Prog. @wont. Electr., Vol. 5. pp. 1-M Pergamon Precs. 1977.

Printed in Great Britain

THIRD-ORDER OPTICAL SUSCEPTIBILITIES

R. W. HELLWARTH

Department of Physics and Electrical Engineering, University of Southern California, Los

CONTENTS

1. Introduction 2
2. General Theoretical Background 5
2.1. Nonlinear susceptibilities 5
2.2. General symmetry properties 5
2.3. Quantum theory of susceptibility tensors 6
3. The Born-Oppenheimer (BO) Approximation 8
3.1. Outline of the approximation method 8
3.2. The electronic energy 9
3.3. The effective polarization operator 10
3.3.1. The dipole operator 10
3.3.2. The susceptibility operator 11
3.3.3. The nonlinear electronic susceptibility operators 12
3.4. Born-Oppenheimer approximation for the total expected polarization density P,(rt) 12
3.5. The linear susceptibility in the BO approximation 13
3.6. The second order susceptibility in the BO approximation 14
4. The Third-Order Polarization in the BO Approximation 15
5. Symmetry Properties of Third-Order Optical Susceptibility in the BO Approximation 16
5.1. Some general properties 16
5.2. Third-order BO susceptibilities for cubic and isotropic media 18
6. Relation of Third-Order Optical Susceptibility to Inelastic Light Scattering 18
6.1. Derivation in Born-Oppenheimer approximation 19
6.2. Application to glasses 20
7. Self-induced Refractive Index Changes of a Monochromatic Beam: c,,*r(- 0, 0, 0, -w) 22
7.1. Introduction 22
7.2. General relations 23
7.2.1. Symmetry relations for cubic and isotropic materials 24
7.3. Self-focusing indices for cubic and isotropic media 24
7.3.1. Measurements of absolute index changes 25
7.3.2. Physical origins of self-focusing 25
7.4. Self-induced polarization and index changes 26
7.4.1. Optically anisotropic media 27
7.4.2. Optically isotropic media 28
8. Effect on a Probe Wave of a Strong Monochromatic Pump Wave: c,,,(- V, V, w, - w) 30
8.1. Introduction 30
8.2. Birefringent crystals 32
8.2.1. Stimulated Raman scattering 32
8.2.2. Ordinary light scattering and c,,& - V, V, - o, o) 33
8.2.3. a.~. Kerr effect 33
8.3. Cubic and isotropic media 34
8.3.1. Stimulated Raman scattering 35
8.3.2. a.c. Kerr effect 36
8.3.3. Raman-induced Kerr effect 37
8.3.4. d.c. Kerr effect 38
8.3.5. Probe beam lens effects 40
9. Three-wave Mixing: c ,,*,(- 2w + v, o, O, - V) 41
10. Field-Induced Second Harmonic Generation: c ,,*,(- 20, o, o, 0) 45
11. Electric-field Induced Absorption and Resonant d.c. Kerr Effect: c~,~,(- O, 0, 0, O) 47
12. Third Harmonic Generation: c& - 30, W, O, O) 49
13. Dispersion in Third-Order Susceptibilities 50
13.1. Dispersion in symmetry character of c,,~, 50
13.2. Theoret_ical magnitude-dispersion corrections 51
13.2.1. D,,*, dispersion 51
13.2.2. c?+, dispersion 52
13.3. Experiments on dispersion of c-coefficients near the BO limit 53
14. Summary and Conclusions 56
14.1. Nonresonant electronic and nuclear BO parameters 56
14.2. Light scattering standards 58
14.3. d.c. Kerr constants as standards 59

JPQE Vol. 5. No. I-A I