Lectures 9-10: Nonlinear optical phenomena

Second-order effects
Third-order effects

Second harmonic generation

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+ 1 Ray and wave optics
+ 2 Light beams and beam optics
+ 3 Optical resonators
+ 4 Photon optics
+ 5 Optical gain
+ 6 Laser oscillation
+ 7 Pulsed lasers
+ 8 Electromagnetic optics and crystal optics
+ 9 Second-order nonlinear optical effects
+ 10 Third-order nonlinear optical effects
11 Electro-optics
12 Acousto-optics
13 Ultrafast optics
14 Laser spectroscopy and microscopy
15 Laser fabrication and materials processing
2
Linear versus non-linear optics
Linear: optics of low-intensity light
★ Intensity of the optical field I=|E|2 is much lower than electric field inside
the atom
★ Optical properties of material are independent of light intensity
★ The principle of superposition is valid: two waves crossing the same
medium do not interact
★ Light can be absorbed, deflected, or delayed, but its frequency is
unchanged

Non-linear: optics of high-intensity light

★ Intensity of the optical field is comparable with atomic field
★ Light can modify optical properties of the medium
★ The principle of superposition is violated: two beams crossing the same
medium can interact with each other
★ Frequency of light can be changed 3
Atomic polarization (分極) by external field
Atomic field (nucleus-electron cloud) Atom in an external DC field
field strength Eat ~ 108 V/m
E
- -
-
- -
+

+ ++
+ +
+
- -
-

displacement 変位

charge displacement and dipole moment P(E)

Q+ Q-
x(E)
displacement 変位

4
Similar model also applies to external AC field at optical frequency
Non-linear polarization
Optical nonlinearity can be introduced by assuming that dielectric susceptibility
is no longer a constant, but depends on the external field:

This dependence can be also represented by using Taylor series expansion

around field zero field (different symbol for field is used in the equations below))
linear term non-linear terms

2nd order 3rd order

In optics we commonly use:

2nd order NL 3rd order NL

susceptibility susceptibility

Nonlinearities can be classified by their order 5

Parametric nonlinearities
Polarization depends on average charge density and displacement:

✦ Carriers oscillate in the AC field of the incident optical wave

✦ Their displacement x(E) is non-linear function of the electric field
+ + +
U

= charge
oscillation in
x
non-linear
potential U

+
0 x

✦ Non-linear polarization can produce interactions with other optical waves

or waves with new frequencies, but its energy is fully re-radiated into the
environment and no energy is deposited in the material (example: optical
harmonics generation) 6
Non-parametric nonlinearities
Polarization also depends on average charge density and displacement:

✦ Carriers oscillate in the AC field of the incident optical wave

✦ Their number is non-linear function of the electric field
✦ Polarization can produce interactions with other optical waves or waves
with new frequencies, and part of its energy is deposited in the material

saturated absorption two-photon absorption

(SA) (TPA)

SA E2
half
absorption coefficient

E2 const.
occupied
TPA virtual state
~I2
half
E1
empty intensity E1
7
Second-order nonlinearities
Non-linear polarization is proportional to the square of field:
Harmonic time variation can be expressed as:
complex conjugate

We obtain DC component and doubled-frequency component:

optical second harmonic

rectification generation (SHG)

8
Non-linearity and lattice symmetry
centro-symmetric medium non-centrosymmetric medium
E E(t) E
U t
U

+ P(t)
x +
0 x t
0
E(t)
E(t)
PNL (t)
t

t t
P(t)

t PNL(t)
P(t)

PNL(t) tt

t
PNL(t)in centro-symmetric media

PNL(t)
t
t
non-centro-symmetric crystals are
needed for 2nd order non-linearities 9
P (t)
 Three-Wave Mixing (TWM)
Field E(t) comprising two harmonic components with frequencies ω1 and ω2:

The nonlinear polarization contains components at five frequencies

(exponential factors containing frequency are omitted):
0:
2ω1:
SHG
2ω2:
ω+=ω1 + ω2: sum-frequency generation (SFG)
ω-=ω1 - ω2: frequency down-conversion (FDC)

It is possible to mix two waves in a non-linear medium and generate a third wave at
sum or difference frequency. This process is called three-wave mixing (TWM).
10
Frequency and phase matching
As an example, we can examine the case of SFG in more detail. If two fields are plane waves,
they can be expressed as:

Non-linear polarization can be also expressed as harmonic plane wave

3
Non-linear polarization can be regarded as a radiation source which produces the third wave:

Field of the third momentum conservation law energy conservation law

wave (phase-matching condition) (frequency-matching condition)

These conditions ensure that temporal and spatial phase of the three waves is the same
(phase matching condition). The sum frequency wave will have maximum amplitude PNL
This requirement is universal. Similar relations can be deduced for the SHG and FDC cases. 11
Interpretation of matching conditions
Wave optics-based
wa
ve
1

wave 3

ave 2
w

Photon optics-based

virtual level virtual level

SFG FDC

12
Collinear and non-collinear TWM

✦ In collinear process all interacting waves

propagate along the same direction and overlap
in their entire path. Interaction length is
determined by the crystal thickness and k-vector
matching.
✦ In non-collinear process interacting waves
propagate along different directions and overlap
only partially. Interaction length is determined by
the length of overlap and matching of k-vector
components along the optical axis.

13
Spatial phase mismatch
We focus on the case of collinear TWM (all waves propagate in the same direction)

Assuming strict frequency matching, non-linear polarization that creates the third wave is expressed as:

We define phase mismatch as:

Then, non-linear polarization (~amplitude of the third wave) can be expressed as:

If we consider three waves propagating and interacting over a finite length L, intensity of the third wave
can be expressed by integrating the above expression:
“sine cardinal” or
integral of oscillating “sampling” f function
harmonic function

Similar result can be obtained also for frequency mismatch, since total phase is ~ (ωt-kz) and roles of
time- and space-dependent phases are equal 14
Tolerable spatial phase mismatch wave-mixing coherence
length in the presence of
phase mismatch or wave-
sinc function has a narrow peak around zero mixing coherence length

sinc(x)

shows interaction
length over which
intensity of the third
wave drops to zero

Efficiency of parametric processes is limited by the tolerable phase mismatch. For example, in
SHG (ω1 = ω2, ω3 = 2ω1) one has to take into account dispersion of the refractive index, which
naturally has different values at the fundamental ( n1) and second-harmonic (n3)
wavelengths. In this case:
Δk = 2(2π/ λ0)|n3-n1|, and Lc = λ0/2(|n3-n1|). For |n3-n1| ≈ 10-2, Lc ≈ 50λ0.
—> Phase matching with large Lc must be ensured in SHG or other parametric processes 15
Dispersive phase mismatch
In collinear TWM three waves travel in the same direction. If they propagate with the same
speed, their phase matching is automatically ensured over infinite propagation length.
However, speed of light (or refractive index) is frequency-dependent due to dispersion.
Phase matching condition for TWM becomes:

Let us consider SGH process as an example. In this case the requirement of Δk =0 (or k3=2k1),
leads to the condition of n2ω = nω. However, dispersion leads to the following situation:

n2ω
n2ω ≠nω
nω

ω 2ω
In these conditions it is impossible to achieve phase matching. This problem is solved by
using anisotropic optical crystals, in which refractive index depends on the propagation
direction, and it is possible to satisfy the condition n2ω = nω along some directions in the
crystal. 16
 Important points

❖ Main differences between linear and non-linear optics;

❖ Types of optical nonlinearities (2nd-, 3rd-order, parametric, non-
parametric);
❖ Three-wave mixing and its basic features;
❖ Frequency and phase-matching conditions;
❖ Phase mismatch and its importance for non-linear optical
processes.
Anisotropic materials Propagation x3 (or z)

Mechanical model of a uniaxial along the Ez=0

optical axis
material (atom) Exy

x3 (or z) optical axis x2 (or y)

x1 (or x)
Ex,y incident wave

(o) Ordinary wave polarized in xy plane, same

refractive index no for any orientation of polarization
nucleus

x3 (or z)
x2 (or y)
Propagation at an
angle with the Ez
x1 (or x)
optical axis

Stiffness constant of the springs define Exy

refractive index of the material: x2 (or y)
x1 (or x)
cx = cy 6= cz nx = ny 6= nz Ex,y incident wave
(o) Same as above;
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Resonant frequencies: (e) Extraordinary wave polarized along z-axis direction

q p refractive index ne depends on the incidence angle
!0xy = cxy /me !0z = cz /me
18
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Double-refraction (birefringence)
Two orthogonally linearly polarized output waves
(normal modes) which have different phase velocities
(or feel different values of refractive index)
Unpolarized
input wave
ordinary wave
n o

extraordinary
wave ne
optical axis

Refractive index ellipsoid for a single-axis (uniaxial) crystal

P
incidence
nx = ny = no nx direction ne(θ)
E E
optical nz = ne
P
axis optical axis
ny z no z

wave propagation direction OP parallel tilted propagation = o(no) E|| y and e(ne) E||z
to optical axis = o(no) wave only orthogonally linearly polarized waves 19
Light propagation in birefringent materials (EN)

20
Light propagation in birefringent materials (JP)

21
 Critical phase matching in SHG
SHG is a degenerate three-wave mixing (ω1 = ω2= ω )

n(2ω)=n(ω) = phase matching At the phase matching angle, refractive

index for sum (second-harmonic)
frequency is equal to that for the
fundamental wave

two e-waves are combined to

produce one o-wave (ee-o process)

★ Type I mixing: oo-e or ee-o

NL crystal is cut at an angle ★ Type II mixing: oe-e or eo-o
crystal
which ensures that (external)
normal incidence corresponds
to (internal) phase matching
angle 22
 Phase matching angular range
Direction-dependent and frequency-dependent
extraordinary refractive index n(θ,ω):

If we allow small angular deviation from the

matching angle θm, what will
be the effect on the SHG efficiency?

Refractive index change Δn corresponding to Δθ:

From this, we can express spatial phase mismatch simply as

, where

SHG intensity drops sharply

when angle deviates from θm. Therefore the name
“critical phase matching” 23
 Quasi-phase matching (QPM)
Some materials have high nonlinear susceptibility d, but their anisotropy in insufficient for
critical phase matching by angular tuning. In such cases QPM approach can be used. Phase is
compensated by using a medium with periodically modulated sign of nonlinear coefficient d.

Periodically-Polled Lithium Niobate (PPLN) crystals

The process of building a periodic modulation into originally uniform crystals is called polling.
There are several polling methods. Lithium niobate (LiNbO3) crystals are ferroelectric (i.e.,
exhibit electric polarization in the absence of external field). Feroellectric polarisation and
sign of d can be periodically reoriented by application of periodically-modulated high-voltage
DC field to the side faces of the crystal using periodic comb-like electrodes.

periodically-poled poling:
medium altering the sign (+-)

alternating sign of
non-linearity
24
 QPM condition
Assuming that nonlinear susceptibility is a periodic harmonic function of coordinate

Intensity of the SFG or SHG waves can be obtained by putting the d(z) under integral

length=integral number of
periods leads to sinc function

sinc() function and I3 will be maximised when argument of the exponential function = 0:

grating period = coherence length

Generally, d(z) is not harmonic but rectangular function of coordinate. In such a case d(z)
can be represented by Fourier series (sum of harmonic functions) and QPM conditions
derived for these harmonics.

25
Non-linear optical crystals
• High magnitude of the nonlinear coefficient
• Dispersion and birefringence suitable for phase matching
• High optical transparency for all wavelengths involved
• Possibility of periodicity poling to achieve QPM
• Resistance against optical damage by intense laser radiation

26
 SHG in practice: laser pointer
Diode-pumped solid-state (DPSS) laser module

laser output
~ 5mW

SHG

27
 SHG in practice: pump laser for femtosecond
Ti:sapphire laser
Green output
~ 10 W
532 nm SHG

pump 2
808 nm

pump1
808 nm

28
 Third-order nonlinearities
In media possessing centrosymmetry, the second-order
nonlinear term is absent since the polarization must
reverse exactly when the electric field is reversed
(hence, d = 0).

The dominant nonlinearity is then of third order and the

material is called Kerr medium

Third-harmonic generation (THG)

By substituting optical field into one can see that Kerr media responds to
optical fields by generating third harmonics and sums and differences of triplets of frequencies.

Optical Kerr effect

THG

However, efficiency of THG is low and rarely used in practice. For this purpose usually second-
order processes are used (SHG followed by SFG between fundamental and second-harmonic
waves) 29
 not to be confused with
Optical Kerr effect electro-optical Kerr effect!

The polarization component at frequency ω corresponds to an incremental change

of the susceptibility Δχ at frequency ω: dielectric impermeability

Since , by differentiating we get , and

Optical Kerr effect

(non-linear refraction)

Optical Kerr effect: refractive index depends on the wave’s intensity

where Optical Kerr Coefficient is (non-linear refraction)

n2 = 10-16 - 10-8 [cm2/W]
It is similar to Electro-Optic Kerr effect (dependence of n on applied external DC field ) 30
 Self-phase modulation (SPM)
As a result of the optical Kerr effect, an optical wave traveling in a third-order nonlinear
medium undergoes an additional phase shift. Optical beam of power P and cross-
sectional area A, traveling a distance L in the medium will acquire phase shift

with Kerr effect contribution expressed as

SPM is useful in applications where light controls light ( for example, intense wave can
induce phase shift of a weak wave, leading to transmission modulation in
interferometers)

31
 Self-focusing (SF)
If an intense optical beam is transmitted through a thin sheet of nonlinear material
exhibiting the optical Kerr effect, the refractive-index change mimics the intensity
pattern in the transverse plane. If the beam has its highest intensity at the center,
the maximum change of the refractive index is also at the center. The sheet then acts
as a graded-index medium that induces nonuniform phase shift, thereby causing
wavefront curvature. Under certain conditions the medium can act as a lens with a
power-dependent focal length. Kerr-lens focusing is useful for laser mode locking.

Self-focusing Kerr-lens mode locking

Related topic: spatial solitons (self-guided beams that due to nonlinearity

neither focus nor diverge during propagation) 32
 Four-wave mixing (FWM) in third-order nonlinear media
In a third-order non-linear media three input waves can be coupled via nonlinearity to produce a third
output wave
Three input waves with frequencies ω1, ω1, and ω3 lead to the total field of

Or , where ω-q = - ωq , negative values of q correspond to c.c. terms

We substitute the field to find non-linear polarization which leads to a sum of 63 = 216
terms

Non-linear polarization is the sum of harmonic components whose frequencies are ω1, …, 3ω1, 2ω1 ± ω2,…,
± ω1, ± ω2, ± ω3, and amplitudes determined by adding appropriate permutations of indices q, r, l.

For example, amplitude of non-linear polarization PNL (ω1 + ω2 - ω3) involves six permutations:

33
 Frequency and phase-matching in FWM
This expression also suggests relationship between the frequencies of the participating waves. From

ω4

one can see that This is frequency-matching condition.

Assuming that waves 1,2,3 are plane waves with correspondingly indexed wave vectors

k4
The fourth wave should be also a plane wave and its wave-vector should satisfy the requirement

This is phase-matching condition.

Several FWM processes occur simultaneously, all satisfying the frequency and phase-matching.
In a photon-based interpretation FWM process can be represented as shown below

34
 Degenerate FWM and phase conjugation
When frequencies of all waves are identical
FWM process is called Degenerate Four-Wave Mixing (DFWM).
Assuming that two of the waves (waves 3 and 4) are uniform plane waves traveling in
opposite directions ,

Polarization density of wave 2 can be then expressed as

Since A3 and A4 are constants, wave 2 emitted by nonlinear polarization will have complex
amplitude complex-conjugate compared to that of wave 1:

The non-linear medium acts as a phase conjugator.

Waves 3 and 4 are called the pump, waves 1 and 2 are called the probe and conjugate
waves, respectively. The conjugate wave is identical to the probe wave except
that it travels in the opposite direction. The phase conjugator is a special mirror that
reflects the wave back onto itself without altering its wavefront.
35
 Phase conjugation and time reversal

36
 FWM and holography (grating recording)
The two counter-propagating
pump waves record a thick
(Bragg) diffraction grating
(permanent or transient).
The probe wave is diffracted
on the grating, the diffracted
probe (the fourth wave) is a
conjugate copy of the probe

If the wavefront of an optical beam is distorted

by a random medium, the original wave can be
restored by use of a conjugator that reflects
the beam onto itself and transmits it once
more through the same medium. This
phenomenon can be exploited in optical
resonators.
37
Two-photon absorption (TPA) Non-parametric
nonlinearity
Polarization depends on average
charge density and displacement:

E2

absorption probability
virtual state

intensity
E1

Probabilities for single-photon and two-photon absorption process:

Ratio p(2p)/p(1p) is very low for intensities I << 10GW/cm2 in best two-photon absorbers (typically
organic molecules), but may become large at higher instantaneous/local intensities obtainable
with pulsed l lasers/tightly focused beams. As a consequence, transparent materials become
strong absorbers. TPA is widely used in laser microscopy and laser fabrication. 38
 Saturated absorption Non-parametric nonlinearity

Polarization depends on average charge density and displacement:

E2, N2

E1, N1

Expression of photon flux via rate equation:

stim. em stim. abs population difference

Stimulated transition probability:

absorption coefficient
stim. em α = γ =0 stim. abs

intensity
39
gain and absorption vanish (or saturate) when N —> 0, leading to optical nonlinearity
 Important points

❖Critical phase matching

❖Main differences second-order and third-order optical
nonlinearities (role of material symmetry, intensity
dependencies);
❖ Optical Kerr effect and its consequences;
❖ Four-wave mixing and phase conjugation;
❖ TPA and saturated absorption.