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Shai Rozenberg

1
Outline
 Introduction

 Mathematical Overview
 The Coupled-Wave Equations for Sum-Frequency Generation
 2nd Order Nonlinear Optical Tensor

 Second Order Nonlinear Effects - SFG, DFG and (SHG as degenerate


case of SFG)
 The coupled equations
 Coherence Length & Phase Matching
 Experimental Configurations
 New Nonlinear Material – Orientation Poled GaAs

 Third Order Nonlinear Effects


 Kerr Effect
 Stimulated Raman Scattering
 Stimulated Brillioun Scattering
 Four Wave Mixing and Phase Conjugation

 Summary and Applications 2


References
Photonics – Optical Electronics In Modern
Communication ,6th Edition/ Amnon Yariv, Pochi
Yeh

Nonlinear Optics ,2nd Edition/ Boyd W.R

Nice pictures from the internet….

3
Introduction
Nonlinear Optics is the study of phenomena
that occur as a consequence of the
modification of optical properties of
material system by the presence of light.
Typically, only laser light is sufficiently intense
to modify the optical properties of a material
system.
Second Harmonic Generation by Franken et
al. in 1961.

4
Some Nonlinear Optical
Phenomena
SFG – Sum Frequency Generation
SHG – Second Harmonic Generation
DFG – Difference Frequency Generation
THG – Third Harmonic Generation
Self Focusing
Saturable Absorption
SRS – Stimulated Raman Scattering
SBS – Stimulated Brillioun Scattering
…

5
Introduction
In case of Linear Optics the induced dipole P~ (t )
moment per unit volume, or polarization ,
~
when applying
E (t ) an electic field is:
~ (1) ~
P (t ) = χ ⋅ E (t )

In Nonlinear Optics, the optical response can


be described by:
~ (1) ~ ( 2) ~ 2 ( 3) ~ 3
P (t ) = χ ⋅ E (t ) + χ ⋅ E (t ) + χ ⋅ E (t ) + ...

1st , 2nd , 3rd


Optical
6
Susceptibiliti
Introduction
More general …

~ ~ ~ ~ ~ ~ ~
Pi (t ) = ε 0 χ ij ⋅ E j (t ) + 2d ijk χ ( 2 ) ⋅ E j (t ) ⋅ Ek (t ) + 4 χ ijkl ⋅ E j (t ) ⋅ Ek (t ) ⋅ El (t ) + ...

7
Nonlinear Susceptibility of Anharmonic
Oscillator

8
Nonlinear Susceptibility of Anharmonic
Oscillator

9
Nonlinear Susceptibility of Anharmonic
Oscillator

10
Nonlinear Susceptibility of Anharmonic
Oscillator

11
Wave Equation Description of Nonlinear Optical
Interactions

12
Wave Equation Description of Nonlinear Optical
Interactions

13
2nd Order Nonlinear Optical Tensor

Only noncentrosymetric crystals can posses a


d ijk
non vanishing term, why?

P0ωi 1 +ω2 = 2d ijk E0ω1j E0ωk2

Centrosymetric crystal will have the same


polarization under fields reversal, so:
( )(
− 2d ijk E0ω1j E0ωk2 = 2d ijk − E0ω1j − E0ωk2 )

d ijk = 0
14
2nd Order Nonlinear Optical Tensor

15
2nd Order Nonlinear Optical Tensor

16
The Coupled-Wave Equations for Sum-Frequency
Generation

Consider the nonlinear coupling of two optical


fields given by:ω1 1 ω1 iω1t
E j (t ) = ( E0 j e + c.c)
2
ω2 1 ω 2 iω 2 t
Ek (t ) = ( E0 k e + c.c)
2
j , k = x, y , z

We consider the ith cartesian component of


ω3 = ωat
the nonlinear polarization 1 + ω2

ω3 =ω1 +ω 2 1 ω 3 iω 3 t
Pi (t ) = ( P0i e + c.c)
2
i = x, y , z 17
The Coupled-Wave Equations for Sum-Frequency
Generation

Limiting our attention to the 2nd order terms


1 ω1 iω1t 1 ω1 iω1t
Pi = 2d ijk E j Ek = 2d ijk ( E0 j e + E0 j e + c.c) ⋅ ( E0 k e + E0ωk2 e iω2t + c.c)
ω 2 iω 2 t

2 2
Consider only the sum terms
ω1 +ω 2 1 ω1 ω 2 i (ω1 +ω 2 ) t 1
Pi = d ijk E0 j E0 k e + d ikj E0ωk2 E0ω1j ei (ω1 +ω2 )t + c.c
2 2
= d ijk E0ω1j E0ωk2 ei (ω1 +ω2 )t + c.c
ω +ω ω ω
Also define :P0i 1 2 = 2d ijk E0 1j E0 k2 and then :
ω1 +ω 2 1 ω1 +ω2 i (ω1 +ω2 )t
Pi = P0i e + c.c
2
18
The Coupled-Wave Equations for Sum-Frequency
Generation

1 ω1 i (ω1t −k1z ) 1
Eiω1 (t ) = ( E0 i e + c.c) = (a1i E1ei (ω1t − k1z ) + c.c)
2 2
1 1
Eiω2 (t ) = ( E0ωi2 ei (ω2t − k2 z ) + c.c) = (a2i E2 ei (ω2t − k2 z ) + c.c)
2 2
1 1
Eiω3 (t ) = ( E0ωi3 e i (ω3t − k3 z ) + c.c) = (a3i E3ei (ω1t −k1 z ) + c.c)
2 2
Ei (t ) = Eiω1 (t ) + Eiω2 (t ) + Eiω3 (t )
i = x' , y' , z '

In the absence of nonlinear response, these three fields are


solutions of the wave equation and are propagating along
independently in the medium. 19
The Coupled-Wave Equations for Sum-Frequency
Generation

∂2 ∂2E ∂ 2 PNL
∇ E = µ 0 2 (ε 0 E + P ) = µ 0ε 2 + µ 0 2
2

∂t ∂t ∂t
( PNL ) i = 2d ijk E j Ek
In this case we have a nonlinear response of the material,
therefore the fields are coupled

(P
ω3 −ω 2
NL ) =d
i
a a E E * i [ ( ω3 −ω 2 ) t − ( k 3 − k 2 ) z ]
ijk 3 j 2 k 3 2 e + c.c
(P
ω3 −ω1
NL ) =d
i
a a E E * i [ ( ω3 −ω1 ) t − ( k 3 − k1 ) z ]
ijk 3 j 1k 3 1 e + c.c
(P
ω1 +ω 2
NL ) =d
i
a a E E * i [ ( ω1 +ω 2 ) t − ( k1 + k 2 ) z ]
ijk 1 j 2 k 1 2 e + c.c

20
The Coupled-Wave Equations for Sum-Frequency
Generation
Slowly varying amplitude approximation
d2 d
E s << k s Es
d 2z dz
s = 1,2,3

d µ
E1 = −iω1 0 d ⋅ E3 E2*e − i ( k3 − k2 − k1 ) z
dz ε1
d * µ
E2 = + iω 2 0 d ⋅ E1 E3*e + i ( k3 − k2 − k1 ) z
dz ε2
d µ
E3 = −iω 3 0 d ⋅ E1 E2*e + i ( k3 − k2 − k1 ) z
dz ε3

d = ∑ d ijk a1i a2 j a3k


ijk 21
The Coupled-Wave Equations for Sum-Frequency
Generation
Some interesting results rise from the
previous derivation:
Conservation of Energy
d 2 2 2
( ε 1 E1 + ε 2 E2 + ε 3 E3 ) = 0
dz
ω3 = ω1 + ω2

If we define the new fields variables

nm
Am = Em
ωm
1 ε0 2 1 ε0 2
Im = nm Em = ωm Am
2 µ0 2 µ0

22
The Coupled-Wave Equations for Sum-Frequency
Generation
The coupled equations become

d
A1 = −iκ ⋅ A3 A2*e − i∆k ⋅ z
dz
d *
A2 = + iκ ⋅ A1 A3*e − i∆k ⋅ z
dz
d
A3 = −iκ ⋅ A1 A2*e − i∆k ⋅ z
dz

µ 0ω1ω 2ω 3   µ 0ω1ω 2ω 3
κ =d =  ∑ d ijk a1i a2 j a3k 
ε 0 n1n2 n3  ijk  ε 0 n1n2 n3

23
Second Harmonic Generation
In this case we consider the interaction of two waves with
frequencies w1 and w3 where w3=2w1

In this 1st experiment efficiencies where 10-8


The utilization of more efficient materials , high intensity
lasers and phase matching techniques has resulted in nearly
100% efficiency.

24
Phase Matching and Coherence
Length
 We look again at the coupled equations and assume the Nondepletion
approximation, in which the amount of power lost from the input beam w1 by
conversion to 2w1 in negligible, therefore E1 is constant.

d µ
E1 = −iω1 0 d ⋅ E3 E2*e − i ( k3 − k2 − k1 ) z
dz ε1 µ e i ( ∆k ) L
−1
⋅ E12 µ 0 id( ∆⋅k )EL 2 e +Li∆k ⋅ z
E3 ( L) = −idω E 0=⋅−diω
µ dz ε
3 1
d * ε
E2 = + iω 2 0 d ⋅ E1 E3*e + i ( k3 − k2 − k1 ) z
dz ε2 E3 (0) = 0

d µ ω3
E3 = −iω 3 0 d ⋅ E1 E2*e + i ( k3 − k2 − k1 ) z ω = ω1 = ,ε = ε 3
dz ε3 2 2  ∆k ⋅ L 
3 / 2 sin  2 
I 2ω∆k =2ωk32 d−22Lk21 µ 0 
η SHG ≡ =   Iω
 ε  ∆k ⋅ L
3
Iω n
d = ∑ d ijk a1i a2 j a3k
ijk
25
Phase Matching and Coherence
Length
 ∆k ⋅ L 
sin 2 
 2  I
3/ 2
I 2ω 2ω 2 d 2 L2  µ 0 
η SHG ≡ =   ω
Iω n3  ε  ∆k ⋅ L

For efficient 2nd harmonic generation , the wavenumber mismatch


needs to be equal for both frequencies, so∆ k = k kor( 2ω ) = 2k( ω )
( 2ω ) − 2 k ( ω ) = 0

If the SHG wave will not be in phase with some other generated
∆k ≠ 0
wave at plane say Z2 and will interfere with the original wave .
We shall define a “coherence length” by the to adjacent spatial peaks

2π 2π
lc = =
∆ k k ( 2ω ) − 2 k ( ω ) λ
lc =
2ω ω 2ω 2( n( 2ω ) − n( ω ) )
∆k = n( 2ω ) − 2 n( ω ) = ( n( 2ω ) − n( ω ) ) 26
c c c
Example : Coherence Length of Frequency
Doubling in KDP

Let λ = 1µm, and assume ordinary waves in


KDP. n( 2ω ) = 1.514928
( ω ) = 1.496044
The refractive indices are(out of a ntable):
λ 10−6
lc = = = 26.5µm
2( n( 2ω ) − n( ω ) ) 2(1.514928− 1.496044)

27
Phase Matching and Coherence
Length
In order to achieve phase matching we need to somehow equalize the
index of refraction for both of the waves…. How??

Refractive index
ne

∆k = ( n( 2ω ) − n( ω ) ) = 0
c no
n( 2ω ) = n( ω )

ω Frequency
When the waves are both in the same polarization it is impossible 2ω
to reach phase matching since the index of refraction increases
with frequency , we can however use different polarization states!!

Meaning , entering the nonlinear crystal at some angle regarding the


ordinary and extaordinary rays.

28
Far from
Show
phase- SHG crystal Movie
matching:

output beam
Input beam

Closer to
phase-matching: SHG crystal

output beam
Input beam

the SH beam is brighter as phase-matching is achieved


29
Quasi Phase Matching
As we have seen before the coherence length
defines the length where the conversion efficiency
is maximal, before any destructive interference
occur.
Another way to “increase” this coherence length
is simply by periodically alternating the crystal
principle axis, meaning that the phase lag is
constantly corrected and enables amplification.

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Intracavity SHG

Extracavity SHG

31
32
Other 2nd Order Nonlinear
Processes
OPA – Optical Parametric Amplification
In its simplest form involves the transfer of
power from “pump” wave w3, to two waves at
lower frequencies w1 and w2(also called
“signal” and “idler”), where w3=w1+w2
OPO – Optical Parametric Oscillator
A configuration in which both signal and idler
oscillate in the resonator.
Frequency Up Conversion

33
Parametric
Laser oscillator
Oscillator

Nonlinear
W3
Crystal

Laser Medium
R1=100% R1<100%
R2=100% R2<100%
R3=0% R3=0%

34
Frequency Conversion in
Semiconductors/M.M Fejer

35
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37
38
Desired Properties of Nonlinear
Crystals
Transparent in wavelengths range of interest
 Oxides – 213nm-4000nm
 Semiconductors – MidIR – 12um
Phase Matchable
Large d coefficient
Low Absorption and Scattering Losses
Resistant to Laser Damage (surface and bulk)
High Thermal Conductivity
Chemically Stable – Resistant to moisture and
oxidation
Mechanically Stable – able to cut and polish.
39
Third Order Nonlinear Optical
Processes
Third Harmonic Generation
Optical Kerr Effect
Stimulated Raman Scattering
Stimulated Brillouin Scattering
Four Wave Mixing and Phase Conjugation

Pi ( 3)
= 4 χ ijkl E j Ek El

40
Non-Linear Optical Interactions

Third Order Polarization – General Case


ω1
χ (3)
r ω3
Input : E (t ) = E1e − iω1t + E 2e − iω 2t + E 3e − iω3t + ...
P (2 ω1 ω
+ )2 =χ
3 EE(3) 2

Polarization : P (t ) = ∑ P (ωn )e
% (3) − iωnt 1 2

P (2 ω1 ω
− )2 =χ
3 EE(3)
1 2
2 *

P (ω1 ) = χ (3) 3E1E1* + 6 E 2E 2* + 6E 3E 3* E1 P (2 ω1 ω


+ )3 =χ
3 EE(3)
1 3
2

P (2 ωω
1 −)
3=χ3 EE(3) 2 *

6 E1E + 3E 2E + 6E 3E  E 2
1 3
P (ω2 ) = χ (3) *
1
*
2
*
3

P (2 ω2 ω χ3
+)1 = EE(3) 2
P (ω3 ) = χ (3) 6 E1E1* + 6E 2E 2* + 3E 3E 3* E 3 2 1

P (2 ω2 ω χ3
−)1 = EE(3)
2 1
2 *

P (3ω1 ) = χ (3)E13 P (3ω 2 ) = χ (3)


E 23 P (3ω 3) = χ (3)
E 33 P (2 ω2 ω χ3
+)3 = EE(3)
2 3
2

P (2 ω2 ω χ3
−)3 = EE(3) 2 *
P (ω1 + ω 2 + ω 3 ) = 6χ ( 3) E1E2 E3 2 3

P (ω1 + ω 2 − ω 3 ) = 6χ (3)E1E 2 E 3* P (2 ω3 ω χ3
+)1 = EE(3)
1 3
2

P (ω1 + ω3 − ω 2 ) = 6χ (3)E1E 2*E 3 P (2 ω3 ω


− 1 ) =3 χ(3)
1 E
* 2
3 E

P (2 ω3 ω χ3
+ )2 = EE(3) 2

P (ω2 + ω3 − ω1 ) = 6χ E E 2 E 3
(3) * 2 3
1 P (2 ω3 ω χ3
− )2 = E E2(3)3 * 2

41
Optical Kerr Effect
Was first discovered by J.Kerr in 1875 that a
transparent liquid becomes doubly refracting
∆ n = n − n⊥ = λ KE
when placed in a strong electric field. 2

According to the previous 3rd nonlinear


equation of polarization we get Ej (t ) 0j
1
2
( E efor
ω iω t
= ) field
+ c.ca

(
1 ω iω t
) ( 1 ω iω t
Pi (t ) = 4 χ ijkl E0 j e + c.c E0 k e + c.c E0l e + c.c
( 3)

2 2
) ( 1 ω iωt
2
)
(ω )
PNLi ( )
(t ) = χ ijkl E0ωj E0ωk E0ωl* + E0ωj* E0ωk E0ωl + E0ωj E0ωk* E0ωl
Since the polariztion has the same frequency
as the applied field the resultant is change of
the index of refraction 42
Optical Kerr Effect
Consider a simple case of an optical beam
polarized along the x-axis:
(ω )
PNLi (
(t ) = 3χ xxxx E0ωx E0ωx E0ωx* )
3cµ 0 χ xxxx − 20 m 2
∆n = n2 I = I = 3 ⋅ 10
n 2ε 0 W
For Silica Fibers
Doped With
Germanium Oxide

43
SRS – Stimulated Raman
Scattering
1888-1970
Won Nobel Prize in
1930
X-Ray diffractions,
acoustics, optics ,
dielectrics ,
ultrasonics ,
photoelectric ,
collodial particles.

44
45
46
SRS – Stimulated Raman
Scattering
Consider both laser and stokes fields are in
the x-axis direction
1
( i (ω t − k z )
E x (t ) = EL e L L + ES ei ( ω S t − k S z ) + c.c
2
)
ωL
PNL (
= EL 6 χ R31 ES ES* + 3χ 13 EL EL* )
ωS
PNL = E ( 3χ
S
3
2 ES ES* + 6 χ R3 2 E E )
L
*
L

χ R31 = χ R3*2

47
Stimulated Raman
Scattering – Coupled
Equations
dEL 1 6µ 0ω L2 (3) 2
= α L EL + i χ R1 Es E L
dz 2 kL
dEs 1 6µ 0ω s2 (3) 2
= − α s Es + i χ R 2 E L Es
dz 2 ks

Assume E laser is constant along z , and


integration along z axis we get:
Es ( z ) = Es (0) exp( GR z − α s z )
2 2

12µ 0ω s2 2
GR = EL Im(χ R(31) )
ks
48
Stimulated Raman
Scattering – Coupled
Equations
It is convenient to describe the energy
exchange in terms of photon flux, the
measure of the number of photons per unit of
area
φ=
I
ω
per unit time.
d
φ L = −α L z − GR' φ Lφ s
dz
d
φ s = −α s z + GR' φ Lφ s
dz

1 + m −1
φ L ( z ) = φ L ( 0) e −α z
γ
1 + m −1 exp (1 − e −αz ) 

α 
1+ m
φ s ( z ) = φ s ( 0) e −α z
 γ
1 + m exp − (1 − e −αz ) 

 α  γ = G '
R
[ φ s ( 0) + φ L ( 0) ]
49
Example : Raman Gain in
SiO2
Consider a laser beam power of 10mW in a
single mode fiber with an effective core area
of 100um2.
The intensity is thus I=10W/m2.
Using the gain coefficient 0f 0.8 x 10-3 cm/MW,
we obtain a Raman gain coefficient of 8 x 10-4
m-1

50
SBS – Stimulated Brillouin
Scattering
In raman scattering incoming photons interact
with vibrational modes causing frequencies
shifts in the range of 1012 -1013 Hz. Similar inelastic
scatterings can occur in which the frequency shift
is caused by physical motion of the molecules or
atoms.

For example, brillioun scattering is caused by


thermally excited acoustic waves. First
discovered by L.Brillioun at early 1922. The
frequency shift is in the range of 1010 Hz

51
SBS – Stimulated Brillouin
Scattering
Brillioun scattering can occur in all
directions
1
( i (ω t − k z )
E x (t ) = E L e L L + ES ei ( ω Bt + k B z ) + c.c
2
)
ωL
PNL (
= EL 6 χ B3 EB EB* + 3χ13 EL EL* )
ωB
PNL = E ( 3χ
S
3
2 EB EB* + 6 χ B3 E E )
L
*
L

52
SBS – Stimulated Brillouin
Scattering
dEL 1 6µ 0ω L2 (3) 2
= − α EL + i χ B EB E L
dz 2 kL
dEB* 1 * 6 µ 0ω B2 (3) 2 *
= α EB + i χ B EL EB
dz 2 kB

Assume E laser is constant along z , and


integration along z axis we get:

53
SBS – Stimulated Brillouin
Scattering

54
Four Wave Mixing and Wave
Conjugation
It is possible, using nonlinear optical processes, to
exactly reverse the propagation direction and
phase variation of a beam of light. The reversed
beam is called a conjugate beam, and thus the
technique is known as optical phase
conjugation

55
Four Wave Mixing and Wave
Conjugation
The most common way of producing optical phase
conjugation is to use a four-wave mixing
technique, though it is also possible to use
processes such as stimulated Brillouin scattering.
A device producing the phase conjugation effect is
known as a phase conjugate mirror (PCM).

56
Summary & Applications
Nonlinear optical phenomena are well known and play
very important role in several fields.
Medicine
Entertainment – disc writing, lasers show,
communication…
Military – countermeasure
Home Land Security
More…

57
Thank You For Your
Attention!

58

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