Lecture 1, Part 2

❑ Light propagation in homogenous nonlinear media

❑ Nonlinear response -> Nonlinear optical phenomena

- second-order nonlinearities
- third-order nonlinearities
Linear responce of a medium
❑ General wave equation in a dielectric medium:
1  2
E  2
P
 E − 2 2 = 0 2
2

c t t
❑ Linear approximation:
- P and E is supposed to have a connection:  0 r E =  0 E + P

 P =  0  r ( ) − 1 E =  0  (1) ( )E

i.e. P is a linear function of E; this is described by a (linear) responce

function, (electric) susceptibility:

 (1) ( ) =  r ( ) − 1 = nˆ 2 ( ) − 1
Nonlinear responce of a medium
❑ In general, P is a nonlinear function of E:

(
P (t ) =  0  (1) E(t ) +  (2) E(t ) 2 +  (3) E(t )3 + )
❑ In a component form:
(
Pi =  0  ij(1) E j +  ijk
( 2)
E j Ek +  ijkl
( 3)
E j Ek El +  )
- (n) describes (n)th order nonlinearity
- (n) and P(n) prescribe (n)th order (nonlinear) optical phenomena:

Pi (2) =  0 ijk
(2)
E j Ek 2nd order nonlinear polarization

Pi (3) =  0 ijkl
(3)
E j Ek El 3th order nonlinear polarization
Nonlinear response
In a nonresonant case:
 ( n+1) 1 Eat is electric field by which the atom
 n = 1, 2,3,... binds valence electrons:
 (n) Eat
Eat  1010 Vm −1  1012 Vm −1
In condensed matter  (1)
1 so

 (2)  Eat−1  10−12 mV −1 10−10 mV −1

Similarly

 (3)  Eat−2  10−24 m 2 V −2 10−20 m 2 V −2

Thus, mainly the lowest nonlinearities (2nd and 3rd) are significant.

for nonlinearities high intensity light sources are needed (pulsed) lasers

also, materials having large  ( n) , n = 2,3, , are needed

 The symmetry of (n)
❑ In general (n) is a tensor, which has elements:
 ij(1) ,  ijk
( 2)
and  ( 3)
ijkl

→ These are restricted by the symmetry properties of a medium

❑ Symmetry operation = coordinate transform, that does not

change the properties of a material

- Eg. If S is tensor’s (2) symmetry operation, it holds that:

 ijk
(2)
=  S i S  j S k 
(2)

 ,  ,
 In particular, if S is an inversion transform, then
 0,   i
S i = − i = 
 −1,  = i
 ijk =  ( − i )( −  j )(−  k )  = −  ijk =0 !!
(2) (2) (2)

 ,  ,
 The symmetry of (n)

 In a medium with inversion symmetry, that is, material properties are

not changed in the transform

r→-r (r=xi+yj+zk)
is always (2) = 0 !

▪ Tensors (1) and (3) do not have this limitation !

 in isotropic (bulk) media (many solids and all liquids and gases)
only 3th order (and other odd-order 5th, 7th , …) nonlinearities can
be detected
Potential nonlinear optical effects
Nonlinear optics is what happens when the polarization is the result
of higher-order (nonlinear!) terms in the field:

P =  0   (1) E +  (2) E 2 +  (3) E3 + ...

What are the effects of such nonlinear terms?

Consider the second-order term:

Since E(t )  E exp(it ) + E * exp( −it ),

E (t ) 2  E 2 exp(2it ) + 2 E + E *2 exp(−2it )
2

2 = 2nd harmonic!

Harmonic generation is one of many exotic effects that can arise!

 Sum- and difference-frequency generation
Suppose there are two different-color beams present:

E(t )  E1 exp(i1t ) + E1* exp(−i1t ) + E2 exp(i2t ) + E2* exp(−i2t )

So:

E (t ) 2  E12 exp(2i1t ) + E1*2 exp( −2i1t ) 2nd-harmonic gen

+ E22 exp(2i2t ) + E2*2 exp(−2i2t ) 2nd-harmonic gen
+ 2 E1 E2 exp i (1 + 2 )t  + 2 E1* E2* exp  −i(1 + 2 )t  Sum-freq gen
+ 2 E1 E2* exp i (1 − 2 )t  + 2 E1* E2 exp  −i (1 − 2 )t  Diff-freq gen

+ 2 E1 + 2 E2
2 2
dc rectification

Note also that, when i is negative inside the exp, the E in front has a *.
Complicated nonlinear-optical effects can occur

Nonlinear-optical processes
are often referred to as:

"N-wave-mixing processes"

where N is the number of

Emitted-light photons involved (including
photon energy the emitted one).

The more photons (i.e., the higher the order) the weaker the effect,
however. Very-high-order effects can be seen, but they require
very high irradiance.
Conservation laws for photons in nonlinear optics

Energy must be conserved:

1 + 2 + 3 − 4 + 5 = sig

sig Momentum must also be conserved:

k 1 + k 2 + k 3 − k 4 + k 5 = k sig

k sig Unfortunately, k sig may not correspond

to a light wave at frequency sig!

Satisfying these two relations simultan-

eously is called "phase-matching."
 Conservation laws for photons in SHG

Energy must be conserved:

1 sig

Energy
1 + 1 = sig  sig = 21
1

Momentum must also be conserved:

k 1 + k 1 = k sig sig = 21 k1 k1

1 21
 2 n(1 ) = n(21 ) k sig
c0 c0
To simultaneously conserve energy and momentum:

 n(1 ) = n(21 ) The phase-matching condition for SHG!

 Phase-matching in SHG

The phase-matching condition for SHG:

n( ) = n(2 )

Unfortunately, dispersion prevents this from ever happening!

Refractive
index

 Frequency
2
First Demonstration of Second-Harmonic Generation

P.A. Franken, et al, Physical Review Letters 7, p. 118 (1961)

The second-harmonic beam was very weak because the process

wasn’t phase-matched.
First demonstration of SHG: The Data

The actual published result…

The second harmonic Input beam

Note that the very weak spot due to the second harmonic is missing.
It was removed by an overzealous Physical Review Letters editor,
who thought it was a speck of dirt.
Phase-matching in SHG using birefringence
Birefringent materials have different refractive indices for different
polarizations. “Ordinary” and “Extraordinary” refractive indices can
be different by up to 0.1 for SHG crystals.

Phase-matching condition can

Refractive index
then be satisfied.
ne
Use the extraordinary polarization
for  and the ordinary for 2: no
ne () = no (2)
 Frequency 2

ne depends on propagation angle, so we can tune for a given .

Some crystals have ne < no, so the opposite polarizations work.
 SH light created in real crystals

Far from
phase-matching: SHG crystal

Output beam
Input beam

Closer to
phase-matching: SHG crystal

Output beam
Input beam

Note that SH beam is brighter as phase-matching is achieved.

Difference-Frequency Generation: Optical
Parametric Generation, Amplification, Oscillation
Difference-frequency generation takes many useful forms.

1 1
2 = 3 − 1 "signal"
3
3 2
"idler"

Parametric Down-Conversion Optical Parametric By convention:

(Difference-frequency generation) Generation (OPG) signal > idler

1 1 1
3
3 2 2
mirror mirror
Optical Parametric Optical Parametric
Amplification (OPA) Oscillation (OPO)
DFG example: THz-wave generation

Difference frequency generation

(optical rectification)

Pi ( 2 ) ( =  −  ' ) =  0  ijk
( 2)
E j ( ) Ek* ( ' )

nonlinear (ZnTe) solid

Another 2nd-order process: Electro-optics
Applying a DC (or AC) voltage to a crystal changes its refractive
indices and introduces birefringence. In a sense, this is sum-
frequency generation with a beam of zero (, or AC,) frequency (but
not zero field!).
A few kV can turn a crystal into a half- or quarter-wave plate.

V Polarizer
If V = 0, the pulse
polarization doesn’t
change.
“Pockels cell”
If V = Vp , the pulse
(voltage may be
transverse or polarization switches to its
longitudinal) orthogonal state.

Abruptly switching a Pockels cell allows us to switch a pulse into or out

of a laser.
Example: Detection of THz-waves

”Free-space Electro-Optic Sampling”:

(1) Electro-optic (Pockels) efect

Pi ( 2 ) ( =  '+) =  0  ijk
( 2)
E j ( ' ) Ek ()
In nonlinear (0.5mm (110)-ZnTe) crystal.

(2) Polarization measurement

- polarization change between
two light fields is directly
proportional to E()
How to detect ONE molecular layer of water (  3 Å)?
• Sum-Frequency Generation (SFG) Spectroscopy can be used to
investigate surfaces at one molecular layer level

• SFG provides information about structure and molecular orientation

VIS SFG
IR
 Sum Frequency Generation (SFG)
• Basic principle:

1
 = 1 + 2

2
Pi (2) ( ) =  ijk
(2)
E j (1 ) Ek (2 )
(2) 2 (2) 2
ISFG  Pi  eff I I
1 2

• Note:  (2)
ijk =0 in media with inversion symmetry !
 SFG from a surface
• at surface (~ a monolayer) the symmetry is always broken SFG
1
2
SFG

(2)=0

(2)=0

forbidden in bulk with inversion symm.

 Infrared-visible SFG
• provides vibrational spectrum of surface monolayer
IR
VIS
SFG

(2)=0

(2)=0 v=1

v=0
Third-order nonlinearities:
Four-wave mixing
Third-harmonic
generation
Induced
gratings
Phase
conjugation
Nonlinear
refractive index
Self-focusing
Self-phase
modulation
Continuum
generation
 Third-harmonic THG Medium

generation (THG)  3

We must now cube the input field:

E(r , t ) = E exp[i(t − kz)] + E* exp[−i(t − kz)]

E (r , t ) = E exp[i (3t − 3kz )] + E * exp[ −i (3t − 3kz )]

3 3 3

+ other terms
Third-harmonic generation is weaker than second-harmonic and
sum-frequency generation, so the third harmonic is usually
generated using SHG followed by SFG, rather than by direct THG.
 Noncollinear THG
We can also allow two different input beams, whose frequencies can
be different.
So in addition to generating the third harmonic of each input beam,
the medium will generate interesting sum frequencies.

THG Signal #1
medium

 +
 +

Signal #2

E (r , t )3 = E 2 E exp{i[(2 +  )t − (2k + k )  r )]} +

1 2 1 2 1 2
+ E 2 E exp{i[(2 +  )t − (2k + k )  r )]} +
2 1 2 1 2 1
+ other terms
Third-order difference-frequency generation:
Self-diffraction
Consider some of the difference-frequency terms:

Signal #1
 −
Nonlinear
medium 2k1 − k 2



 −
Signal #2 2k2 − k1

E (r , t ) = E E exp{i[(21 − 2 )t − (2k1 − k2 )  r )]} +

3
1
2 *
2

+ E22 E1* exp{i[(22 − 1 )t − (2k2 − k1 )  r )]} +

+ other terms
 Degenerate four-wave mixing (4WM)
Consider only processes with three input frequencies
and an output frequency that are identical.
Identical frequencies = degenerate.

 = −  + 

Because the k-vectors can have different directions, we’ll distinguish

between them (as well as the fields):

k pol = k1 − k2 + k3
P (3) ( ) =  0  (3) ( =  −  +  ) E1 ( ) E2* ( ) E3 ( )

Degenerate four-wave mixing gives rise to an amazing variety of

interesting effects. Some are desirable. Some are not.
Some are desirable some of the time and not the rest of the time.
Degenerate 4WM gives a nonlinear refractive index
2 E 1 2 E 2 P
Recall the inhomogeneous wave equation: − 2 = 0 2
z 2
c0 t 2
t
and the polarization envelope (the linear and nonlinear terms):
 (1) (3) 
P = 0  E +  E E = 0  +  E  E
2
 (1) (3) 2

   
Substituting the polarization into the wave equation (assuming slow
variation in the envelope of E compared to 1/):
2 E 1 2 E    2
E
− =    + 
(1) (3) 2
E
z 2 c02 t 2
0 0
  t 2
1 +  (1) +  (3) E 2  2
 E
2
   E = 0
− since 0 0 = 1/ c02
z 2 c02 t 2

n = 1+  + 
(1) (3) 2
So the refractive index is: E
 Nonlinear Refractive Index
The refractive index in the presence of linear and nonlinear
polarization:
n = 1 +  (1) +  (3) E
2

Now, the usual refractive index (which we’ll call n0) is: n0 = 1 +  (1)

n = n + = n0 1 + 
2 (3) 2 (3) 2
So: 0 E E / n02

Assume that the nonlinear term << n0 :

n  n0 1 + 12  (3) E / n02   n0 +  (3) E / 2n0

2 2
So:
 

Usually, we define a “nonlinear refractive index”: n2   (3) / 2n0

I E
2
n  n0 + n2 I since
 The nonlinear refractive index magnitude and
response time
A variety of effects give rise to a nonlinear refractive index.
Those that yield a large n2 typically have a slow response.

Thermal effects yield a huge nonlinear refractive index through thermal

expansion due to energy deposition, but they are very very slow.
As a result, most media, including even Chinese tea, have nonlinear
refractive indices!
 Whole-beam self-focusing
The nonlinear refractive index, n = n0 + n2 I, causes beams to self-focus.

If the beam has a spatial Gaussian intensity profile, then any nonlinear
medium will have a spatial refractive index profile that is also Gaussian:
2 2
n = n0 + n2 I 0 exp(−2r / w0 )
2 2
Near beam center:  n0 + n2 I0 (1 − 2r /w0 )

The phase delay vs. radial co-ordinate will be:

 (r ) = n k0 L  n0 k0 L + n2 k0 L I 0 (1 − 2r 2 / w02 )
 (r )  constant − 2n2 k0 L I 0 (r 2 / w02 )
This is precisely the behavior of a lens!
But one whose focal power scales with the intensity.
Whole-beam self-focusing
 Small-scale self-focusing
If the beam has variations in intensity across its profile, it undergoes
small-scale self-focusing.

Intensity
Each tiny bump in the beam undergoes
its own separate self-focusing,
yielding a tightly focused spot inside
the beam, called a “filament.”

Position

Such filaments grow exponentially with distance.

And they grow from quantum noise in the beam, which is always there.

As a result, an intense ultrashort pulse cannot propagate through any medium

without degenerating into a mass of tiny highly intense filaments,
which, even worse, badly damage the medium.
 Small-scale self-focusing vs. distance
A somewhat noisy beam becomes a very noisy one.
 Phase conjugation
When a nonlinear-optical effect produces a light wave proportional to E*,
the process is called a phase-conjugation process. Phase conjugators can
cancel out aberrations.

exp ikz 
Distorting exp ikz − i ( x, y )
medium
 ( x, y )
A normal mirror leaves
the sign of the phase
unchanged

exp i ( −k ) z − 2i ( x, y )  exp i ( −k ) z − i ( x, y ) 

A phase-conjugate
mirror reverses the
sign of the phase

exp[i ( −k ) z + i ( x, y ) − i ( x, y )] exp i ( −k ) z + i ( x, y ) 

The second traversal through the medium cancels

out the phase distortion caused by the first pass!
 Self-Phase Modulation & Continuum Generation
The self-modulation develops a phase vs. time proportional to the input pulse
intensity vs. time.

Esig ( z , t ) = Esig (0, t ) exp i n k z  = Esig (0, t ) exp i [n0 + n2 I (t )]k z

 Esig (0, t ) exp in2 k I (t ) z 

Pulse Intensity vs. time The further the pulse
travels, the more
modulation occurs.
That is:  ( z, t ) = n2 k z I (t )

A flat phase vs. time yields the narrowest spectrum. If we assume the pulse
starts with a flat phase, then SPM broadens the spectrum.

This is not a small effect! A total phase variation of hundreds can occur! A broad
spectrum generated in this manner is called a continuum.
Experimental Continuum
spectrum in a fiber
Continua created by Low
propagating 500-fs 625- Energy
nm pulses through 30 cm
of single-mode fiber.

Medium
Energy
Broadest spectrum
occurs for highest
energy
supercontinuum High
Energy
UV Continuum in Air!
308 nm input pulse; weak focusing with a 1-m lens.

The Supercontinuum
Laser Source
 The continuum from
microstructure optical
fiber is ultrabroadband

Cross section of the

microstructure fiber.

The spectrum extends

from ~400 to ~1500 nm
and is relatively flat (when
averaged over time).

This continuum was created using unamplified Ti:Sapphire pulses.

J.K. Ranka, R.S. Windeler, and A.J. Stentz, Opt. Lett. Vol. 25, pp. 25-27, 2000