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.

  Autorentext

  Eric Olaf Potma is Professor at the University of California, Irvine, in the Department of Chemistry. His research interests are quantitative imaging with nonlinear optical microscopy, nonlinear optics of individual molecules and nanostructures, and nonlinear optical scan probe microscopy.

  Inhalt

  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 (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