Preface xiii
 
Acknowledgments xv
 
1 Light: Electromagnetic Radiation 1
 
1.1 Introduction 1
 
1.2 Electromagnetic Fields 1
 
1.3 Transverse Waves 7
 
1.4 Polarization States 15
 
1.5 Reflection and Transmission at Interfaces 19
 
1.6 Transformation of the Field by a Lens 23
 
1.7 Intensity and Energy 29
 
Bibliography 31
 
2 Focused Light 33
 
2.1 Introduction 33
 
2.2 Interference of Multiple Waves 34
 
2.3 The Scalar Focal Field 38
 
2.4 The Focused Vector Field 49
 
2.5 Aberrations 60
 
Bibliography 65
 
3 Ultrafast Pulses 67
 
3.1 Introduction 67
 
3.2 Optical Pulses in the Frequency Domain 68
 
3.3 Optical Pulses in the Time Domain 77
 
3.4 Measurement of Pulse Duration 88
 
3.5 Pulse Properties and Nonlinear Optical Signals 95
 
3.6 Noise 97
 
Bibliography 102
 
4 Classical Model of Nonlinear Optics 105
 
4.1 Introduction 105
 
4.2 Linear Optical Response 105
 
4.3 Nonlinear Optical Response 115
 
4.4 Properties of Nonlinear Susceptibilities 124
 
Bibliography 134
 
5 Semiclassical Model of Nonlinear Optics 137
 
5.1 Introduction 137
 
5.2 Quantum Mechanical Concepts 138
 
5.3 Density Matrix Formalism 147
 
5.4 Perturbation Expansion for the Density Matrix 152
 
5.5 Linear and Nonlinear Susceptibilities 159
 
5.6 Quantization of the Electromagnetic Field 164
 
Bibliography 172
 
6 Nonlinear Optical Signals: Molecular Transitions, Signal Radiation, Propagation, and Detection 175
 
6.1 Introduction 175
 
6.2 Molecular Transitions 175
 
6.3 Spatial Properties of Radiated Signal 187
 
6.4 Signal Radiation and Detection 205
 
Bibliography 211
 
7 Multiphoton Absorption and Fluorescence Microscopy 213
 
7.1 Introduction 213
 
7.2 Physics of Nonlinear Absorption 214
 
7.3 Optical Sectioning and Imaging Resolution 223
 
7.4 Direct Detection of Multiphoton Absorption 228
 
7.5 Fluorescence Detection of Multiphoton Absorption 232
 
Bibliography 241
 
8 Pump-Probe Microscopy 245
 
8.1 Introduction 245
 
8.2 Pump-Probe Signals in Microscopy 246
 
8.3 Electronic Pump-Probe Spectroscopy 250
 
8.4 Detection of Pump-Probe Signals 264
 
8.5 Imaging Based on the Photothermal Effect 269
 
Bibliography 277
 
9 Harmonic Generation Microscopy 281
 
9.1 Introduction 281
 
9.2 Molecular Response in Harmonic Imaging 282
 
9.3 SHG Imaging of Fibrillar Structures 292
 
9.4 THG Imaging of chi¯(3) Discontinuities 304
 
Bibliography 310
 
10 Sum-Frequency Generation Microscopy 313
 
10.1 Introduction 313
 
10.2 Molecular Vibrations 314
 
10.3 Molecular Vibrations in Sum-Frequency Generation 324
 
10.4 Collinear Sum-Frequency Generation Microscopy 334
 
10.5 Third-Order Sum-Frequency Generation Microscopy 344
 
Bibliography 348
 
11 Coherent Raman Scattering Microscopy 351
 
11.1 Introduction 351
 
11.2 The Raman Effect 353
 
11.3 Coherent Raman Scattering 359
 
11.4 Raman Spectroscopy of Lipids 373
 
11.5 Imaging Properties of CARS 378
 
11.6 Imaging Properties of SRS 387
 
11.7 Spectral Resolution 391
 
Bibliography 398
 
Appendix A Fourier Transform Relationships 401
 
Appendix B Wavenumbers Unit 403
 
Appendix C Power Spectral Density of W