INTRODUCTION TO NONLINEAR OPTICAL EFFECTS IN MOLECULES AND POLYMERS

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1 INTRODUCTION TO NONLINEAR OPTICAL EFFECTS IN MOLECULES AND POLYMERS PARAS N. PRASAD Photonics Research Laboratory Department of Chemistry State University of New York Buffalo, New York and DAVID J. WILLIAMS Corporate Research Laboratories Eastman Kodak Company Rochester, New York A Wiley-Interscience Publication JOHN WILEY & SONS, Inc. New York Chichester Brisbane Toronto Singapore

2 CONTENTS 1. Introduction Nonlinear Optics and Photonics, Nonlinear Optical Materials, Basic Research Opportunities, Multidisciplinary Research, Scope of This Book, 6 2. Basis and Formulation of Nonlinear Optics Interaction of Light with a Medium, Light Propagation through an Optical Medium, The Harmonie Oscillator Model for Linear Optical Processes, Nonlinear Optical Media, The Anharmonic Oscillator Model for Nonlinear Optical Effects, Anisotropie Media, Tensors, Symmetry, 27 Appendix, 29 References, Origin of Microscopic Nonlinearity in Organic Systems Microscopic Nonlinearity, Brief Review of o and n Electrons and Bonding, Equivalent Internal Field Model, 39 vii

3 viii CONTENTS 3.4 Additivity Model for Molecular Hyperpolanzabilities, Quantum-Chemical Approaches,, Derivative versus Sum-over-States Method, Derivative Methods, Sum-over-States Approach, Two-Level Model, The Free-Electron Model, Orientational Nonlnearity, 56 References, Bulk Nonlinear Optical Susceptibility Induced Polarization, Relationship between Microscopic and Macroscopic Nonlinearities in Crystals, Poled Polymers, Langmuir-Blodgett Films, Third-Order Susceptibilities in Crystals, Polymers, and Langmuir-Blodgett Films, Relation of x i3) between Film-Based and Laboratory-Based Coordinate Systems, 80 References, Second-Order Nonlinear Optical Processes General Considerations, Second-Harmonic Generation, Parametric Processes, Sum-Frequency Generation, Parametric Up-conversion, Difference-Frequency Generation, Parametric Oscillator, Low-Frequency Effects, Electrooptic Effect, Optical Rectification, 104 References, Measurement Techniques for Second-Order Nonlinear Optical Effects Electric Field-Induced Second-Harmonic Generation Method, Solvatochromic Measurements, Methods for Measuring x <2 \ Kurtz Powder Technique, Electrooptic Measurements, 122 References, 131

4 CONTENTS ix 7. A Survey of Second-Order Nonlinear Optical Materials Perspective, Structural Requirements for Second-Order Optical Nonlinearity, Crystals and Inclusion Complexes, Poled Polymers, Langmuir-Blodgett Films, 160 References, Third-Order Nonlinear Optical Processes The Various Third-Order Processes and Resulting Polarizations, Third-Harmonic Generation, Self-Action, Two-Photon Absorption, Degenerate Four-Wave Mixing, Coherent Raman Effects, Third-Harmonic Generation, Electric Field-Induced Second-Harmonic Generation, Degenerate Four-Wave Mixing, Resonant Nonlinearity, Other Mechanisms Contributing to the Intensity Dependence of the Refractive Index, Intensity-Dependent Phase Shift, Cascading Effect, 196 References, Measurement Techniques for Third-Order Nonlinear Optical Effects A General Discussion of the Measurement of x i3 \ Selective Measurement Techniques, Third-Harmonic Generation, Electric Field-Induced Second-Harmonic Generation, Degenerate Four-Wave Mixing, Optical Kerr Gate, Self-Focusing Methods, Surface Plasmon Nonlinear Optics, Nonlinear Fabry-Perot Method, Measurement of Microscopic Nonlinearities, y, 218 References, A Survey of Third-Order Nonlinear Optical Materials Perspective, Structural Requirements for Third-Order Optical Nonlinearity, 224

5 x CONTENTS 10.3 Liquid Materials and Solutions, Conjugated Polymers, Polydiacetylenes, Poly-p-phenylene Vinylenes and Analogues, Polyacetylene, Polythiophene, Other Conjugated Polymers, Macrocycles, Polysilanes, Organometallic Structures, 246 References, Nonlinear Optics in Optical Waveguides and Fibers Basic Concepts of Guided Waves, Nonlinear Optics with Guided Waves, Second-Order Nonlinear Optical Processes, Second-Harmonic Generation in a Planar Waveguide, Phase Matching in a Periodically Poled Waveguide, Second-Harmonic Generation in Organic Crystal Cored Fibers, Third-Order Nonlinear Optical Processes, Material Requirements for Waveguides, 268 References, Device Concepts Introduction, Frequency Conversion, Light Modulation, Spatial Light Modulators, Mach-Zehnder Interferometer, Optical Switching, Optical Bistability, Sensor Protection, Optical Phase Conjugation, 292 References, Issues and Future Directions Microscopic Processes, Local Fields, Materials for Second-Order Nonlinear Optics, Materials for Third-Order Nonlinear Optics, 300 References, 302 Appendix: Units Index

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