Foundations of Nonlinear Optical Microscopy

Foundations of Nonlinear Optical Microscopy Concise yet comprehensive resource presenting the foundations of nonlinear optical microscopy Foundations of Nonlinear Optical Microscopy brings together all relevant principles of nonlinear optical (NLO) microscopy, presenting NLO microscopy within a consistent framework to allow for the origin of the signals and the interrelation between different NLO techniques to be understood. The text provides rigorous yet practical derivations, which amount to expressions that can be directly related to measured values of resolution, sensitivity, and imaging contrast. The book also addresses typical questions students ask, and answers them with clear explanations and examples. Readers of this book will develop a solid physical understanding of NLO microscopy, appreciate the advantages and limitations of each technique, and recognize the exciting possibilities that lie ahead. Foundations of Nonlinear Optical Microscopy covers sample topics such as: Light propagation, focusing of light, pulses of light, classical description of light-matter interactions, and quantum mechanical description of light-matter interactions Molecular transitions, selection rules, signal radiation, and detection of light Multi-photon fluorescence and pump-probe microscopy Harmonic generation, sum-frequency generation, and coherent Raman scattering Senior undergraduate and graduate students in chemistry, physics, and biomedical engineering, along with students of electrical engineering and instructors in both of these fields, can use the information within Foundations of Nonlinear Optical Microscopy and the included learning resources to gain a concise yet comprehensive overview of the subject.

Table of Contents:
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 χ(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 White Noise 405 Appendix D Fermi’s Golden Rule 407 Appendix E Population Dynamics with Relaxation 411 Appendix F Stimulated Raman Scattering with Quantized Fields 413 Index 415