C.

Bulutay Lecture 22
Semiconductor Electronic Structure & Optical Processes
Nonlinear Optics [SI Units]
NL susceptibilities
NL susceptibility of a classical anharmonic oscillator
o Noncentrosymmetric Media
o Centrosymmetric Media
2
nd
Order Nonlinearity
Crystal Symmetry
Phase Matching
3
rd
Order Nonlinearity
Two Photon Absorption
Ref: Boyd and mainly Fox
In This Lecture:
C. Bulutay Lecture 22
Semiconductor Electronic Structure & Optical Processes
Nonlinear Susceptibility Tensor
0
0
0


In linear optics:
1
r
r
D E P
E
P E

= +
=
=
= +

Actually the dielectric response of the medium is NL, so in NL optics in addition
to the linear term the resultant polarization contains a series of NL terms
( )
(1) (2) 2 (3) 3
0
0
(1) (2) (3) 2

1
1
NL
NL
NL NL
r
P E E E
E
E E




= + + +
=
= +
= + + + +

Assume an isotropic
medium, so drop the
vector notation
C. Bulutay Lecture 22
Semiconductor Electronic Structure & Optical Processes
( )
Hence, an important aim in NL optics is to determine or a particular order
of such as . Majority of phenomena can be attributed to first three
orders of . Also take into account the effect
NL
NL n

( )
( )
( )
(1) (1)
0
, ,
(2) (2)
0
( )
(3) (3)
0
( )
of xtal anisotropy.
( ) ; ( )
( ) ; , ( ) ( )
( ) ; , , ( ) ( ) ( )
i ij j
j x y z
i n m ijk n m n m j n k m
jk mn
i o n m ijkl o n m o n m j o k n l m
jkl mno
P E
P E E
P E E E



=
=
+ = +
+ + = + +

keep the sum
n
+
m
fixed
while sweeping over n and m
Rank-3 tensor: 3
3
=27 entries however,
most zero or same due to symm.
Rank-4 tensor: 3
4
=81 entries however,
most zero or same due to symm.
C. Bulutay Lecture 22
Semiconductor Electronic Structure & Optical Processes
NL susceptibility of a classical anharmonic oscillator
Noncentrosymmetric Media
We shall consider the Lorentz model of the atom governed by an anharmonic
potential well:
(2)

Ionic potential for a
noncentrosymmetric xtal
U(x)U(-x)
( )
2 2 3
0 0 0 3
2
0 3
2 2
0 0 0 3
2
2
0 0 0 0
2
1 1
( )
2 3
Assuming
Hence the restoring force becomes:
( )
The equation of motion of a bound e under
an AC electric field at frequency :
U x m x m C x
C x
dU
F x m x m C x
dx
d x dx
m m m
dt dt

= +
= = +
+ +
>
2
0 3 0
cos x m C x eE t + =
Damping term
Long wavelength
assumption for EM
C. Bulutay Lecture 22
Semiconductor Electronic Structure & Optical Processes
Due to the existance of the anharmonic term, we express the e displacement as:
( )
( )
( )
2
1 2
1 2 1
0
1
2 2
0
0
(1)
0
2
(1)
2 2
0 0 0
1
( ) . .
2
Assuming weak nonlinearity, , solution for
1
Since, ( , ) ( , )
( ; ) ( )
( ; )
Then solv
i t i t
x t X e X e c c
X X X
e
X
m
i
P t Nex t
E t
Ne
m i

= + +
=
+
=
=
=
(
+

>
(2) (1)
2
2
2 (1) (1)
0 0 3
(2)
2 3
e for via which yields in terms of
( ; ) (2 ; 2 )
(2 ; , )
X
m C
N e



(

=
It is directly proportional to anharmonic term C
3
. This simple model is reasonably
successful in predicting the dispersion in a large number of noncentrosymmetric
xtals.This is due to empirical finding that C
3
does not vary much between materials
C. Bulutay Lecture 22
Semiconductor Electronic Structure & Optical Processes
Centrosymmetric Media
In a centrosymmetric xtal, the ionic binding potential seen by a valence e
can be modelled as:
Ionic potential for a
centrosymmetric xtal
U(x)=U(-x)
harmonic term
So, for centrosymmetric xtals (media having inversion symmetry like the
diamond structure) the most important NL susceptibility is the 3rd-order
since the 2nd-order identically vanishes
(3)

( )
2 2 4
0 0 0 4
2 3
0 0 0 4
(1)
(2)
3
0 0 4
(3)
1 1
( )
2 4
( )
Under the same long wavelength EM wave at :
same as in the previous case
0 due to inversion symmetry of the xtal
(3 ; , , )
U x m x m C x
dU
F x m x m C x
dx
m C

= +
= = +

=
3
(1) (1)
3 4
( ; ) (3 ;3 )
N e
(

anharmonic term
C. Bulutay Lecture 22
Semiconductor Electronic Structure & Optical Processes
2
nd
Order Nonlinearities
If the medium is excited by two sinusoidal waves at
1
and
2
(2) (2)
0 1 1 2 2
(2)
0 1 2 1 2 1 2
( ) cos cos
1
cos ( ) cos ( )
2
sum diff
P t E t E t
E E t t



=
(
(
= + +
(

_ _
Nonlinear frequency mixing
If
1
=
2

sum
=2 Second Harmonic Generation (frequency Doubling)

diff
=0 Optical Rectification
This is the reverse of Pockels effect (linear electro-optic effect):
A DC field changes the optical refractive index
C. Bulutay Lecture 22
Semiconductor Electronic Structure & Optical Processes

1
+
2
-
2

1
-
2
In quantum mechanical terms:
In the sum process two input photons at
1
and
2
are annihilated
and a new photon at
sum
is created
In the difference process, one photon at
1
is annihilated and two
new photons at
2
and
diff
are created.
The creation of the photon at
2
is stimulated by the presence of a
large number of existing photons at this frequency from the input
field. Here,
2
field is also amplified, so-called parametric
amplification
C. Bulutay Lecture 22
Semiconductor Electronic Structure & Optical Processes
A summary of 2
nd
order NL Effects
Ref: Fox
C. Bulutay Lecture 22
Semiconductor Electronic Structure & Optical Processes
Crystal symmetry (2
nd
order NL)
(2)
(2) (2)
: 3-rank tensor with 27 components
Some of them are the same, for instance:

because the response of the medium cannot
depend on the mathematical ordering
ijk
same
xyz y z xzy z y
E E E E

(2)
of the fields
Only 18 physically distinct components of
ijk

So, a contracted tensor, d
ij
, so-called nonlinear optical coefficient
tensor is introduced so that
(2) (2)
11 0 14 0
So, for instance , etc.
xxx xyz
d d = =
C. Bulutay Lecture 22
Semiconductor Electronic Structure & Optical Processes
Crystal symmetry (contd)
On top of these intrinsic permutation symmetries, due to the
constraints from the specific crystal symmetry much of the
components are enforced to be zero
For instance,
For crystals having inversion symmetry (centrosymmetric)
d
ij
=0 for all i,j
For the zinc-blende structure the only non-zero terms are
d
14
=d
25
=d
36
C. Bulutay Lecture 22
Semiconductor Electronic Structure & Optical Processes
Phase Matching
Nonlinear effects are generally small, and we therefore need a long
length of the NL medium to obtain a useful NL conversion
efficiency. For this to work we need that the phases of the NL
waves generated throughout the whole xtal are all the same so that
the fields add together coherently; this regime is called phase
matching.
The phase matching can be given an intuitive physical
interpretation if we notice that if n
2
=n

, then k(2)=2k(). This

corresponds to a momentum conservation in the NL process. In the
more general case when a photon of wavevector k is generated by
mixing two photons with wavevectors k
1
and k
2
, the phase
matching condition can be written as
k=k
1
+k
2

2 c/n(2)
c/n()
phase velocities of the input
and its 2
nd
harmonic
C. Bulutay Lecture 22
Semiconductor Electronic Structure & Optical Processes
A summary of 3
rd
order NL Effects
Ref: Fox
C. Bulutay Lecture 22
Semiconductor Electronic Structure & Optical Processes
Expressions are involved...
Ref: Aversa-Sipe PRB 52 14636 95
Repeated 6 times due to intrinsic permutation symmetry...
C. Bulutay Lecture 22
Semiconductor Electronic Structure & Optical Processes
Example: Two-Photon Absorption
( )
( ) ( ) ( )
( )
( )( )
( ) ( )
( )
{ }
( )
( ) ( )
( )
( ) ( )
2
2
(2)
,
0
, ,
(2)
2 2
(2)
(2) (3)
1/ 2 3/ 2
1 2
2

, , ; 2 ,

, ; ,
2 ,
Im ; , ,
Near the Band edge: , 2
cv ck vk
k c v
ck ik ik vk
cv
i
ik vk
dcba
g g
eA
W e M e k E E
cm
e p e p
M e k
E E
dW W
K
dI I
K I
W E W E

| |
=
|
\ .

=

= =

h
h
, ,
h
h h
h h
over intermediate (virtual) states
2 Photon Absorption coef.
2nd order perturbation theory for 2 photon absorption