Introduction to Nonlinear Optics

H. R. Khalesifard
Institute for Advanced Studies in Basic
Sciences
Email: khalesi@iasbs.ac.ir

Contents
1. Introduction
2. The essence of nonlinear optics
3. Second order nonlinear phenomena
4. Third order nonlinear phenomena
5. Nonlinear optical materials
6. Applications of nonlinear optics
Introduction
Question:
Is it possible to change the
color of a monochromatic
light?

Answer:
Not without a laser light
output
N
L
O

s
a
m
p
l
e

input
Stimulated emission, The MASER
and The LASER
(1916) The concept of stimulated emission Albert
Einstein
(1928) Observation of negative absorption or stimulated
emission near to resonant wavelengths, Rudolf
Walther Ladenburg
(1930) There is no need for a physical system to always
be in thermal equilibrium, Artur L. Schawlow
v h
E
1

E
2

Absorption
E
1

E
2

v h
Spontaneous
Emission
E
1

E
2

v h v h v h
Stimulated
Emission
LASER
(MASER)
Light (Microwave) Amplification
by
Stimulated
Emission of Radiation
The Maser
Two groups were working on Maser in 50s

Alexander M. Prokhorov and Nikolai
G. Bassov (Lebedev institute of
Moscow)
Charles H. Townes, James P. Gordon
and Herbert J. Zeiger (Colombia
University)



Left to right: Prokhorov, Townes and Basov at the Lebede
institute (1964 Nobel prize in Physics for developing the
Maser-Laser principle)
Townes (left) and
Gordon (right) and
the ammonia maser
they had built at
Colombia University

The LASER
(1951) V. A. Fabrikant A method for the application of
electromagnetic radiation (ultraviolet, visible, infrared, and radio
waves) patented in Soviet Union.
(1958) Townes and Arthur L. Schawlow, Infrared and Optical
Masers, Physical Review
(1958) Gordon Gould definition of Laser as Light Amplification
by Stimulated Emission of Radiation
(1960) Schawlow and Townes
U. S. Patent No. 2,929,922
(1960) Theodore Maiman Invention of the first Ruby Laser
(1960) Ali Javan The first He-Ne Laser

Maiman
and the
first ruby
laser
Ali Javan and
the first He-Ne
Laser
Properties of Laser Beam
A laser beam
Is intense
Is Coherent
Has a very low divergence
Can be compressed in time up to few
femto second


Applications of Laser
(1960s) A solution looking for a
problem

(Present time) Medicine, Research,
Supermarkets, Entertainment,
Industry, Military, Communication,
Art, Information technology,



Start of Nonlinear Optics
Nonlinear optics started
by the discovery of
Second Harmonic
generation shortly
after demonstration
of the first laser.
(Peter Franken et al
1961)
2. The Essence of Nonlinear Optics
When the intensity
of the incident light
to a material
system increases
the response of
medium is no
longer linear
Input intensity
O
u
t
p
u
t

Response of an optical Medium
The response of an
optical medium to
the incident
electro magnetic
field is the
induced dipole
moments inside
the medium

v h
v h
v h
v h

Nonlinear Susceptibility
The general form of polarization
+ + + + =
l k j
) (
ijkl k j
) (
ijk j
) (
ij i i
E E E E E E P P
3 2 1 0
Dipole moment per unit volume or polarization
j ij i i
E P P _ + =
0
Nonlinear Polarization
Permanent
Polarization
First order
polarization:
Second order
Polarization
Third Order
Polarization

j ij i
E P
) 1 ( 1
_ =
k j ijk i
E E P
) 2 ( 2
_ =
l k j ijkl i
E E E P
) 3 ( 3
_ =
How does optical nonlinearity
appear
The strength of the
electric field of the light
wave should be in the
range of atomic fields
N
a
0

e
v h
2
0
/ a e E
at
=
2 2
0
/ me a =
esu 10 2
7 =
~
at
E
Nonlinear Optical Interactions
The E-field of a laser beam


2
nd
order nonlinear polarization
C.C. ) (
~
+ =
t i
Ee t E
e
) C.C. ( 2 ) (
~
2 2 ) 2 ( * ) 2 ( ) 2 (
+ + =
t i
e E EE t P
e
_ _
e
e
e 2
) 2 (
_
2
nd
Order Nonlinearities
The incident optical field


Nonlinear polarization contains the following terms
. . ) (
~
2
1
2 1
C C e E e E t E
t i
t i
+ + =

e
e
(OR) ) ( 2 ) 0 (
(DFG) 2 ) (
(SFG) 2 ) (
(SHG) ) 2 (
(SHG) ) 2 (
*
2 2
*
1 1
) 2 (
*
2 1
) 2 (
2 1
2 1
) 2 (
2 1
2
2
) 2 (
2
2
1
) 2 (
1
E E E E P
E E P
E E P
E P
E P
+ =
=
= +
=
=
_
_ e e
_ e e
_ e
_ e
1
e
2
e
) 2 (
_
1
e
2
e
2 1 3
e e e + =
Sum Frequency Generation
1
e
3
e
2
e
Application:
Tunable radiation in the
UV Spectral region.
Application:
The low frequency
photon, amplifies in
the presence of high
frequency beam . This
is known as parametric
amplification.
2
e
1
e
1
e
2
e
) 2 (
_
2
e
1
e
2 1 3
e e e =
Difference Frequency
Generation
1
e
3
e
2
e
Phase Matching
e
) 2 (
_
e 2
Since the optical (NLO) media are dispersive,
The fundamental and the harmonic signals have
different propagation speeds inside the media.

The harmonic signals generated at different points
interfere destructively with each other.
SHG Experiments
We can use a
resonator to increase
the efficiency of SHG.
Third Order Nonlinearities
When the general form of the incident electric field is in
the following form,


The third order polarization will have 22 components
which their frequency dependent are

t i t i t i
e E e E e E t E
3 2 1
3 2 1
) (
~
e e e
+ + =
3 , 2 , 1 , , ), 2 ( ), 2 (
) ( ), ( , 3 ,
= +
+ + +
k j i
j i j i
k j i k j i i i
e e e e
e e e e e e e e
The Intensity Dependent
Refractive Index
The incident optical field



Third order nonlinear polarization


C.C. ) ( ) (
~
+ =
t i
e E t E
e
e
) ( | ) ( | ) ( 3 ) (
2 ) 3 ( ) 3 (
e e e e e e _ e E E P + = =
) ( | ) ( | ) ( 3 ) ( ) (
2 ) 3 ( ) 1 ( TOT
e e e e e e _ e _ e E E E P + = + =
The total polarization can be written as
One can define an effective susceptibility
) 3 ( 2 ) 1 (
eff
| ) ( | 4 _ e t _ _ E + =
The refractive index can be defined as usual
eff
2
4 1 t_ + = n
By definition
I n n n
2 0
+ =
where
2
0
| ) ( |
2
e
t
E
c n
I =
) 3 (
2
0
2
2
12
_
t
c n
n =
Mechanism n
2
(cm
2
/W) (esu) Response time (sec)
Electronic Polarization
10
-16
10
-14
10
-15

Molecular Orientation
10
-14
10
-12
10
-12

Electrostriction
10
-14
10
-12
10
-9

Saturated Atomic
Absorption
10
-10
10
-8
10
-8

Thermal effects
10
-6
10
-4
10
-3

Photorefractive Effect
large large Intensity dependent
) 3 (
1111
_
Typical values of nonlinear refractive index
Material
1111
Response
time
Air 1.210
-17

CO
2
1.910
-12
2 Ps
GaAs (bulk room
temperature)
6.510
-4
20 ns
CdS
x
Se
1-x
doped
glass
10
-8
30 ps
GaAs/GaAlAs (MQW) 0.04 20 ns
Optical glass (1-100)10
-14
Very fast
Third order nonlinear susceptibility of some material
Processes due to intensity
dependent refractive index
1. Self focusing and self defocusing
2. Wave mixing
3. Degenerate four wave mixing
and optical phase conjugation
Self focusing and self defocusing
The laser beam has Gaussian intensity
profile. It can induce a Gaussian refractive
index profile inside the NLO sample.
) 3 (
_
Wave mixing
/2) Sin( 2
0
u

n
= A
Optical Phase Conjugation

Phase conjugation mirror
M
M

PCM
PCM
s
Aberration correction by PCM
PCM
Aberrating
medium
PCM
s
Aberrating
medium
What is the phase conjugation
C.C. ) , (
~
+ =
t i
s s
e E t r E
e
r ik
s s
s
e A E
.
s

=
The signal wave
The phase conjugated wave
C.C. ) , (
~
*
+ =
t i
s c
e rE t r E
e
Degenerate Four Wave Mixing
) 3 (
_
A
1
A
2

A
3

A
4

All of the three incoming beams A
1,
A
2
and A
3
should be originated
from a coherent source.
The fourth beam A
4,
will have the same Phase, Polarization, and
Path as A
3.
It is possible that the intensity of A
4
be more

than that of A
3

Mathematical Basis
. . ) ( ) . (
~
) . (
C C e r A t r E
t r k i
i i
i
+ =
e
The four interacting waves
The nonlinear polarization
) ). (( *
3 2 1
) 3 ( *
3 2 1
) 3 ( NL
3 2 1
6 6
t r k k k i
e A A A E E E P
e
_ _
+
= =
The same form as the phase
conjugate of A
3

Holographic interpretation of
DFWM
) 3 (
_
A
1
A
2

A
3

A
4

Bragg diffraction
from
induced dynamic
gratings