Second-order nonlinear optical characterization techniques : an introduction

Although chemists, biochemists, biologists, and material scientists are often interested in using nonlinear optical techniques for characterizing their samples, they seldom have the necessary background to exploit these methods. Designed for nonspecialists, Second-Order Nonlinear Optical Characterization Techniques: An Introduction focuses on the potential of second-order nonlinear optics as a powerful characterization tool. Avoiding extensive mathematical details, this multidisciplinary book does not require a background in advanced mathematics or physics.

After introducing linear optics from the perspective of polarizability and linear susceptibility, the authors cover incoherent second-harmonic generation. They then deal with the study of surfaces and interfaces, exploiting the intrinsic surface sensitivity of second-harmonic generation and sum-frequency generation. The final chapter discusses second-order imaging techniques, including confocal microscopy and two-photon excited fluorescence microscopy.

Accessible to a wide range of scientists, this concise book stresses the reliability of nonlinear optical processes for probing surfaces and interfaces. Drawing on the insight offered in the text, scientists from many disciplines can now clearly understand and use second-order nonlinear optical methods.

Preface	p. ix
The Authors	p. xiii
Chapter 1 General aspects of second-order nonlinear optics	p. 1
1.1 Linear optical phenomena	p. 1
1.1.1 Interaction of light with matter	p. 1
1.1.2 Wave propagation in optical media	p. 3
1.1.3 Tensor properties of polarizability and susceptibility	p. 7
1.2 Nonlinear optical phenomena	p. 8
1.3 Examples of nonlinear optical phenomena	p. 9
1.4 Symmetries in second-order nonlinear optics	p. 11
1.5 Second-order polarizabilities and susceptibilities	p. 21
1.6 Beyond the electric-dipole approximation	p. 24
References	p. 26
Chapter 2 Determination of molecular symmetry with hyper-Rayleigh scattering	p. 27
2.1 Hyper-Rayleigh scattering: General principles	p. 27
2.2 Experimental techniques and equipment	p. 34
2.3 Determination of molecular symmetries	p. 41
2.4 Switching the first hyperpolarizability at the molecular level	p. 48
2.5 Probing aggregation and supramolecular structure in solution	p. 53
References	p. 59
Chapter 3 Characterization of interfaces, surfaces, and thin films	p. 63
3.1 Second-harmonic generation and sum-frequency generation from surfaces: General principles	p. 63
3.1.1 Introduction	p. 63
3.1.2 The wave equation for SFG and SHG	p. 68
3.2 Experimental techniques and equipment	p. 75
3.2.1 Absolute and relative measurements	p. 75
3.2.2 Maker fringe technique	p. 76
3.3 Probing the symmetry of interfaces, surfaces, and thin films	p. 80
3.3.1 Interpreting Maker fringe patterns	p. 80
3.3.2 Oxide photonic glasses	p. 81
3.3.2.1 Induction of SONL properties in oxide glasses	p. 82
3.3.2.2 Thickness and profile effect of the NLO layer in poled oxide glasses	p. 86
3.3.3 Organic- and polymer-oriented materials	p. 89
3.3.3.1 Langmuir-Blodgett (LB) films	p. 91
3.3.3.2 Poled organic polymer films	p. 93
3.4 Molecular orientation at surfaces	p. 96
3.4.1 Relationship between bulk response and molecular response	p. 96
3.4.2 Application to an uniaxial polar interface	p. 101
3.4.2.1 Experimental ODF-based approach	p. 101
3.4.2.2 Mean-field potential approach: The liquid-oriented model	p. 107
3.5 Surface adsorption and surface reactions	p. 108
References	p. 112
Chapter 4 Characterization of surface chirality by second-harmonic generation and sum-frequency generation	p. 115
4.1 Chirality and second-order nonlinear optics: general principles	p. 115
4.1.1 Chirality and optical activity	p. 115
4.1.2 Nonlinear optical activity in second-harmonic generation	p. 119
4.1.3 Nonlinear optical activity and magnetic-dipole contributions	p. 126
4.1.4 SHG from chiral films: basic theory	p. 128
4.1.4.1 Second-harmonic generation-Circular dichroism	p. 132
4.1.4.2 SHG-ORD	p. 133
4.1.5 Sum-frequency generation in chiral isotropic liquids	p. 135
4.2 Experimental procedures	p. 136
4.2.1 Continuous polarization measurements	p. 136
4.2.2 Probing the chiral xyz component to study chirality	p. 140
4.2.3 SHG-CD and SHG-ORD measurements	p. 140
4.3 Second-harmonic generation in nanostructures	p. 141
4.4 Applications to biological systems	p. 143
4.5 Molecular origin	p. 144
4.6 Relation with the Faraday effect	p. 145
References	p. 147
Chapter 5 Second-order nonlinear optical imaging techniques	p. 149
5.1 General principles	p. 149
5.1.1 Introduction to nonlinear imaging techniques	p. 149
5.1.2 Basics of microscopy: Gaussian beam optics	p. 151
5.1.3 Confocal microscopy	p. 155
5.2 Experimental techniques and equipment	p. 158
5.2.1 Two-photon excited fluorescence imaging	p. 158
5.2.2 Two-photon excited second-harmonic generation imaging	p. 161
5.3 Applications	p. 164
References	p. 166
Appendix	p. 169
Index	p. 173

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