Chapter 2 :

Fundamentals of
non linear optics

Objectives of the chapter :

1) introduction to the basis of NLO from a

macroscopic point of view

2) non linear susceptibility tensor

It began 60 years ago with…

T.H. Maiman, Nature (1960) P.A. Franken, A.E. Hill, C.W. Peters and G. Weireich, Phys. Rev. Lett. (1961)
Founding principles

« classical » optics  linear constitutive equations

with

Tensor of rank 2 represented by a 3x3 matrix

>> linear relationship but doesn’t mean that always parallel to

Valid only if is weak enough to have linear relationships between the

elements of and , and independant of

Invalid if is too strong at microscopic scale inside the medium

® example of laser light or high local fields densities

in integrated optical structures or optical fibers
 ® the relationship between is much more complex

® semi-quantic calculation from density matrix [ref Bloembergen]

® successive approximations
® polynomial representation with successive powers of [ref Boyd]

Static polarisation
Exists only in rare
ferroelectric materials 3rd order polarization

1st order polarization 2nd order polarization

Linear response Non linear responses

Linear susceptibility Non linear susceptibilities , , …

Tensor of rank 2 Tensors of rank 3, 4, …
 A similar relationship could be written for the dipole moment at the
microscopic scale
local fields

µ j  µ
j   
ji iE +  ( 2)

jik i k .E   
jikl .E i .E k .E l  ...

2nd and 3rd order

Dipole moment of a microscopic element
microscopic
(crystal unit, atom, molecule, …)
Linear polarisability hyperpolarisabilities

® optimizing the microscopic structure to enhance b or g is necessary to optimize

the NL properties of a material

® at any order it is necessary to have a molecular or crystallographic arrangement

or a crystallographic symmetry group which shows only a few non zero tensor
moduli at macroscopic scale
It follows, for a non ferroelectric material :

® a linear response :

® and non linear effects :

Þ new constitutive equation for :

similar to new and specific to non

linear case linear interaction

® Non linear susceptibilities description is not easy and requires algebra of tensors

® Indeed, if a tensor of rank 2 (linear case) could be represented as a « simple » 3x3 matrix
in a 3D space, the number of elements is 9=32

® This number increases to 27=33 or 81=34 for a tensor of rank 3 or 4

Nevertheless, several considerations allow to reduce the number of significant parameters.

(see chapter 3-1)
Furthermore, the semi-quantic calculation shows that each order n of the electric field oscillates
at the frequency :

which results from the interaction between n fields at the pulsations that exist in the medium

The n fields do not necessarily exist at the input

but could result from the non linear effects (see later)

Þ In case of a finite number of frequencies in the medium, the fields and polarization could be
described by their associated Fourier series :

Fourier series

idem
 It follows, for any single spectral modulus :

Linear response PL

Non linear response PNL

® The non linear susceptibilities and polarization

mix all the pulsations up together

® This is a main difference with linear optics and

Notes : « classical » electromagnetism which suppose
1 - spatial terms are implied in order to make it easier
that waves at differents pulsations never
= (idem for E and c )
interfere
2 - summation over the repeated indexes is implied
For each pulsation wl existing in the medium, it can be written a set of Maxwell’s equations
for the Fourier moduli :

And the following propagation equation:

mix up all the co-existing wave

in interaction into the medium

plays the role of an electric field source

and brings out new fields and new phenomena
(depending on the experimental conditions)
 Note that in the previous relationships:

® The successive orders of polarization decrease in magnitude

® Depending on the medium and the experimental conditions, the

probability to observe simultaneously second order and third order
non linear effects is very weak

® We will see further that the emergence of a second order or a third

order interaction requires specific characterstics of the medium
which can not exist simultaneously in the same medium
Main NL phenomena

Order Phenomena Applications

1 (linear) refraction Wave guides, optical fibres
Optical wave mixers,
w1 ± w2  w3 (3 waves mixing) Optical parametric oscillation,
Parametric amplification,
Brillouin scattering
 2
w + w  2w Frequency doubling

w + 0  w (Pockels effect) Electrooptic modulator

w1 + w2 + w3  w4 (4 waves mixing) Raman spectroscopy

w + w + w  3w 3rd harmonic generation
Optical bistability
w + w - w  w (Kerr effect) Amplification, logical gates
3 
Real time holography

Phase conjugaison mirrors

Ultra fast optical gates, Solitons