e
a
2
2
4
|
.
|
\
|
=
tc
o g
E E E E + =
initial final
( ) ( ) ( ) | | ( ) ( ) ( ) = +
q
v c
k A E q V q k A
V
k E k E E k A
final initial
1
ECE 407 Spring 2009 Farhan Rana Cornell University
The Exciton State
The final state:
( ) =
+
k
k k
b c k A
V
0
1
final
h
r
( ) ( )
( ) ( ) = =
= =
+
+
+
+
k
k
r k i
v
k
k
r k i
v
k
k
r k i
c
k
k
r k i
c
b
V
e
r b
V
e
r
c
V
e
r c
V
e
r
. .
. .
5
ECE 407 Spring 2009 Farhan Rana Cornell University
The Exciton State
The probability with which we can destroy and electron in the conduction band at
location and create an electron in the valence band at location is given by
the expression:
e
r
h
r
( ) ( )
( )
V
r r A
r r
e h
e c h v
2
2
final
0
=
+
The above result shows that the conduction band electron and the valence band hole
in real space are localized near each other and their relative positions are described by
the wavefunction ( ) r A
( ) =
+
k
k k
b c k A
V
0
1
final
Interaction
Superposition
In real space
(semi-classical picture)
Electron (-)
Hole (+)
In k-space
ECE 407 Spring 2009 Farhan Rana Cornell University
Optical Transition Rate for the Exciton States
The transition rate (per unit volume per second) is given by the Fermis golden rule:
( ) e o
t
=
| | initial final
2
initial final
states
final ll
1 2
E E V
V
R
A
Where as before:
= =
+
+
+
|
k
k k
vc
o
k
k k
cv
o
c b n P
m
A e
V b c n P
m
A e
V
( )
( )
( ) =
=
=
+ +
+ +
|
k
cv
o
k k
cv
o
k k
k
k
k k
cv
o
k
k k
k A
V
n P
m
A e
b c n P
m
A e
c b k A
V
b c n P
m
A e
c b k A
V
V
*
*
'
' '
*
final final
1
.
2
0 .
2
0
1
0 .
2
'
1
0
The optical matrix element is then:
6
ECE 407 Spring 2009 Farhan Rana Cornell University
Optical Transition Rate for the Exciton States
( ) =
|
k
cv
o
k A
V
n P
m
A e
V
*
final final
1
.
The optical matrix element is:
We get:
( ) ( )
( )
2
2
2
2
final final
* *
final final
0 .
0 .
2
1
.
A V n P
m
A e
V
r A V n P
m
A e
k A
V
n P
m
A e
V
cv
o
cv
o
k
cv
o
|
.
|
\
|
=
= = =
|
|
( )
|
.
|
\
|
|
.
|
\
|
=
=
=
|
e o
t
2
2
, ,
1
0 1
2
2
0 2 .
2
2
n
E
E A n P
m
A e
R
o
g m n
m
n
n
cv
o
{ ..... 3 , 2 , 1
2
initial final
= + = n
n
E
E E E
o
g
All final exciton states can be labeled by the hydrogen atom indices n, , m :
( ) =
+
k
k k
m n
b c k A
V
0
1
, , final
\
|
|
.
|
\
|
=
=
=
|
e o
t
2
2
, ,
1
0 1
2
2
0 2 .
2
2
n
E
E A n P
m
A e
R
o
g m n
m
n
n
cv
o
The transition rate (per unit volume per second) is:
In the hydrogen atom, only the s-orbitals have non-zero probability at the center
Therefore:
( )
|
.
|
\
|
|
.
|
\
|
=
=
|
e o
t
2
2
0 , 0 ,
1
2
2
0 2 .
2
2
n
E
E A n P
m
A e
R
o
g n
n
cv
o
The delta function is usually replaced by a Lorentzian whose width is related to the
exciton (bound electron-hole pair) lifetime:
( )
2
2
2
2
0 , 0 ,
1
2
2
0 2 .
2
2
I + |
.
|
\
|
I
|
.
|
\
|
=
=
|
e
t t
n
E
E
A n P
m
A e
R
o
g
n
n
cv
o
The exciton absorption spectrum consists of sharp lines below the bandgap energy
7
ECE 407 Spring 2009 Farhan Rana Cornell University
e
( ) e
|
R
g
E
Complete Optical Absorption Spectrum
( ) ( ) ( ) ( ) e o
t
e
|
.
|
\
|
=
|
k E k E
V
n P
m
A e
R
v c
k
cv
o
2
.
2
2
2
2
( ) ( )
2
2
2
2
0 , 0 ,
1
2
2
0 2 .
2
2
I + |
.
|
\
|
I
|
.
|
\
|
=
=
|
e
t t
e
n
E
E
A n P
m
A e
R
o
g
n
n
cv
o
Exciton lines
n=1
n=2
n=3
n=4
This part can be also obtained by
considering the non-bound
solutions of the attractive Coulomb
potential
ECE 407 Spring 2009 Farhan Rana Cornell University
Moving Excitons
( ) =
+
k
k k
b c k A
V
0
1
The state:
describes a stationary exciton (with no momentum)
We can construct a state with a non-zero momentum as well
Consider the state:
In k-space
(Superposition)
( ) =
+
+
+
k
Q k Q k
b c Q Q k A
V
0 , ,
1
2 1
2 1
( ) ( ) ( ) | |
( ) ( )
+ + + =
+
+
+
+
+
+
q k
Q k Q k
k
Q k Q k
v c
b c q V q k A
V
b c Q k E Q k E E Q Q k A H
,
2 1 initial 2 1
0
1
0 , ,
2 1
2 1
=
+ + +
8
ECE 407 Spring 2009 Farhan Rana Cornell University
Moving Exciton States
( ) ( )
h e h e r
g v c
m
Q
m
Q
m
Q k
m
Q k
m
k
E Q k E Q k E
2 2
. .
2
2
2
2 2
1
2
2
2
1
2 2 2
2 1
+ + + + + = + +
Note that:
The equation to be solved is:
( ) ( ) ( ) | |
( ) ( ) ( )
2 1 final
,
2 1
2 1 initial 2 1
, , , ,
1
, ,
Q Q k A E q V Q Q q k A
V
Q k E Q k E E Q Q k A
q k
v c
=
+ + +
A bound solution is possible only if:
Q
m
m
Q Q
m
m
Q
m
Q k
m
Q k
e
r
h
r
h e
= = = +
2 1
2
2
1
2
0
. .
( ) ( ) =
+
+ k Q
m
m
k Q
m
m
k
e
r
h
r
b c Q k A
V
Q
0 ,
1
( ) ( ) ( )
( )
( ) Q r A
m m
Q
E E Q E Q r A r V
m
h e
g r
r
,
2
,
2
2 2
initial final
2
2
|
|
.
|
\
|
+
=
(
V
Upon inverse Fourier transforming:
ECE 407 Spring 2009 Farhan Rana Cornell University
Moving Exciton States
The equation:
( ) ( ) ( )
( )
( ) Q r A
m m
Q
E E Q E Q r A r V
m
h e
g r
r
,
2
,
2
2 2
initial final
2
2
|
|
.
|
\
|
+
=
(
V
is identical to the previous one except that the solutions now will have an extra
kinetic energy term:
( )
( )
{ ..... 3 , 2 , 1
2
2 2
2
initial final
=
+
+ + = n
m m
Q
n
E
E E Q E
h e
o
g
The extra term stands for the kinetic energy of the moving exciton which is moving
with a velocity:
( ) ( )
( )
h e
Q
m m
Q
Q E Q v
+
= V =
final exciton
1
The state:
( ) ( ) =
+
+ k Q
m
m
k Q
m
m
k
e
r
h
r
b c Q k A
V
Q
0 ,
1
9
ECE 407 Spring 2009 Farhan Rana Cornell University
Interaction of Moving Excitons with Radiation
The transition rate (per unit volume per second) is given by the Fermis golden rule:
( ) e o
t
=
| | initial final
2
initial final
states
final ll
1 2
E E V
V
R
A
Where as before: = =
+
+
+
|
k
k k
vc
o
k
k k
cv
o
c b n P
m
A e
V b c n P
m
A e
V
( ) ( )
0
0 .
2
, '
1
0
' '
'
*
final final
=
=
+
+
+
|
k
k
k
cv
o
k Q
m
m
k
Q
m
m
k
b c n P
m
A e
c b Q k A
V
V Q
h
r
e
r
The optical matrix element is then:
unless: 0 = Q
= =
+
+
+
+
+
|
k
q k k
vc
o
k
k q k
cv
o
c b n P
m
A e
V b c n P
m
A e
V
( ) 0
final final
=
|
V Q
=
The momentum of the absorbed photon is the momentum of the photogenerated
exciton!
ECE 407 Spring 2009 Farhan Rana Cornell University
The Exciton Gas and BEC
Consider the exciton dispersion relation:
( )
( )
{ ..... 3 , 2 , 1
2
2 2
2
initial
=
+
+ + = n
m m
Q
n
E
E E Q E
h e
o
g
A large exciton population generated by light (or by any other mechanism) quickly
acquires a thermal (Bose-Einstein) distribution with a non-zero Fermi level:
( ) Q E
( )
( ) ( )
1
1
=
KT E Q E
f
e
Q n
0 = Q