Laser Stimulated Scattering and Multiphoton Excitation

Description

Laser Stimulated Scattering and Multiphoton Excitation is the first book to comprehensively cover quantum electrodynamic theory of stimulated scattering and multiphoton excitation processes, as well as various stimulated scattering effects. These include stimulated Raman scattering (SRS) and stimulated Brillouin scattering (SBS), as well as more recent advances in the field such as stimulated Kerr scattering (SKS), stimulated Rayleigh-Bragg scattering (SRBS) and stimulated Mie scattering (SMS). The book goes on to discuss multiphoton excitation-based nonlinear optical effects, photoelectric effects, atomic and molecular ionization effects, and molecular dissociation effects. Each chapter includes a description of the key concepts and mechanisms alongside the necessary theoretical formulations, as well as engaging with the latest experimental research achievements and the scientific and technological applications. Laser Stimulated Scattering and Multiphoton Excitation is essential reading for academics, research scientists, and students working or interested in the areas of nonlinear optics, nonlinear photonics, laser spectroscopy, physical optics, physical chemistry, and optoelectronic engineering. cover titlepage copyright Dedication Contents Preface 1 Introduction 1.1 Characterization of Optical Radiation Field 1.1.1 Intensity and Brightness 1.1.2 Spatial and Temporal Coherence 1.1.3 Photon Mode and Photon Degeneracy 1.1.4 Basic Properties of Photons 1.1.5 Features of an Intense Laser Field 1.2 Two Theoretical Regimes 1.2.1 Semiclassical Theory 1.2.2 Quantum Theory of Radiation 1.3 Two Main Areas Covered in this Book 1.3.1 Stimulated Scattering Effects 1.3.2 Multiphoton Excitation Effects 2 About Light Scattering 2.1 Scattering in Optically Pure Media 2.1.1 Molecular Rayleigh Scattering 2.1.2 Brillouin Scattering in a Continuum Medium 2.1.3 Molecular Raman Scattering 2.1.4 Molecular Rayleigh-Wing Scattering 2.2 Mie Scattering in a Medium Containing Impurity Particles Suspension 2.2.1 Cross-Section of Mie Scattering 2.2.2 Wavelength Dependence of Mie Scattering 2.2.3 Angular Distribution of Mie Scattering 2.3 Spontaneous and Stimulated Light Scattering 2.3.1 Spontaneous Light Scattering 2.3.2 Stimulated Light Scattering 2.3.3 Gain Mechanisms of Stimulated Scattering Effects 3 Quantum Electrodynamic Theory of Light Radiation 3.1 Energy of Classical Electromagnetic Field 3.1.1 Vector Potential of the Electromagnetic Field 3.1.2 Energy Density of the Electromagnetic Field 3.2 Quantization of Electromagnetic Field: Photons 3.2.1 Quantization of the Electromagnetic Field 3.2.2 The Concept of Photon 3.2.3 Photon Creation and Annihilation Operators 3.2.4 Vector Potential of Quantized Electromagnetic Field 3.3 Combined Quantum System of the Photon Field and a Molecule 3.3.1 Interaction Energy between the Quantum Electromagnetic Field and a Molecule 3.3.2 Eigenfunction of the Combined Quantum-Mechanical System 3.4 One-Photon Emission and Absorption 3.4.1 One-Photon Emission Process 3.4.2 One-Photon Absorption Process 4 Stimulated Raman Scattering 4.1 Quantum-Electrodynamic Theory of Stimulated Raman Scattering 4.1.1 Quantum Picture of Raman Scattering 4.1.2 Theoretical Description of Raman Scattering 4.1.3 Molecular Raman Scattering Cross-Section 4.1.4 Spontaneous and Stimulated Raman Scattering 4.1.5 Gain Coefficient of Stimulated Raman Scattering (SRS) 4.1.6 Pump Spectral-Linewidth Influence on Gain Coefficient 4.1.7 Stokes and Anti-Stokes SRS 4.1.8 Threshold Requirement for Pump Intensity I0 4.2 Raman Media and SRS Setups 4.2.1 Raman Media 4.2.2 Experimental Setups 4.2.3 Major Issues of Experimental Studies 4.3 Four-Wave Frequency Mixing and SRS 4.3.1 Four-Wave Frequency Mixing (FWFM) 4.3.2 Raman Resonance-Enhanced FWFM in SRS Processes 4.3.3 Examples of SRS Output Accompanied by FWFM emissions 4.4 Self-Focusing Effect in SRS Processes 4.4.1 SRS Processes Accompanied with Self-Focusing 4.4.2 Raman Resonance-Enhanced Refractive-Index Change 4.4.3 Raman Resonance-Enhanced Self-Focusing in Calcite and Benzene 4.4.4 Self-Focusing of SRS in Optical Quartz Glass Fibers 4.5 Self-Termination Effect of SRS in Liquid Media 4.5.1 Origin of Self-Defocusing of Both SRS and Pump Beams in Liquids 4.5.2 Recent Studies of Self-Termination Effect of SRS in Liquids 4.5.3 Methods of Reducing the Self-Defocusing Influence 4.6 Spectral Super-Broadening Effect of Backward SRS in Liquids 4.6.1 Experimental Observations 4.6.2 Theoretical Explanation: Different XPM Influence of Pump Sub-Pulses 4.7 Special SRS Effects 4.7.1 Spin-Flip SRS in Semiconductor Crystals 4.7.2 Electronic Transition SRS in Metal Vapors 4.7.3 Rotational Transition SRS in Molecular Gases 5 Stimulated Brillouin Scattering 5.1 Fundamental Description of Stimulated Brillouin Scattering (SBS) 5.1.1 Stokes Scattering Generation 5.1.2 Anti-Stokes Scattering Generation 5.2 Equations of Interaction between Light and Acoustic Field 5.2.1 Acoustic-Field Equation of Medium under Action of Intense Light 5.2.2 Electromagnetic Field Equation in Medium with Photoelastic Effect 5.3 Solution of Coupled Equations and Gain Coefficient of SBS 5.3.1 Coupled Wave Equations and Their Solutions 5.3.2 Exponential Gain and Threshold Condition of SBS 5.4 Materials and Experimental Setups for SBS Studies 5.4.1 Materials of SBS 5.4.2 Experimental Setups of SBS 5.5 Major Issues of Experimental Studies on SBS 5.5.1 Pump Threshold and Nonlinear Reflectivity of SBS 5.5.2 Measurements of Induced Hypersonic Field 5.5.3 Start-Delay of SBS Generation 5.5.4 Deference and Competition between SRS and SBS 6 Stimulated Kerr Scattering 6.1 Early Reported Stimulated Rayleigh-Wing Scattering in Kerr Liquids 6.1.1 Reorientational Kerr Effect in Liquids 6.1.2 Early Reported Stimulated Rayleigh-Wing Scattering (SRWS) 6.2 Discovery of a Super-Broadband Stimulated Scattering 6.3 Mechanisms of Rayleigh–Kerr and Raman–Kerr Scattering 6.4 Theory of Stimulated Kerr Scattering (SKS) 6.4.1 Molecular Kerr Scattering Cross-Section 6.4.2 Exponential Gain of SKS 6.5 Experimental Studies of SKS 6.5.1 Forward Stimulated Rayleigh–Kerr Scattering from a CS2-Core Fiber System 6.5.2 Forward Stimulated Raman–Kerr Scattering (SRmKS) from a C6H6-Core Fiber System 6.5.3 Forward SKS from Other Liquid-Core Fiber Systems 6.5.4 Studies of SKS in a Short CS2 Liquid Cell 6.5.5 Self-Termination Effect of SKS in CS2 Liquid 7 Stimulated Rayleigh–Bragg Scattering 7.1 Stimulated Thermal Rayleigh Scattering (STRS) in a Linearly Absorbing Medium 7.1.1 Early Theory of STRS 7.1.2 Early Experimental Studies on STRS 7.1.3 Recent Experimental Studies of Thermal Influence on the Stimulated Scattering in a Linearly Absorbing Medium 7.2 Stimulated Rayleigh–Bragg Scattering (SRBS) in a Multiphoton Absorbing (MPA) Liquid Medium 7.2.1 Finding of Frequency-Unshifted Backward Stimulated Scattering in a Two-Photon Absorbing (2PA) Medium 7.2.2 Physical Model of SRBS 7.2.3 Pump Threshold Requirement for SRBS 7.2.4 Pump Spectral Linewidth Requirement for SRBS 7.3 Experimental Studies of SRBS in MPA Liquid Media 7.3.1 Original Studies of SRBS in a 2PA Dye Solution 7.3.2 Experimental Study of SRBS in a 3PA Dye Solution 7.4 Recent Studies of SRBS 7.4.1 High-Efficiency SRBS Generation in Two-Photon Active Dye Solutions 7.4.2 Mechanisms of Induced Refractive-Index Changes of a Multiphoton Active Solution Medium 7.4.3 Experimental Verification of the Proposed Theoretical Model 8 Stimulated Mie Scattering 8.1 Mechanism of Stimulated Mie Scattering 8.1.1 Background of the Finding of Stimulated Mie Scattering 8.1.2 Principle of Stimulated Mie Scattering (SMS) 8.1.3 Mechanism for Induced Refractive-Index Change of a Mie Scattering Medium 8.2 SMS Generation in a Gold (Au)-Nanorods Suspension 8.2.1 Scattering Medium 8.2.2 Experimental Setup and Output/Input Measurement 8.2.3 Far- and Near-Field Patterns and Temporal Waveforms 8.2.4 Spectral Property of SMS 8.3 SMS Studies in Semiconductor Nanocrystal Suspensions 8.3.1 CdSe-CdS-ZnS Quantum Rods Suspended in Chloroform 8.3.2 CdTexSe1x Quantum Dots in Chloroform 8.3.3 CdSe Nanocrystals in Chloroform 8.3.4 Perovskite Nanocrystals Suspended in n-Hexane 8.4 Experiments Verifying the Mechanism of SMS 8.4.1 Viscosity Effect of a Solvent 8.4.2 Frozen Effect of Nanoparticles in a Solid 8.4.3 Opto-Thermal Effect on Stimulated Scattering in a Linearly Absorbing Mie Scattering Medium 9 Optical Phase-Conjugation Properties of Backward Stimulated Scattering 9.1 Introduction to Optical Phase-Conjugation (OPC) 9.1.1 Background of the Invention of OPC Technique 9.1.2 Definition of a Backward Phase-Conjugate Wave (PCW) 9.1.3 Special Function of a Backward PCW 9.1.4 Frequency-Degenerate FWM Method 9.1.5 Holographic Model of Backward PCW Generation via Degenerate FWM 9.1.6 Partially Degenerate FWM Method 9.2 Backward Stimulated Scattering (BSS) with OPC Properties 9.2.1 Early Observation of OPC Behavior in BSS 9.2.2 Theoretical Explanation: Quasi-Collinear FWM Model 9.2.3 Mathematical Treatments in Unfocused-Beam Approximation 9.3 Experimental Studies on OPC Properties of Various Types of BSS 9.3.1 OPC Properties of Backward Stimulated Brillouin Scattering (SBS) 9.3.2 OPC Properties of Backward Stimulated Rayleigh-Bragg Scattering (SRBS) 9.3.3 OPC Properties of Backward Stimulated Mie Scattering (SMS) 9.4 Applications of Backward OPC Generation 10 Multiphoton Absorption (MPA) Theories 10.1 Intermediate States and Virtual Energy Levels 10.1.1 Similarity between Raman Scattering and Two-Photon Absorption (2PA) 10.1.2 Rigorous Diagrammatic Description of Two-Photon Absorption (2PA) 10.2 Two-Photon Absorption (2PA) Process 10.2.1 Molecular 2PA Probability 10.2.2 Transition Matrix Elements of 2PA 10.2.3 2PA Cross-Section 10.3 Three-Photon Absorption (3PA) Process 10.3.1 Molecular 3PA Probability 10.3.2 Transition Matrix Elements of 3PA 10.3.3 3PA Cross-Section 10.4 Four-Photon Absorption (4PA) Process 10.4.1 Molecular 4PA Probability 10.4.2 4PA Cross-Section 10.5 m-Photon Absorption (MPA) Process 10.5.1 Molecular MPA Probability 10.5.2 MPA Cross-Section 11 Multiphoton Nonlinear Optical Effects 11.1 Formulations of MPA-Induced Light Attenuation 11.1.1 Two-Photon Absorption (2PA)-Induced Intensity Attenuation 11.1.2 Three-Photon Absorption (3PA)-Induced Intensity Attenuation 11.1.3 Multiphoton Absorption (MPA)-Induced Intensity Attenuation 11.2 Highly Multiphoton Active Materials 11.2.1 Need for Highly Multiphoton Active Materials 11.2.2 Basic Structures of Multiphoton Active Chromophores 11.2.3 Features of Novel Multiphoton Active Materials 11.3 Characterizations of MPA Materials 11.3.1 Selection of Excitation Wavelengths 11.3.2 Measurements of MPA Cross-Section at Discrete Wavelengths 11.3.3 Time-Regime Dependence of Measured Cross-Section Values 11.3.4 Saturation Effect of MPA in Sub-Picosecond Regime 11.3.5 Measurements of MPA Spectra 11.3.6 Characterization of MPA-Induced Fluorescence Emission 11.4 Multiphoton Pumped (MPP) Upconversion Lasing 11.4.1 General Features of MPP Lasing Materials and Devices 11.4.2 Two-Photon Pumped (2PP) Cavity Lasing 11.4.3 3P–4P Pumped Lasing 11.4.4 Spectral Asymmetry between Forward and Backward MPP Lasing 11.5 MPA-Based Optical Limiting, Stabilization, and Reshaping 11.5.1 Principles of Optical Limiting 11.5.2 MPA-Based Optical Limiting 11.5.3 MPA-Based Optical Stabilization 11.5.4 MPA-Based Optical Reshaping 11.6 MPA-Based 3D Data Storage and Microfabrication 11.6.1 Common Features of MPA for Data Storage and Microfabrication 11.6.2 3D Data Storage in Two-Photon Active Materials 11.6.3 Two-Photon Polymerization-Based 3D Microfabrication 12 Multiphoton Photoelectric Effects 12.1 Introduction to Photoelectric Effects 12.1.1 One-Photon Photoemission Effect 12.1.2 Electronic Band Structures of Solids 12.1.3 One-Photon-Induced Photoconductivity in Semiconductors 12.1.4 Image-Potential States (IPSs) of the Electron at Metal Surface 12.2 Multiphoton Photoemission (MPPE) Effects 12.2.1 Early Observations of MPPE Phenomena 12.2.2 Resonance-Enhanced MPPE Effects 12.2.3 MPPE Studies on Clean Metal Surfaces 12.2.4 MPPE Studies on Adsorbed Metal Surfaces 12.2.5 Angle-Dependent MPPE Studies 12.2.6 Other Related MPPE Studies 12.3 Multiphoton Photoconductivity (MPPC) Effects 12.3.1 Mechanisms of Multiphoton-Induced Photoconductivity 12.3.2 Observations of MPPC Effects in Semiconductors and Dielectric Media 12.3.3 2PPC-Based Spectroscopic Studies on Semiconductors 12.3.4 MPPC-Based Autocorrelation Measurements of Ultrashort Laser Pulses 12.3.5 Other Related Studies 13 Multiphoton Ionization of Atoms and Molecules 13.1 Principle of Laser Ionization of Atoms and Molecules 13.1.1 Features of Laser Ionization 13.1.2 Types of Resonance-Enhanced Multiphoton Ionization (REMPI) 13.1.3 Simultaneous and Multi-Step Multiphoton Excitation Processes 13.1.4 Rydberg States of Atoms and Molecules 13.1.5 Experimental Setup and Devices 13.2 Multiphoton Ionization (MPI) Studies of Atoms 13.2.1 A Brief Overview of the Studies 13.2.2 Nonresonant MPI of Atoms 13.2.3 Rydberg States Studies of Atoms 13.2.4 Photoelectron Detection Studies 13.3 Multiphoton Ionization Studies of Molecules 13.3.1 A Brief Overview of the Studies 13.3.2 Rydberg States Studies of Molecules 13.3.3 Vibronic Spectral Studies of Molecules 13.3.4 Rotational Spectral Studies of Molecules 13.3.5 Photoelectron Detection MPI Studies of Molecules 13.3.6 Time-Resolved MPI Studies of Molecules 14 Multiphoton Dissociation of Molecules 14.1 General Descriptions of Multiphoton Dissociation (MPD) of Molecules 14.1.1 Molecular Energy-Level Structures 14.1.2 Multiphoton Excitation-Induced Molecular Dissociation 14.1.3 Intensity Dependence of MPD Product 14.1.4 Experimental System for MPD Studies 14.2 Multiphoton Dissociation Using Visible and UV Laser Radiation 14.2.1 Features of Visible or UV MPD 14.2.2 Two-Photon Excited Dissociation Studies 14.2.3 Three-Photon Excited Dissociation Studies 14.2.4 Multi (>3)-Photon Excited Dissociation Studies 14.3 Multiphoton Dissociation Using IR Laser Radiation 14.3.1 Earliest Works of IR multiphoton dissociation (IRMPD) 14.3.2 Basic Mechanism of IRMPD 14.3.3 Dissociation Dependence on Laser Fluence 14.3.4 Isotope-Selective IRMPD Studies 14.3.5 Two-Frequency IRMPD Studies 14.3.6 IRMPD Spectroscopy Index