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Nonlinear Optics

Lecture 6
Boundary problem for SHG in the
noncentrosymmetric media
( ) ( )
( )
( ) ( )
1
(1)
(1)
1
1
(1)
(1)
1
, . ;
2
1
, .
2
1
, .
2
i
i i T
i R
i i t
i i
i i t
T T
i i t
R R i
t e c c
t e c c
t e c c
e
e e
e e
e
e
÷
÷
÷
= +
= +
= +
k r
k r
k r
E r A
E r A
E r A
Incident wave generates regular reflected and
transmitted waves at the same frequency
according to Snell’s law and Fresnel formulas
It also generates 2
nd
order polarization,
responsible for SH propagating inside the
medium as well as reflected from the medium
( )
( )
( )
( )
(1) (1)
(1)
( 2)
( 2)
2
1 1
(1) (1) (1)
2 1
2 2
1 1
(2) (2) (2)
1
2 2 2
(1) (2)
1 1
(2) (2) (2)
2
2 ; 2
2 2
16
;
4
2 2
;
s s
T
T
R
T
i i
eff T s T
i
T i
T T T
T T
R i
R R R
P d A e p e k k
c
p e
E A e k
c c
k k
E A e k
c
e c e
e
e c e
te
e c e
±
±
( = ÷ = =
¸ ¸
= + =
( ( ÷
¸ ¸ ¸ ¸
= =
k r k r
k r
k r
k r
Reflected wave is necessary
to satisfy boundary
conditions at the interface.
Here we assume that
nonlinear polarization
generates TE wave (s-
polarization) and neglect
birefringence
Snell’s law for SH
( ) ( ) ( )
(1) (2) (2) (2) (2)
(2) (2)
1 1 1
sin sin sin
sin 2 sin 2 sin
s s T T R R
T s T T R T
k k k u u u
c e u c e u c e u
= =
= =
Usual requirement that the boundary conditions must be obeyed everywhere
along the plane interface result in the condition that components of the wave
number of all SH waves along the interface be equal to each other.
Taking into account that the wave generated by nonlinear polarization with
propagates in the same direction as the linear transmitted wave so that
we obtain the last missing relation to

determine all propagation angles
(1)
2
s T
= k k
( ) ( )
1 1
sin sin
T s R i
c e u c e u =
Equations for the fields
1
2
(0, , 0) , 0,
y
x
y
E
E i
E
c z y
e
c
| | c
= ¬ = ÷
|
c c
\ .
E B Maxwell equations give:
On the incident side of the interface one has only reflected SH, so that
( ) ( )
( 2) ( 2) ( 2) ( 2)
sin sin (2) (2) (2) (2) (2)
1
0 ; ( 0) 2 cos
R R R R
ik x ik x
R R x R R R
E A e B A e
u u
c e u ÷ = ÷ = ÷
On the transmission side of the interface there are two waves propagating at two
different wave numbers so that
( ) ( )
( )
( )
( ) ( )
(1)
( 2) ( 2)
( 2) ( 2)
(1)
2 sin
sin (2) (2)
1 1
sin (2) (2)
1
2 sin
1
1 1
4
( 0)
2
( 0) 2 cos
4 cos
2
s T
T T
T T
s T
ik x
ik x
T T
T T
ik x
x T T T
ik x
T s
T T
p e
E A e
B A e
p e
u
u
u
u
t
c e c e
c e u
t c e u
c e c e
±
±
+ = +
÷
+ =
+
÷
Equation for reflection and
transmission amplitudes
( ) ( )
( ) ( )
( )
( ) ( )
( ) ( )
( ) ( )
( ) ( )
( ) ( )
( ) ( )
(2) (2)
1 1
1
(2) (2) (2) (2)
1 1
1 1
(2)
1 1
(2)
(2) (2)
1 1
1 1
(2)
1 1
(2)
1 1
4
2
4 cos
2 cos 2 cos
2
cos 2 cos
4
2
2 cos 2 cos
2 cos cos
4
2
R T
T T
T s
R R R T T T
T T
T s R R
T
T T
T T R R
T T T
R
T T
p
A A
p
A A
p
A
p
A
t
c e c e
t c e u
c e u c e u
c e c e
c e u c e u
t
c e c e
c e u c e u
c e u c e
t
c e c e
±
±
±
±
= +
÷
÷ = +
÷
+
= ÷
÷
+
÷
=
÷
( ) ( )
(2) (2)
1 1
2 cos 2 cos
s
T T R R
u
c e u c e u +
Reflected wave
( ) ( )
( ) ( )
( ) ( )
( ) ( )
( )
( 2)
(2) (2)
(2)
1 1
(2)
(2) (2)
1 1
1 1
2
1 1
2 cos cos
4
2
2 cos 2 cos
4
1
2 2
R
i
R R
T T T s
R
T T
T T R R
eff
T R
E A e
p
A
p p
c e u c e u
t
c e c e
c e u c e u
t t
c
c e c e
±
± ±
=
÷
= ~
÷
+
÷ ~ ÷
+
k r
Transmitted waves
( ) ( )
( ) ( )
( ) ( )
( ) ( )
( ) ( )
( ) ( )
( )
(1) ( 2)
(1)
(2)
1 1 2 (2)
(2) (2)
1 1
1 1
(2)
1 1 2
(2) (2)
1 1
1 1
1 (2)
cos 2 cos
4
2
2 cos 2 cos
cos 2 cos
4
1
2
2 cos 2 cos
4 /
T T
T
T s R R i i
T
T T
T T R R
T s R R i i kz
T T
T T R R
R
p
E e e
p
e e
p c
A
c e u c e u
t
c e c e
c e u c e u
c e u c e u
t
c e c e
c e u c e u
t e
±
A
±
±
(
+
( = ÷ =
÷
( +
¸ ¸
(
+
( ÷ =
÷
( +
¸ ¸
+
k r k r
k r
( )
( ) ( )
( ) ( )
( )
( )
( )
(2)
1 1
(2) (2)
1 1 1
1 (2)
1
cos 2 cos
cos
1
2 cos 2 cos
4 /
1 4
i kz
T s R R
s
T T T R R
R T
eff
T
e
k
p c
p
A iz ik z
c e u c e u
u
c e c e u c e u
t e
t
c
c e
A
±
±
+
÷
~
A
+
+ = ÷ ÷
( )
( ) ( )
( )
(2) (1) (2) (2) (1)
(2) 1
1 1
2 cos 2 cos
2 2 cos cos
T T z T T T s
z T T T s
k k k
c
u u
e
c e u c e u
A = ÷ = ÷ =
÷
k k e
e
Third order nonlinearities
( ) ( )
(3) (3)
4 4 1 2 3 1 2 3
{1,2,3}
1
; , , ( , ) ( , ) ( , )
2
i ijkl j k l
P E E E e _ e e e e e e e =
¿
r r r
General form of the 3
rd
order nonlinear polarization:
Optical Kerr effect 4 1 2 2
e e e e = + ÷
( ) ( )
(3) (3)
1
3 3 ; , , ( , ) ( , ) ( , )
2
i ijkl j k l
jkl
P E E E e _ e e e e e e e =
¿
r r r
3
rd
harmonic generation
4
e e e e = + +
( ) ( )
(3) (3)
1 1 1 2 2 1 2 2
3 ; , , ( , ) ( , ) ( , )
i ijkl j k l
jkl
P E E E e _ e e e e e e e = ÷ ÷
¿
r r r
Intensity dependent refractive index e e e e = ÷ +
( ) ( )
(3) (3)
1
3
; , , ( , ) ( , ) ( , )
2
i ijkl j k l
jkl
P E E E e _ e e e e e e e = ÷ ÷
¿
r r r
Effective dielectric constant
( )
( )
( ) ( )
( ) ( ) ( )
2
2
1 1 2 ( )
1
1, 1, 1,
2 2
2
2 ( )
1
1, 1 1,
2
4
0
NL
i i i
NL
i ij ij j
j
E E P
c c
E E
c
e c e
te
e e e
e
e c e o c e
V + = ÷
( V + + =
¸ ¸
¿
r r r
r r
In the case of optical Stark effect and intensity dependent refractive index, the
nonlinear polarization can be presented as a filed-dependent dielectric constant
For Kerr effect, the dielectric constant is modulated by a strong pump field at frequency
ω
2
, while the weak probe wave propagates at the frequency ω
1.

( )
( ) (3)
1 1 2 2 2 2
12 ; , , ( , ) ( , )
NL
ij ijkl k l
kl
E E c t _ e e e e e e = ÷ ÷
¿
r r
In the case of the field modulated refractive index, we deal with the self-modulation of
the index by the wave propagating at the frequency ω.
( )
( ) (3)
6 ; , , ( , ) ( , )
NL
ij ijkl k l
kl
E E c t _ e e e e e e = ÷ ÷
¿
r r
Effective refractive index
Assume that the light in linearly polarized, and let’s choose one of the coordinate axes
(x) along the polarization direction. Also assume that the sample has cubic symmetry,
so that its optically isotropic and Then we can introduce intensity-
dependent effective refractive index
ij ij
c co =
( )
2
(3)
0
(3)
2
0
0
6 ; , , ( , )
3
( , )
ij iixx x ij
x
E
n n E
n
c c t_ e e e e e o
t_
c e
(
= + ÷
¸ ¸
= ~ +
r
r
In the literature, intensity dependent refractive index is often written down as
0 2
n n n I = +
Taking into account that we find
2
0
8
n c
I E
t
=
2
(3)
2
2
0
24
n
n c
t
_ =
Typical values of the nonlinear refractive index coefficient are given in Table 4.1.1
of Boyd’s. They can range between for electronic nonlinearities and

for thermal effects
2
16
10
cm
W
÷
2
6
10
cm
W
÷
Third order susceptibility in isotropic
materials
In the most general case, when all frequencies are different and there are no additional
permutation symmetries, the isotropy condition requires any tensor of the 4
th
rank to have
the form of


With three independent coefficients.
3
rd
harmonic generation: all frequency are the same so, all permutation of indexes are
equivalent, hence


Nonlinear refractive index: first two frequencies are the same, thus


Polarization in the later case becomes
(3) (3) (3) (3)
1122 1212 1221 ijkl ij kl ik jl il jk
_ _ o o _ o o _ o o = + +
( )( )
(3) (3)
1122
3
ijkl ij kl ik jl il jk
_ _ e o o o o o o = + +
( ) ( )
(3) (3) (3)
1122 1221 ijkl ij kl ik jl il jk
_ e e e e _ o o o o _ o o = + ÷ = + +
( )
2 2
(3) (3) (3) * 2 (3) (3) (3) * 2
1 1122 1221 1122 1221
3 3
2 ; 3
2 2
i i i
P E E e _ _ _ _
(
= + = +
¸ ¸
E E P E E E E
Alternative notation for the 3
rd
order
susceptibility
( )
2 2
(3) (3) (3) * 2 (3) (3) (3) * 2
1 1122 1221 1122 1221
(3) (3)
1122 1221
2
(3) * 2
3 3
2 ; 3
2 2
3 ; 3
1
2
i i i
P E E
A B
A B
e _ _ _ _
_ _
(
= + = +
¸ ¸
= =
= +
E E P E E E E
P E E E E
( )
( ) ( )
( )
( ) ( ) (3)
2
(3) (3) * (3) *
1122 1122 1221
2
(3) (3) (3) * *
1122 1221 1221
2
* *
(3)
1122 1221
3
; ; , , ( , ) ( , )
2
3 3 3
2 2 2
3 3
2
2 2
1
2
3
2
2
eff eff
i ij j ij ijkl k l
kl
ij i j i j
ij i j i j
ij i j i j
P E E E
E E E E
E E E E
A B E E E E
A
_ _ _ e e e e e e
_ o _ _
_ _ o _
o
_ _
= = ÷ ÷ =
+ + =
÷ + + =
' ' + +
' = ÷
¿ ¿
r r
E
E
E
( )
(3) (3)
1221
; 3 B _ ' =
/ 6 / 3 molecular orientation
/ 1 / 2 noneresonant electrons
/ 0 / 0 electrostriction
B A B A
B A B A
B A B A
' ' = = ÷
' ' = =
' ' = =
Basis of circularly polarized light
Circularly polarized light is described by combination of two beams polarized in utually
perpendicular directions with a phase shift between them equal to π/2
Left-hand circular (counterclockwise) Right-hand (clockwise)
;
2 2
i i
E E
o o
o o
+ ÷
+ + ÷ ÷
+ ÷
= =
= +
x y x y
E
Non-linear polarization in the circular basis
2
(3) * 2
2 2
2 * 2 *
1
2
1 1
;
2 2
A B P P
P A E B E P A E B E
o o
+ + ÷ ÷
+ + ÷ ÷ ÷ +
= + = +
= + = +
P E E E E
E E E E
One can rewrite the polarization in the circular basis as
Where the terms quadratic in the field are given by
2 2
* 2
; 2 E E E E
+ ÷ + ÷
· = + = E E E
Thus, circular components of the polarization become
( ) ( )
( )
2 2 2 2
( )
2
2
( )
;
NL
NL
P A E A B E E P A E A B E E
P E
A E A B E
_
_
+ + ÷ + ÷ ÷ + ÷
± ± ±
± ±
( (
= + + = + +
¸ ¸ ¸ ¸
=
= + +
Wave equation in the circular basis
( )
( )
( )
2 2 2 ( )
2
1
2 2 2
2 2 2 2
2
1
2 2 2 2
2 2 2 ( )
2
1
2 2 2 2
2 2
2
2
2 2 2 2
1 1
2 2
2 2
1
4
4
4
; 4 4
2
NL
NL
NL
n E P
E
n
c t c t
c t c t
n E P
E
c t c t
n E
E n n n A E A B E
c t
n n B E E
n
t
t
t
t_ t
t
+ +
+
÷ ÷
÷
± ±
± ± ± ±
+ ÷ ÷ +
c c
V = +
c c
c c
V = + ¬
c c
c c
V = +
c c
c
V = = + = + + +
c
÷ ÷
E P
E
If the absence of damping, the wave equation has a solution in which amplitudes of
different polarization components are constants. In this case, the solutions are regular
plane waves, but with intensity dependent refractive indexes
Polarization rotation in the medium with
intensity dependent refractive index
( ) ( )
/ /
/
( )
1 1
; ; /
2 2
cos sin
ˆ ˆ
;
cos sin
2
in z c in z c
in z c i i
i
E z E E A e A e
e A e A e n n n n z c
x x y
i
e
y y x
e e
e u u
u
o o o o
o o u e
u u
o
u u
+ ÷
+ + ÷ ÷ + + ÷ ÷
÷
+ + ÷ ÷ + ÷
±
±
= + = + =
+ = + = A
'
= ÷ ' '
±
=
'
= +
x y