Frequency Doubling and Second Order Nonlinear Optics

Paul M. Petersen DTU Fotonik, Ris campus Technical University of Denmark, Denmark
(email: paul.michael.petersen@risoe.dk)

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Outline of the talk

The first observation of second harmonic generation Nonlinear optical effects in solids The nonlinear wave equation (formulation of the interaction in nonlinear materials) Second order nonlinear optics Contracted notation for the second order susceptibility Three wave mixing Frequency doubling Phase matching in materials with birefringence

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The first observation of second harmonic generation

Second harmonic generation (SHG) was first demonstrated by P. A. Franken et al. at the University of Michigan in 1961. They focused a ruby laser with a wavelength of 694 nm into a quartz sample. They sent the output light through a spectrometer and recording the spectrum on photographic paper, which indicated the production of light at 347 nm. (Note that the SHG spot does not appear in the publication!)

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Conversion of red lasers into blue lasers

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Generation of new waves in a nonlinear medium

Light interacts with the nonlinear medium. The incident beams are modified and new beams are generated.

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Optical Polarisation induced in Solids

The optical electrical field induces electrical dipole moments in the nonlinear material. The induced dipoles modify the incident beam and for strong optical fields leads to the generation of new k-vectors and new frequencies.
The optical field vector

P is the dipole moment per unit volume. The induced dipoles represents accelerating charged particles that radiates electromagnetic radiation perpendicular to the acceleration vector.

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Second Order Nonlinear Polarization

The relation between the induced optical polarisation in the material and the electric field. a) In a linear material b) In a crystal without inversion symmetry.

The optical polarisation induced by an applied sinussoidal electric field with frequency . The polarisation consists of three contributions with frequencies , 2 and 0 (dc-term)

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Nonlinear Optical Effects in Solids

The nonlinear optical effects are described by the polarization: (1) (2) (3) D = 0E + P , Pi ( E ) = ( 0 ij E j + 2 ijk E j Ek + 4 ijkl E j Ek El +) Linear optics is described by ij(1) : The optical properties are independent of the light intensity The frequency of light does not change due to interaction with light The principle of superposion is valid Nonlinear optics is described by ijk(2) and ijkl(3) Light can interact with light The principle of superposion is not valid New waves with new k-vectors and new frequencies are generated
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Nonlinear Optical Effects in Solids

The nonlinear optical effects are described by the polarization:
D = 0E + P ,
(1) (2) (3) Pi ( E ) = ( 0 ij E j + 2 ijk E j Ek + 4 ijkl E j Ek El +)

ij(1) describes the linear 1. order optical properties: absorption () and refraction (n) ijk(2) describes the 2. order nonlinearities: frequency doubling, electro-optic effect, and parametric oscillation, etc. ijkl(3) describes 3. order nonlinearities: quadratic kerr effect, intensity-dependent refractive index, four-wave mixing, self-focusing, etc.

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Quantum mechanical determination of the susceptibility

The material response is given by the polarization:

P(t ) = 0 E{ ( )eit + ( )eit }

(1)

The susceptibility () may be determined by calculating P(t) quantum mechanically and then determine () by comparison with Eq.(1).

The macroscopic polarization with N atoms in a volume V is:

P(t ) = Nd (t ) / V
3

Where the electric dipole moment is

d (t ) = (t )eX (t )d r , X= x j
j=1

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Formulation of the interaction in nonlinear materials

The Maxwell equations:

D H H = J + , E=-0 , t t D= 0 E + P , J = E
lead to:
E 2E 2 P NL E = 0 + 0 0 2 + 0 t t t 2
2

the nonlinear wave equation

The nonlinear polarization term PNL leads to the generation of new waves with new k-vectors, polarization, and frequencies: i ( t k z ) E ( z , t ) = A e + c.c. For a new wave: i i the nonlinear wave equation reduces (SVEA-approximation) to:
i i

dAi i (it ki z ) 0 1 0 i (i t ki z ) + c.c. = + c.c. + i e i Ai e 0 i dz 2 0 i

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2 P NL t 2

The nonlinear wave equation

dAi i (it ki z ) 0 1 0 i (i t ki z ) e + c.c. = + c.c. + i i Ai e dz 2 0 i 0 i
i
1

2 P NL t 2

This is the fundamental equation that governs the generation of a new wave Ei ( z , t ) = Ai ei ( t k z ) + c.c.
i i

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Second Order Nonlinear Optics

The interaction between light and matter is given by:
(1) (2) (3) Pi ( E ) = ( 0 ij E j + 2 ijk E j Ek + 4 ijkl E j Ek El + )

where
(2) Pi , NL 2 ( E ) = 2 ijk E j Ek

describes the second order nonlinearities. The notation

(2) ijk = dijk

is often used in the literature where dijk is a third order tensor. with 27 elements.
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Contracted Notation for the Second Order Susceptibility

Pi , NL 2 ( E ) = 2dijk E j Ek
since where
(2) ijk = dijk

dijk = dikj

The third order tensor may be represented by a (3x6) matrix:

d11 K dil = M O d 31 L
with 18 elements.

d16 M a36

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Generation of new waves using second order nonlinearities

Sum frequency generation 1 , 2 Second harmonic generation , Difference frequency generation 1 , 2
Nonlinear crystal
Nonlinear crystal
Nonlinear crystal

1+ 2

1-2

Optical parametric oscillator (OPO) pump

M Nonlinear crystal M

signal , idler

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Three Wave Mixing

Two waves E(1) and E(2) may due to the interaction with the second order nonlinear polarization generate a third beam E(3)

1 , 2
The three waves are given by:

Nonlinear crystal

1, 2, 3

E1 (1 ) = A1ei (1t + k1z ) + c.c. , E2 (2 ) = A2 ei (2t + k2 z ) + c.c. , E3 (3 ) = A3ei (3t + k3 z ) + c.c.

where we have assumed all waves to be polarized in the same direction. For the three waves the nonlinear wave Equation reduces to:
c i dc dA1 = 0 1 A1 1 0 A3 A2*e ikz dz n1 2n1
i dc c dA2 = 0 2 A2 2 0 A3 A1*e ikz ' dz 2n2 n2 dA3 i dc c = 0 3 A3 3 0 A1 A2 eikz dz 2n3 n3

The fundamental equations that describes second order nonlinear interaction.

0 c = 0 0 i n3

where k=k3-k1-k2 , = (2- 1 2 )/2 , and where we have used (1 2=1 for 1= 2 and 1 2=0 for 1 #2)
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Frequency doubling
1= , 2=
The fundamental equation
Nonlinear crystal

, 3=2
reduces to:

dA3 c i dc = 0 3 A3 3 0 A1 A2 eikz dz 2n3 n3

i0 dc 2 dA(2 ) = A ( )eikz dz n(2 )

where absorption is neglected. If we assume that A1=A2=A() is undepleted we obtain the second harmonic intensity:
3 3 2 2 2 0 c d 2 sin(kL / 2) I (2 ) = 2 L I ( ) 2 n ( )n(2 ) kL / 2 2

where L is the length of the nonlinear crystal.

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Phase matching in materials with birefringence

Strong SHG signals are obtained when :
k=k 3 -k1 -k 2 =k 3 -2k1 = 2 (n(2 ) n( )) = 0 c

Phase matching condition

It was suggested independently by Giordmaine(ref.1) and Maker et al(ref.2)) that index matching may be obtained in birefractive crystals by correct choice of polarisation and angle of propagation. The intersection defines the propagation direction.

In Ref. 2 phase matching in KDP with an 300-fold increase of blue light intensity was observed in 1962

Ref.1: J.A.Giordmaine, Phys. Rev. Letters, 8, 19(1962); Ref2: P. Maker et. al, Phys. Rev. Letters, 8, 21(1962),

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Type I and II phase matching

Type I phase matching: The refractive index of an extraordinary beam is given by: ne ( ) =
no ne

n0 2 sin 2 + ne 2 cos 2 Phase matching is obtained in negative uniaxial crystals (ne<n0) when n (2 , ) = n
e m

Type II phase matching: In this case the fundamental beam consist of both an ordinary beam and an extraordinary beam and in this configuration the beam at 2 fulfils the condition:

ne ( m , 2 ) = (ne ( m , ) + n0 ( ))
and the frequency doubled beam will be an extraordinary beam
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Suggested further reading: Nonlinear Optics by R. W. Boyd Academic Press Optical Electronics in Modern Communications by A. Yariv, Oxford University Press The Principles of Nonlinear Optics by Y. R. Shen, Wiley

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