Linear optics vs nonlinear optics

• Linear Optics- Optics of weak light:

Light is deflected or delayed but its frequency is unchanged.
Superposition principle holds
• Nonlinear optics-Optics of intense light:
We are concerned with the effects that light itself induces as it
propagates through the medium.
Superposition principle not valid
LASER generate coherent radiation at different
wavelength (meter wavelength to soft x-ray
region)
But not possible to produce light that covers all
wavelength of interest even though variety of
active materials are available to produce lasers
Necessary to transform frequency of light
generated by laser into desired frequency
Nonlinear process such as: Harmonic generation,
Sum and different frequency generation,
Parametric Oscillations can generate new
frequency
 Nonlinear optics

• Nonlinear optics (NLO) is the branch of optics that describes

the behaviour of light in nonlinear media, that is, media in
which the polarization density P responds non-linearly to the
electric filed E of the light.

• The non-linearity is typically observed only at very high light

intensities ( typically 108 V/m) such as those provided by lasers.
 Second-harmonic generation

Second-harmonic generation (SHG, also called frequency

doubling) is a non linear optical process in which two photons with the
same frequency interact with a nonlinear material, are "combined", and
generate a new photon with twice the energy of the initial photons, that
conserves the coherence of the excitation.

It is a special case of sum-frequency generation (2 photons), and more

generally of harmonic generation.
a) Geometry of SHG and b) Energy level scheme of SHG process
The polarization in response to the field strength can be expressed as

are known as second and third order nonlinear optical

susceptibilities

tion.
The electric field of a laser beam can be written as
It is seen that the second order polarization of consists of a contribution
at zero frequency (the first term) and a contribution at frequency 2ω (the
second term).
The later contribution can lead to the generation of radiation of second –
harmonic frequency.
The first contribution in above equation does not lead to the generation of
electromagnetic radiation (second time derivative vanishes), consequently
optical rectification occurs in which a static electric filed is created across
the nonlinear crystal
Second-harmonic generation process
 Use of Second harmonic generation

Frequency doubling
•Second-harmonic generation is used by the laser industry to make green 532 nm lasers
from a 1064 nm Nd:YAG laser source.
Ultra-short pulse measurement
Characterizing an ultrashort pulse cannot be done directly with electronics only, as the time-
scale is below 1ps ( 10-12 sec) . SHG has the advantage of mixing two input fields to generate
the harmonic one, to perform such a pulse measurement.

Second-harmonic generation microscopy

In biological and medical science, the effect of second-harmonic generation is used for high-
resolution optical microscopy. Because of the non-zero second-harmonic coefficient, only
non-centrosymmetric structures are capable of emitting SHG light.
Characterization of crystalline materials
Second harmonic generation is also relevant to characterize organic or inorganic crystals since
is one of the most discriminant and rapid technique to detect non centrosymmetry
 Optical parametric oscillator

An optical parametric oscillator (OPO) is a parametric oscillator that

oscillates at optical frequencies. It converts an input laser wave (called
"pump") with frequency ωp into two output waves of lower frequency (ωs, ωi )
by means of second-order nonlinear optical interaction.
The sum of the output waves' frequencies is equal to the input wave
frequency: ωs+ ωi= ωp. the two output waves are called "signal" and "idler",
where the output wave with higher frequency is the "signal".

A special case is the degenerate OPO, when the output frequency is one-half
the pump frequency, ωp, which can result in half harmonic generation when
signal and idler have the same polarization.

Optical parametric oscillators are used as coherent light sources for various
scientific purposes, and to generate squeezed light for quantum mechanics
research.
 Sum and difference frequency generation

Optical field of two distinct frequency components incident upon a second order
nonlinear medium

We know the second order contribution to the nonlinear polarisation

The nonlinear polarization is then

e
h
T
 Sum and difference frequency generation

The complex amplitudes of frequency components of nonlinear polarization hence are

Second harmonic generation

Second harmonic generation

Sum frequency generation

Difference frequency generation

(OR) Optical rectification

 Sum frequency generation
The nonlinear polarization for sum frequency generation is given by

a) Geometry and b) energy level of sum frequency generation

produce tunable radiation in the ultraviolet region

 Difference frequency generation
The nonlinear polarization for difference frequency generation is given by

a) Geometry and b) energy level of diffrence frequency generation

produce tunable radiation in the visible region

 Phase matching

Many phase-sensitive nonlinear processes, in particular parametric processes such as

frequency doubling, sum and difference frequency generation, parametric amplification
and oscillation, and also four-wave mixing, require phase matching to be efficient.

Essentially, this means ensuring that a proper phase relationship between the interacting
waves is maintained along the propagation direction.

Only if that condition is fulfilled, amplitude contributions from different locations to the
product wave are all in phase at the end of the nonlinear crystal.

In other words, some phase mismatch should be close to zero in order to obtain an
effective nonlinear interaction.
For example, phase matching of frequency doubling with collinear beams the
phase mismatch is given by

where k1 and k2 are the wavenumbers of the fundamental and second-harmonic

beam, respectively. Without chromatic dispersion, k2 = 2 k1 would hold, so that
the phase mismatch vanishes. However, dispersion generally causes a non-zero
phase mismatch (Figure 1) if no special measures are taken to avoid
this.

Figure 1: Phase mismatch for second-harmonic generation. Due to chromatic dispersion, the
wavenumber of the second harmonic is more than twice as large as that for the
fundamental wave. This can be avoided, e.g., by choosing a different polarization in a
birefringent crystal.
Only with phase matching, a high conversion efficiency can be achieved
Otherwise, the direction of energy transfer changes periodically according
to the change in the phase relation between the interacting waves. The
energy then oscillates between the waves rather than being transferred in
a constant direction.

Figure 2: Addition of amplitude contributions from different parts of the crystal.

 Nonlinear absorption
In nonlinear process the absorption coefficient depends on the optical intensity
(radiant flux). In some cases, there is only nonlinear absorption and no linear
absorption: the absorption coefficient vanishes for vanishing intensities. In other
cases, there is absorption at low intensities, but the absorption coefficient rises or is
reduced for higher intensities. The latter case (with reduced absorption coefficients
for rising intensities) is called saturable absorption.
A typical nonlinear absorption process is two-photon absorption (TPA). Here, the
energies of two photons are combined to excite a single electron into a higher state –
e.g. above the band gap of a semiconductor. Thus, there can be absorption (at high
enough intensities) even when the energy of a single photon is insufficient for getting
across the band gap. The effective absorption coefficient is proportional to the optical
intensity.
Similarly, there are multiphoton absorption processes involving more than two
photons per process. These are relevant, for example, for laser material processing in
transparent media such as glasses. The deposition of laser energy is possible only
with high peak powers as can be reached in short or ultrashort pulses of light.
 Two-photon absorption (TPA)

Two-photon absorption (TPA) is the absorption of two photons of identical

or different frequencies in order to excite a molecule from ground state to a
higher excited state. The energy difference between the involved lower and
upper states of the molecule is equal to the sum of the photon energies of the
two photons absorbed. Two-photon absorption is a third-order process, typically
several orders of magnitude weaker than linear absorption low light intensities.

It differs from linear absorption in that the optical

transition rate due to TPA depends on the square
of the light intensity, thus it is a nonlinear optical
process, and can dominate over linear absorption
at high intensities.
 z-scan technique

Z-scan is a simple experimental technique to measure intensity dependent nonlinear susceptibilities of

third-order nonlinear optical materials.

In the experiment, a Ti:sapphire ( = 800 nm) laser with a pulse duration of 100 fs was applied at
a pulse repetition rate of 100 Hz.

The intensity profile of the laser beam was confirmed to be a Gaussian distribution.

Initially, a glass cuvette of 1 mm thickness was filled with colloidal solution of alloy nanoparticles
and placed on a uniaxial stage.

A collimated Ti:sapphire laser beam was focused by a lens with desired focal length.

A sample was then moved along the beam axis around the focal area to observe the change in
intensity of the transmitted beam.
The experimental setup for the z-scan measurement is shown in Figure below
The nonlinear absorption coeecient can be calculated from the normalized transmittance, T(z), for OA z-scan
experiment that can be expressed by

 −q0 ( z , 0 ) 
m



T (z) = ,
m =0
( m + 1) 2
3
Where
q0 ( z , 0 ) =  I 0 Leff ( 1 + z 2 z0 2 )
I 0 = 2 Pin 0 2 is the peak intensity at the focus of z-scan experiment and
(
Leff = 1 − e − 0 L ) 0
is the effective thickness of the sample deduced by

,
Here, L is the sample length, z is the position of a sample and z0 is the Rayleigh length of the
beam. The nonlinear absorption coefficient β is obtained by fitting the experimental data
with ist equation
 Nonlinear absorption
Nonlinear light absorption is a basic phenomenon of the interaction between the
light and the matter.
Saturable absorption

Saturable absorption is a property of materials

where the absorption of light decreases with
increasing light intensity.

Reverse saturable absorption

A class of nonlinear absorbers in which the excited
state absorption is large compared to the ground state
absorption can undergo a process called reverse
saturable absorption (RSA), also known as reversible
saturable absorption.

Open aperture scheme

 nonlinear refraction
When an intense laser beam passes through a material, the electric field of the beam can induce a
change in the refractive index of the material that is proportional to the intensity of the beam.
This nonlinear effect is called the Kerr effect.

The total refractive index of the material is the sum of the

refractive index, n 0 , with no laser beam present and the
term n 2 I, where n 2 is the second-order nonlinear refractive
index and I is the intensity of the beam.
n = n0 + n 2 I

The change in refractive index can be positive or negative.

Values of n 2 are generally small (e.g. approximately 3 x 10-
16 cm2 W-1 for silica), so that high beam intensities are

required to have a significant effect.

Closed aperture scheme

To calculate a nonlinear refractive index, the normalized transmittance for the CA z-scan experiment T(z) was fitted
to the following equation ,

T ( z) = 1+
4x
 −
(
4 x2 + 3 ) 
(x 2
)(
+ 9 x +1
2
) (x
,
where
2
)(
+ 9 (2)x + 1
2
)
where x=z/z0 is the relative position from the beam waist, andΔΦand ΔΨare the nonlinear
phase shifts due to nonlinear refraction and absorption related with

 = k  I 0 Leff  =  I 0 Leff , 2 (3)

( ) ( ) 
12
 2 2
The absolute value of third order nonlinear refractive index is calculated by  ( 3) =  Re  ( 3) + Im  ( )
3

where
 0 c 2 n02  0 c 2 n02 
Re  (esu) = 10
(3) −4
 c  r(3) cm2 W-1 ), Im  (esu) = 10
(3) −2
cm2 W-1 ),
 4 2
c is the velocity of light in vacuum and ε0 is the vacuum permittivity.
The values of third order nonlinear susceptibility are shown in Table

estimated sample
parameters Rh–Pd Rh–Pt
β (10-12 cm/W) 1.63 4.39
γ (10-16 cm2/W) 1.10 1.17
Reχ(3) (10-12 esu) 1.51 1.61
Imχ(3) (10-11 esu) 1.43 3.85
χ(3) (10-11 esu) 1.44 3.85