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Introduction to Nonlinear Optics

MOHAMMAD IMRAN AZIZ


Assistant Professor
PHYSICS DEPARTMENT
SHIBLI NATIONAL COLLEGE, AZAMGARH
(India).

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How to make a laser in
three easy steps …

 • Pick a medium that has the potential for optical gain – i.e.,
an
 amplifying medium.
 • Select a means of putting energy into that medium – i.e.,
an
 excitation system.
 • Construct an optical feedback system for stimulating
further
 emission, i.e., an optical resonator.

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Introduction

Question:
Is it possible to change
the color of a
monochromatic light?

NLO sample
input output

Answer:
Not without a laser light

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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

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E2 E2
hν hν

E1 E1
Absorption Spontaneous
Emission

E2
hν hν hν

E1
Stimulated
Emission
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Light (Microwave) Amplification
by
Stimulated
Emission of Radiation

LASER
(MASER)
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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)

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

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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

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Maiman
and the
first ruby
laser

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Ali Javan and
the first He-
Ne Laser

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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

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

 (Present time) Medicine, Research, Supermarkets, Entertainment,


Industry, Military, Communication, Art, Information technology, …

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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)

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2. The Essence of Nonlinear
Optics
When the intensity
of the incident

Output
light to a material
system increases
the response of
medium is no
longer linear

Input intensity

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Response of an optical
Medium
The response of an
optical medium hν
to the incident µ
electro magnetic hν
hν µ
field is the µ µ

induced dipole hν
moments inside µ
the medium

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Nonlinear Susceptibility
Dipole moment per unit volume or polarization

Pi = Pi 0 + χ ij E j

The general form of polarization

Pi = Pi + χ E j + χ
0 (1)
ij
(2)
ijk E j Ek + χ (3)
ijkl E j Ek El + 

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Nonlinear Polarization
 Permanent 0
Polarization
Pi
 First order
polarization: Pi = χ E j
1 (1)
ij
 Second order
Polarization Pi = χ E j Ek
2 ( 2)
ijk
 Third Order
Polarization
Pi = χ E j Ek El
3 ( 3)
ijkl

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How does optical nonlinearity
appear
The strength of the
electric field of the
e
light wave should be
in the range of atomic hν a0
fields N
Eat = e / a 2
0

a0 =  2 / me 2
=7
Eat ≈ 2 ×10 esu
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Nonlinear Optical
Interactions
 The E-field of a laser beam
~
E (t ) = Ee − iωt + C.C.
 2nd order nonlinear polarization
~ ( 2)
P (t ) = 2 χ ( 2 ) EE * + ( χ ( 2 ) E 2 e −2iωt + C.C.)


ω χ ( 2)

ω
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2nd Order Nonlinearities
 The incident optical field
~ − iω1t − iω 2 t
E (t ) = E1e + E2 e + C.C.
 Nonlinear polarization contains the following
terms
P (2ω1 ) = χ E1
( 2) 2
(SHG)
P (2ω 2 ) = χ ( 2 ) E22 (SHG)
P (ω1 + ω 2 ) = 2 χ ( 2 ) E1 E2 (SFG)
P (ω1 − ω 2 ) = 2 χ ( 2 ) E1 E2* (DFG)
P ( 0) = 2 χ ( 2)
( E1 E + E2 E ) (OR)
*
1
*
2
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Sum Frequency Generation
ω2 ω2
χ ( 2) ω 3 = ω1 + ω 2
ω1 ω1

Application: ω2
Application:
Tunable radiation in the ω3
Tunable radiation in the ω1
UV Spectral region.
UV Spectral region.

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Difference Frequency
Generation
ω2 ω2
χ ( 2) ω 3 = ω1 − ω 2
ω1 ω1
Application:
Application:
The low frequency ω2
The low frequency
photon,ω 2 amplifies in
photon, amplifies in ω1
the presence of high
the presence of high ω3
frequency beam ω . This
frequency beam 1. This
is known as parametric
is known as parametric
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Phase Matching

ω
χ ( 2)


•Since the optical (NLO) media are dispersive,
•Since the optical (NLO) media are dispersive,
The fundamental and the harmonic signals have
The fundamental and the harmonic signals have
different propagation speeds inside the media.
different propagation speeds inside the media.
•The harmonic signals generated at different points
•The harmonic signals generated at different points
interfere destructively with each other.
interfere destructively with each other.
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SHG Experiments

 We can use a
resonator to
increase the
efficiency of SHG.
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Third Order Nonlinearities
 When the general form of the incident electric
field is in the following form,
~ − iω1t − iω 2 t − i ω 3t
E (t ) = E1e + E2 e + E3e
The third order polarization will have 22
components which their frequency dependent
are
ω i ,3ω i , (ω i + ω j + ω k ), (ω i + ω j − ω k )
(2ω i + ω j ), (2ω i − ω j ), i, j , k = 1,2,3
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The Intensity Dependent
Refractive Index
 The incident optical field
~ − iω t
E (t ) = E (ω )e + C.C.

 Third order nonlinear polarization

P (ω ) = 3χ (ω = ω + ω − ω ) | E (ω ) | E (ω )
( 3) ( 3) 2

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The total polarization can be written as

P TOT
(ω ) = χ E (ω ) + 3χ (ω = ω + ω − ω ) | E (ω ) | E (ω )
(1) ( 3) 2

One can define an effective susceptibility

χ eff = χ (1)
+ 4π | E (ω ) | χ 2 ( 3)

The refractive index can be defined as usual

n = 1 + 4π χeff
2

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By definition

n = n0 + n2 I
where
n0 c
I= | E (ω ) |2

12π 2 (3)
n2 = 2 χ
n0 c
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Typical values of nonlinear refractive index

Mechanism n2 (cm2/W) χ1111


( 3) (esu) Response time

(sec)
Electronic 10-16 10-14 10-15
Polarization
Molecular 10-14 10-12 10-12
Orientation
Electrostriction 10-14 10-12 10-9
Saturated Atomic 10-10 10-8 10-8
Absorption
Thermal effects 10-6 10-4 10-3
Photorefractive large large Intensity dependent
Effect

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Third order nonlinear susceptibility of some material

Material  1111 Response


time
Air 1.2×10-17

CO2 1.9×10-12 2 Ps

GaAs (bulk room 6.5×10-4 20 ns


temperature)
CdSxSe1-x doped 10-8 30 ps
glass
GaAs/GaAlAs 0.04 20 ns
(MQW)
Optical glass (1-100)×10-14 Very fast

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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

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Self focusing and self
defocusing
 The laser beam has Gaussian
intensity profile. It can induce a
Gaussian refractive index profile
inside the NLO sample.

χ ( 3)

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Wave mixing

λ
Λ=
2n0Sin(θ/2)

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Optical Phase Conjugation
 Phase conjugation mirror

PCM
M

s
PCM

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Aberration correction by
PCM

Aberrating
medium
PCM

s Aberrating
medium
PCM

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What is the phase
conjugation
The signal wave

~ Es = ε̂ s As e ik s .r
Es (r , t ) = Es e − iωt + C.C.

The phase conjugated wave

~ * − iω t
Ec (r , t ) = rEs e + C.C.

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Degenerate Four Wave
Mixing
A1 A2

χ ( 3)
A3

A4
•All of the three incoming beams A1, A2 and A3 should be originated
•All of the three incoming beams A1, A2 and A3 should be originated
from a coherent source.
from
•Theafourth
coherent
beam source.
A4, will have the same Phase, Polarization, and
•The fourth beam A4, will have the same Phase, Polarization, and
Path as A3.
Path as A3.
•It is possible that the intensity of A4 be more than that of A3
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Mathematical Basis
The four interacting waves

~
Ei (r.t ) = Ai (r )e i ( ki .r −ωt ) + C.C.

The nonlinear polarization

* i (( k1 + k 2 − k 3 ).r −ωt )
P NL
= 6 χ E1 E2 E = 6 χ A1 A2 A e
( 3) *
3
( 3)
3

The same form as the phase


The same form as of
conjugate theAphase
3
conjugate of A3
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Origin of Nonlinearities in
Optics
 The fast response of media to an
electromagnetic wave in visible and
near IR is caused by a displacement
of electrons, both free ones in metals
and bound ones in dielectrics.

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Origin of Nonlinearities in
Optics
The fast response of media to an
electromagnetic wave in visible and
near IR is caused by a displacement
of electrons, both free ones in metals
and bound ones in dielectrics.

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1. Free electrons
The motion of electron in the field of a light wave:
 
[ 
E (t ) = E0 exp i (ωt − k r ) ]
(1
 
[ 
H (t ) = H 0 exp i (ωt − k r ) ]
is described by an equation:

[
e  1   
]
2
d r
2
= − E + V × H  (2)
dt m c 
 
[  
]
BecauseV ∝ E , the vector productV × H is proportional E 2 .
to
The solution of (2) can be found in a
form:   ( 2 )   ( 3)   
r = γ E + γ EE + γ EEE + ...
(1)
(3)
wher γ (1) is γ ( 2 ) , γ ( 3) ... are nonlinear polarisabilities.
 
e linear
The induced, electrical dipole moment isd = er (4)
equal to
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2. Bound electrons
For the case of bound electron the equation has the following
form:
 
r + 2 βr + ω r + F = − e E (t )
  2 
(5)
NL
m

where the FNL takes into account real anharmonisity of
term   the 
oscillator:FNL = ar r + br r r + ...

Considerin FNL as a small term the solution of (5) can be
presented as:
  ( 2 )   ( 3)   
r = γ E + γ EE + γ EEE + ...
(1)
(3)

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3. Macroscopic characteristics
To describe the media response for the electromagnetic field

one must calculate a polarization vector P , which is a dipole
moment of a unit volume.
  
P = Nd = Ner (6
Where N is the concentration of electrons. )
  
If a nonlinear dependenced of E on takes placed the

P vectors and can be presented in the form:
      ( 2 )   ( 3)   
d = d ( E ) = d L + d NL = γ E + γ EE + γ EEE + ...
(1) (7
        )
P = P ( E ) = PL + PNL = χ E + χ EE + χ EEE + ...
(1) (2) ( 3) (8)
γ ( 2) , χ (2)
whereγ (1) , χ (1) are tensors of 2 rank, are tensors of
3 rank
and
χ ( n ) −so(non.
≥ 2) are nonlinear susceptibilities

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4. Local field factor
In a microscopic model of nonlinearity (we presented two
such models) it is important to describe correctly microscopic γ (n )
and macroscopic
χ (n ) values. For crystals of cubic
symmetry:
 n 2
(ω ) + 2 
χ (1) (ω ) = Nγ (1)   (9)
 3 
where the term in brackets is so-called Lorentz factor (local
field factor). For nonlinear susceptibility in particular for
quadratic nonlinearity:
 n 2
(ω ± ω ) + 2   n 2
(ω1 ) + 2 
χ (ω1 ± ω2 ) = Nγ (ω1 ± ω2 ) 
(2) (2) 1 2
 ×  ×
 3   3 
 n 2 (ω2 ) + 2 
×  (10)
 3 
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5. How high is the nonlinearity
If the response of the media is caused by electrons in
nonresonant
χ (n ) case for the following ratio is valid:
χ ( n +1) 1
= (11)
χ (n)
EA
E
where A is an interatomic field. For hydrogen A E ≈ 10 9
V cm .
One can see from this that appreciable nonlinear effects can
be observed at relatively high light intensities, which are the
features of pulse lasers. The nonlinear optics experiments
became real after innovation of Q-switched laser with pulse
duration of 10-8 s and intensities of 1010 -1011 W/cm2. Now
femtosecond lasers became available, which generate pulses
with duration of 6-30·10-15 s at the intensity up to 1017 -1020
W/cm2. In this case the electric field in the light wave exceeds
the value of EA. It opens completely new branch of optics:
physics of superstrong fields.
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Besides the above electronic nature of nonlinear response a
strong nonlinearity can be caused by an anharmonisity of
atomic oscillation in molecules, orientation of polar molecules
in an electric field, heating of medium. The slower is a
mechanism responsible for nonlinearity the stronger is the
nonlinearity.
Let us present the values of characteristic time constants and
the values of χ (n ) for different mechanism of nonlinear
polarization.
Mechanism nonresonant resonant orientation in
electronic electronic liquid crystals
Time constant, s 10-14 10-7 -10-8 1-10-1
χ (2), esu 10-9 10-6 -10-8

χ (3)
, esu 10-14 -10-15 10-10 10-1 -10-2

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III. Optical
Harmonic
Generation
The high intensity light wave induces
the nonlinear polarization in a
medium. The wave of polarization is
a source for new electromagnetic
waves.

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1. Second-harmonic generation
First of all we should notice that the tensor χ ( 2) , for
centrosymmetric media is equal to zero.
( 2 ) 
PNL = χ EE( 2) (12)
The operation of symmetry transforms the terms from (12) in
the following way:
χ ( 2) → χ ( 2)
 
E → −E (13)
 
P → −P
( 2)    ( 2)
Then PNL = χ EE = χ (− E )(− E ) = − PNL
( 2) ( 2)
, that can not take
place under nonzero χ ( 2) .
The same is valid for all even order χ (n)
, n = 2m .

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For a simplicity we assume that the medium is isotropic.
Then the polarization:
P = P (1) + P ( 2) + P (3) + ... = χ (1) E + χ ( 2) E 2 + χ (3) E 3 + ... (14)
The incident waves propagating in z-direction can be
presented as: E1 = E10 cos(ω1t − k1 z )
E2 = E20 cos(ω2t − k 2 z ) (15)
( 2)
PNL = χ ( 2) [ E10 cos(ω1t − k1 z ) + E20 cos(ω2t − k 2 z )]2 =
= χ ( 2 ) [ E102 cos 2 (ω1t − k1 z ) + E202 cos 2 (ω2t − k 2 z ) +
+ 2 E10 E20 cos(ω1t − k1 z ) cos(ω2t − k 2 z )] =
= χ ( 2 ) {0.5 E102 [1 + cos 2(ω1t − k1 z )] + 0.5 E202 [1 + cos 2(ω2t − k 2 z )] +
+ E10 E20 cos[(ω1 + ω2 )t − ( k1 + k 2 ) z ] +
+ E10 E20 cos[(ω1 − ω2 )t − (k1 − k 2 ) z ]} (16)
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A spectrum of polarization waves contains new
frequencies: 2ω , 2ω , ω + ω , ω − ω , ω = 0 .
1 2 2 1 2 1

E1 , E2

0 ω1 ω2 ω
P

0
ω-
2 ω1 2ω1 ω+
2 ω1
2ω2 ω
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2. Third-harmonic generation
If the medium possesses cubic nonlinearity, under the action
of two monochromatic waves ω1 ωand
2 Pthe
( 3)
polarization
would contain the components with frequencies:
3ω1 , 3ω2 , 2ω1 ± ω2 , 2ω2 ± ω1 .

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IV. Wave Nonlinear
Optics
As the optical harmonic generation takes
place both induced waves of polarization and
free running electromagnetic waves of
harmonics are propagating in the medium. If
the dimensions of the medium are much
larger than pumping wavelength the phase
matching determines the efficiency of the
energy transfer from the pumping wave to
harmonics. Let us consider the phase
matching conditions for the case of second
harmonic generation.
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1. Maxwell equations
The propagation of the light in the medium is described by
Maxwell equations:
 wher
  1 ∂B e 
 rot E = − B = µH
 c ∂ t
   
  4π  1 ∂D D = E + 4πP = (18)
rot H = j+ (17)  (1) NL
 c c ∂t = E + 4πP + 4πP

div B = 0 For optical
  range
div D = 4π ρ µ = 1, ρ = 0, j = 0 (19)
Combining first and second equations from (17) one may
obtain so-called wave equation:
 
 1 ∂ E 4π ∂ D
2 2
∆E = 2 2 + (20)
c ∂t c ∂t 2

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Inserting (18) into (20) we are getting:
 (1) NL
 1 ∂ E 4π ∂ P
2 2
4π ∂ P
2
∆E − 2 2 − = (21)
c ∂t c ∂t 2
c ∂t 2
The nonlinear polarization term in the right hand side of (21)
plays a role of a source of electromagnetic waves
2. Phase mismatch
For quadratic media( χ ( 2 ) ≠ 0)and relatively low nonlinearity the
plane wave solution of (21) for the intensity of the second
harmonic looks like:
2 ω (nω − n2ω ) z
sin
[ χ ( 2 ) I ω ]2 c (22)
I 2ω ∝ ⋅ 2
n22ω  ω ( nω − n2ω 
)
 c 
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Phase ∆ k = 2 kω − k 2 ω = (nω − n2ω )
mismatch c
max
I2ω/I2ω
1

Δkz/2
-2π -π 0 π 2π
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For the case of the exact phase matching the energy of the
pumping wave can be completely transferred into second
harmonic
I
I2ω


0
L 2L z
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3. Phase matching
How the condition ∆ k = 2kω − k 2ω = 0 or nω − n2ω = 0 can be
realized? In an isotropic medium with normal dispersion n2ω> nω
and∆ k never equals to zero
Directions of
phase matching
But in birefringent uniaxial
crystal there are two beams
ordinary and extraordinary. For
o
so-called negative crystal no>ne. nω
If pumping wave is ordinary one
and second harmonic is nω
e

extraordinary one the material


dispersion ( n2ω > nω ) can be n
o

compensate for the difference in
refractive indices for o and e e
beams: ω n o
= n e

n 2ω
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For the process of third-harmonic generation the condition of
phase matching looks the same: ∆k = 0
As it was mentioned alreadyχ ( 2) and χ (3) values for the fast
nonresonant electronic polarization do not much differ for
many materials and the only way to enhance the efficiency of
nonlinear energy transformation is to phase match the
interacting waves.

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V. Other Nonlinear
Effects
1. Modulation of a refractive index
Cubic nonlinearity causes not only wave generation with new
frequency but also appearance of a wave of nonlinear
polarization with the frequency of pumping wave:
ω1 = ω1 + ω1 − ω1 (23)
2
PNL (ω1 ) = χ (ω1 ; ω1 , ω1 ,−ω1 ) E (ω1 ) E (ω1 )
( 3)

As a result of such selfaction a nonlinear refractive index n2I


appears at the frequency ω1 :
n = n0 + n2 I n2 ∝ χ (3) (ω1 ; ω1 , ω1 ,−ω1 ) (24)
For the fast nonresonant nonlinearity n2 is relatively small:
n2~10-13 cm2/kW.
For slower mechanisms of the nonlinearity n2 can be much
larger in particular for liquid crystals: n2~0.1 cm2/kW.
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2. Selffocusing
If the intensity of a laser beam is high enough instead of
diffraction an opposite effect of selffocusing takes place.
Phase velocity depends on the intensity through nonlinear
refractive index:
Vph =c/n0+n2I (25)
If n2 > 0 the phase velocity at the axis of the beam is lower
and nonlinear medium is working as a lens.

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Phase front
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VI. Nonlinear
Optical
Diagnostics
Nonlinear susceptibilities χ and χ are tensors and they
( 2) ( 3)

inherit the symmetry properties of the crystalline medium. It


means that nonlinear optical effects are structure sensitive. It
can be employed to study different structure transformations.
A lot of such experiments were done. I will mention just one
related with laser induced melting of semiconductors.
R melting Ge, Si
point
RL
R(t)
RS
laser pulse

t
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1. Nonlinear optical diagnostics of phase
transitions
Semiconductor in liquid
Idea of stateMetal in liquid
experiment
Powerful laser beam
R statemelting 23
AB
65

which melts the surface point


NL
(Ruby, Nd:YAG , Eximer) RS
nonlinear
reflection
Pro

NL
NL
RL
bin
gH
e-N

L
n
RL
eb

tio
eam

lec

Pro linear
ref

b
ear

las ing N r RLS


reflection
Lin

er b d:Y linea 2 )ω
eam AG n
( )ω No tion (
lec
ref laser pulse
Semiconductor
t

aziz_muhd33@yahoo.c
o.in
VIII. Conclusions
1.Nonlinear optics is an attractive and fast
developing part of modern optics.
2.Nonlinear effects are structure sensitive in
their nature. It can be used for time-
resolved monitoring of structural
transformation (up to femtosecond time
resolution).
3.Artificial photonic media on the base of
porous semiconductors open new exciting
possibilities for the control of nonlinear
o.inoptical processes.
aziz_muhd33@yahoo.c

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