Lecture 12: Introduction to

nonlinear optics II.

Petr Kužel
Propagation of strong optic signals (proper nonlinear effects)
• Second order effects
! Three-wave mixing
Phase matching condition
! Second harmonic generation
! Sum frequency generation
! Parametric generation
• Third order effects
! Four-wave mixing
! Optical Kerr effect
 Nonlinear polarization
Pi (ω) = ε 0 χij (ω)E j (ω) + ∫ dω1 χ ijk
( 2)
(ω; ω1 , ω2 )E j (ω1 )Ek (ω2 ) + !
%"""" "$""""" #
ω= ω1 + ω2

Pi = ε 0 χij E j + χ ijk
( 2)
E j Ek + !

Intrinsic symmetry: χijk = χ ikj

For symmetric tensors Voigt notation can be introduced:

indices (ij) 11 22 33 23 or 32 13 or 31 12 or 21
contraction (l) 1 2 3 4 5 6

A 3×6 matrix χil is introduced,  χ11 χ12 χ13 χ14 χ15 χ16 
 
where l = 1…6 is a contracted index, χil =  χ 21 χ 22 χ 23 χ 24 χ 25 χ 26 
and i =1…3. χ
 31 χ32 χ33 χ34 χ35 χ36 
 Three-wave mixing
Coupling between two optical waves ω1 and ω2:
{
E ω1 (t ) = Re E ω1 eiω1t = } 12 (E ω1
eiω1t + ( E ω1 )∗ e −iω1t = ) 12 (E ω1
eiω1t + c.c. )
E ω2 (t ) = Re{E ω2
}= 12 (E
e iω 2 t ω2
) = 12 (E
e iω 2 t + ( E ω 2 ) ∗ e − iω 2 t ω2
eiω2t + c.c. )
The total field:

E = E ω1 (t ) + E ω2 (t ) = (
1 ω1 iω1t
2
E e + E ω2 eiω2t + c.c. )
Linear part of the polarization PL:
(
PL = ε 0 χ(ω1 ) E ω1 (t ) + χ(ω2 ) E ω2 (t ) )
Nonlinear part of the polarization PNL:

PNL = χ ( 2) E E =
1 ( 2) ω1 ω1 2iω1t
4
χ E E e ( + E ω2 E ω2 e 2iω2t + 2 E ω1 E ω2 ei (ω1 +ω2 )t

+ 2 E ω1 ( E ω2 )∗ ei (ω1 −ω2 )t + E ω1 ( E ω1 )∗ + E ω2 ( E ω2 )∗ + c.c. )

 Nonlinear polarization for three
wave mixing
PNL = χ ( 2) E E =
4
χ (
1 ( 2) ω1 ω1 2iω1t
E E e + E ω2 E ω2 e 2iω2t + 2 E ω1 E ω2 ei (ω1 +ω2 )t

+ 2 E ω1 ( E ω2 )∗ ei (ω1 −ω2 )t + E ω1 ( E ω1 )∗ + E ω2 ( E ω2 )∗ + c.c. )

If we take into account the dispersion, the susceptibility is weighted: χ(2)(ω1, ω2)

The polarization PNL, when introduced into the Maxwell equations, becomes
the source of the radiation at frequencies 2ω1, 2ω2, ω1 + ω2 et ω1 − ω2
It causes an energy transfer between the fundamental and the mixed spectral
components
Three wave mixing: two initial components (ω1 and ω2) give raise to a third
one (ω3)
A phase matching condition has to be fulfilled : at most one efficient energy
transfer channel is in general possible
Second harmonic generation (SHG)
Coupling between ω and 2ω — other spectral components are omitted:

E = E ω (t ) + E 2ω (t ) = (
1 ω iω t
2
)
E e + E 2ω e i 2ωt + c.c.

Pi ω, NL =
2
(
1 ( 2 ) 2 ω ω ∗ iω t
χ ijk E j ( Ek ) e + c.c. )
ω
Pi ,2NL = χ ijk
4
(
1 ( 2 ) ω ω 2 iω t
E j Ek e + c.c. )
The wave equation in the time domain then reads:
∂2E ∂ 2 PNL
∇ E = µ 0ε 2 + µ 0
2
∂t ∂t 2
Absorption can be taken into account in ε; however, we neglect it here
The waves are supposed to propagate along z; their amplitudes do not
depend on x and y.
 SHG: continued
E ωj (z , t ) =
1 ω
2
( )
E j ( z ) ei (ωt − k1z ) + c.c. E 2j ω (z , t ) = (
1 2ω
2
)
E j ( z ) e i (2ωt − k2 z ) + c.c.

The energy transfer between the two waves is assumed to be very small in
the scale of the wavelength:
dE ωj d 2 E ωj dE 2j ω d 2 E 2j ω
k1 >> 2
k 2 >>
dz dz dz dz 2

Coupled wave equations:

 2 2 2 E ωj dE ωj  i (ωt −k1z ) ∂ 2 Pjω, NL

(
 ω nω c − k1
2
2
− ik1 )
dz
e

+ c.c. = µ 0
∂ t 2
 

( ) 
2ω 2ω 2 2ω
E dE i (2 ωt − k2 z ) ∂ Pj , NL
 (2ω) n22ω c 2 − k22
2 j
− ik 2
j  e + c.c. = µ 0
 2 dz  ∂t 2
 
 Coupled-wave equations
 2 2 2 E ωj dE ωj  i (ωt −k1z ) ∂ 2 Pjω, NL

(
 ω nω c − k1
2
2
)
− ik1
dz
e

+ c.c. = µ 0
∂ t 2
 


(
 (2ω) n2ω c − k2
2 2 2 2 E 2j ω
2
)
− ik 2
dE 2j ω  i (2ωt − k2 z )
dz
e

+ c.c. = µ 0
∂ 2 Pj2,ωNL
∂ t 2
 
The wave equations without coupling define the wave vectors k1 and k2:
ω2 nω2 c 2 − k12 = 0 (2ω)2 n22ω c 2 − k 22 = 0

We finally obtain:

dE ωj iωη0 ( 2) 2ω ω ∗ −i (k2 −2 k1 )z
=− χ jkl Ek ( El ) e
dz 2nω
dE 2j ω iωη 0 ( 2) ω ω −i (2 k1 −k2 )z
=− χ Ek El e
dz 2n2ω jkl
 Constant field approximation
The fundamental wave is supposed not to be depleted:
dE 2j ω iωη 0 ( 2) ω ω −i (2 k1 −k2 )z
=− χ jkl Ek El e
dz 2n2ω

Solution:
E 2j ω ( z ) = B − A ei∆kz

with
∆k = k 2 − 2k1
2) ω ω
ω η0 χ (jkl Ek El
A=
2 n2ω ∆k

B determined from the boundary condition: E 2j ω ( z = 0) = 0

 SHG solution
ω η0 1 − ei∆kL ( 2) ω ω
E 2j ω ( L) = χ jkl Ek El
2n2ω ∆k

I 2ω
n
= 2ω E 2j ω ( L)
2 1
= η30
( ) 2
ω2 χ (eff2) L2
I ω2
sin 2 ( 12 ∆kL)
2η0 2 n2ω nω2 (12 ∆kL )2
Character of the solution depends critically on the value of ∆k
∆k ≠ 0
Both waves do not propagate with the same phase velocity: they are not
constantly in phase, but become periodically out-of-phase. This leads to
a modulation of I2ω with the period (called coherence length):
2π 2π λ
lc = = =
∆k k 2 − 2k1 2(n2ω − nω )

Typically: n2ω − nω ≈ 10−2, lc ≈ 100 µm. This is the maximum crystal

length that can efficiently participate to SHG.
 Phase matching condition
∆k = 0 ⇒ k 2 = 2k1 n2ω = nω

I 2ω =
1
η30
( )
( 2) 2
ω χ eff
2
I ω2 L2
2 n2ω nω2

All the crystal length participates efficiently to the generation

z (optical axis)
How to achieve the phase matching
condition: θ k1
no,2ω
• Compensation of the birefringence no,ω
ne,2ω(θ)
and the dispersion
OO-E interaction ne,ω
ne, 2ω (θ ) = no,ω

no−,2ω − no−,22ω ne,2ω

sin θ =
2
ne−,22ω − no−,22ω
 Phase matching condition:
continued
z (optical axis)
EO-E interaction:
∆k = 0 ⇒ k 2ω,e = kω,o + kω,e θ
no,2ω
k

ne, 2ω (θ ) =
1
2
(no,ω + ne,ω (θ ))
no,ω
ne,ω

ne,2ω(θ)
The choice of the polarizations ne,2ω ne,ω(θ)
depends on the available coeffi-
cients of χijk (e.g. χ111 couples only
parallel polarizations and thus can
never allow the phase matching)
 Three-wave mixing: summary
General equations of three-wave mixing
ω1 ± ω2 ± ω3 = 0 (frequency transformation)
k1 ± k 2 ± k3 = 0 (phase matching condition)
Sum and difference frequency generation (SFD, DFD):
•Input: two strong beams ω1 and ω2 ω1 ± ω2 = ω3
•Output: strong beam ω3 k1 ± k 2 = k3
Parametric generation (amplification of weak beams):
•Input: strong ω3 + weak ω1 ω3 − ω1 = ω2
•Output: medium ω2 + medium ω1 k3 − k1 = k 2

Up-conversion
•Input: strong ω1 + weak ω2 ω1 + ω2 = ω3
•Output: weak ω3 k1 + k 2 = k3
 Four-wave mixing
Third order effect:
ω4 ( 3) ω1 ω2 ω3
PNL = χ ijkl E j Ek El

Required conditions for the wavelength transformation:

ω4 = ω1 + ω2 + ω3 ω4 + ω3 = ω1 + ω2
or etc.
k 4 = k1 + k 2 + k3 k 4 + k3 = k1 + k 2
Degenerated cases are frequently used
Transient grating experiments
 Propagation in Kerr-like media
Degenerated case (one very strong optical beam):
ω
PNL = 3χ (3) E ω E ω E ω ( ) ∗

Indices are omitted (i.e. the beam is linearly polarized and it is an

eigenmode of the medium
The beam propagated along z:
E ω (z , t ) = A(z )ei (ωt − kz )

Wave equation:

(
 2 2 2
 ω n c − k A − 2ik
2
)
dA  i (ωt −kz )
e = −3µ 0ω2 χ (3) A2 A∗ei (ωt −kz )
 dz 

Linear wave equation:

Nonlinear polarization
definition of k
 Propagation in Kerr media:
continued
Remaining terms in the wave equation
dA 3 µ 0 ω ( 3) 2
= −i χ A A
dz 2 ε0 n

if χ(3) is real then

 3η0 ωχ (3) 2 
A = A0 exp − i A0 z  = A0e −ik1z E ω (z , t ) = A(z )e i (ωt − kz − k1z )
 2n 
The wave vector is renormalized:
ω 3χ (3) 2
K = k + k1 =  n + A0 

c 2ε 0 n 
The effective refractive index depends on the intensity of the beam:
 3η0 χ (3) 
n′ = n + n2 I  n2 = 
 ε 

 Propagation in Kerr media
Self-phase modulation (ultrashort pulses)
refractive index is time dependent
phase of the pulse is modulation
creation of new frequency components (bandwidth broadening)
pulse shortening
Self-focusation (intense beams)
Kerr lensing due to spatial profile of the beam