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Ultrashort Pulse Lasers and Ultrafast Phenomena

✍ Scribed by Takayoshi Kobayashi


Publisher
CRC Press
Year
2023
Tongue
English
Leaves
708
Edition
1
Category
Library

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✦ Synopsis


This book describes the basic physical principles of techniques to generate and ultrashort pulse lasers and applications to ultrafast spectroscopy of various materials covering chemical molecular compounds, solid-state materials, exotic novel materials including topological materials, biological molecules and bio- and synthetic polymers. It introduces non-linear optics which provides the basics of generation and measurement of pulses and application examples of ultrafast spectroscopy to solid state physics. Also it provide not only material properties but also material processing procedures. The book describes also details of the world shortest visible laser and DUV lasers developed by the author’s group. It is composed of the following 12 Sections: The special features of this book is that it is written by a single author with a few collaborators in a systematic way. Hence it provides a comprehensive and systematic description of the research field of ultrashort pulse lasers and ultrafast spectroscopy.

    • Generation of ultrashort pulses in deep ultraviolet to near infrared

    • Generation of ultrashort pulses in terahertz

    • Carrier envelope phase (CEP)

    • Simple NLO processes with a few colors

    • Multi-color involved NLO processes

    • Multi-color ultrashort pulse generation

    • NLO materials

    • NLO processes in time-resolved spectroscopy

    • Low dimension materials

    • Conductors and superconductors

    • Chemical reactions and material processing

    • Photobiological reactions

    ✦ Table of Contents


    Cover
    Half Title
    Title Page
    Copyright Page
    Table of Contents
    Preface
    Author
    Section 1 Generation of Ultrashort Pulses in Deep Ultraviolet to Near Infrared
    Section 1.1 Ultrashort Visible Near-Infrared Pulses
    Chapter 1.1.1 Noncollinearly Phase-Matched Femtosecond Optical Parametric Amplification with a 2000 cm[sup(–1)] Bandwidth
    References
    Chapter 1.1.2 Simultaneous Compression and Amplification of a Laser Pulse in a Glass Plate
    1.1.2.1 Introduction
    1.1.2.2 Principle
    1.1.2.3 Experimental Setup
    1.1.2.4 Experimental Results and Discussion
    1.1.2.5 Conclusion
    References
    Chapter 1.1.3 Pulse-Front-Matched Optical Parametric Amplification for Sub-10-fs Pulse Generation Tunable in the Visible and Near Infrared
    1.1.3.1 Introduction
    1.1.3.2 Experimental
    1.1.3.3 Results and Discussion
    1.1.3.4 Conclusion
    References
    Chapter 1.1.4 Visible 4 fs Pulse From Dispersion Control Optical Parametric Amplifier
    1.1.4.1 Introduction
    1.1.4.2 Configuration of the System
    1.1.4.3 Analysis and Discussion
    1.1.4.4 Conclusion
    References
    Chapter 1.1.5 Ultrafast Laser System Based on Noncollinear Optical Parametric Amplification for Laser Spectroscopy
    1.1.5.1 Introduction
    1.1.5.2 Experimental
    1.1.5.3 Results and Discussion
    1.1.5.4 Conclusion
    References
    Chapter 1.1.6 Development of Ultrashort Pulse Lasers for Ultrafast Spectroscopy
    1.1.6.1 Introduction
    1.1.6.2 Light Sources for Studying Ultrafast Processes
    1.1.6.3 Electronic Relaxation and Vibrational Dynamics
    1.1.6.4 Principles and Advantages of Broad-Band Ultrafast Spectroscopy
    1.1.6.5 Ultrashort Visible Pulse Generation Based on Non-Linear Optical Parametric Amplifier (NOPA)
    1.1.6.6 Ultrashort Deep Ultraviolet Laser
    1.1.6.6.1 DUV Pulse Generation
    1.1.6.6.2 Sub-10 fs DUV Laser Pulse Obtained by Broad-Band CPFWM
    1.1.6.6.3 DUV Pulse Stability Optimization
    1.1.6.7 Conclusion
    References
    Section 1.2 Ultrashort Ultraviolet, Deep-Ultraviolet, and Infrared Pulses
    Chapter 1.2.1 Generation of Stable Sub-10 fs Pulses at 400 nm in a Hollow Fiber for UV Pump-Probe Experiment
    1.2.1.1 Introduction
    1.2.1.2 Experimental Setup
    1.2.1.3 Experimental Results and Discussion
    1.2.1.4 Conclusion
    References
    Chapter 1.2.2 Sub-10 fs Deep-Ultraviolet Pulses Generated by Chirped-Pulse Four-Wave Mixing
    1.2.2.1 Introduction
    1.2.2.2 Experimental
    1.2.2.3 Results and Discussion
    1.2.2.4 Conclusion
    References
    Chapter 1.2.3 Generation and Optimization of Femtosecond Pulses by Four-Wave Mixing Process
    1.2.3.1 Introduction
    1.2.3.2 Cascaded FWM in Bulk Media
    1.2.3.2.1 Principle of Cascaded FWM
    1.2.3.2.2 Generation of Wavelength-Tunable Self-Compressed Multicolored Pulses by Nondegenerate Cascaded FWM
    1.2.3.2.3 Pulse Cleaning by Degenerate Cascaded FWM
    1.2.3.3 UV Pulse Generation by FWM in Hollow Fiber
    1.2.3.3.1 Chirped-Pulse FWM in a Gas-Filled Hollow Waveguide
    1.2.3.3.2 Broadband Chirped-Pulse FWM
    1.2.3.3.3 Practical Issues in Broadband Chirped-Pulse FWM
    1.2.3.3.4 Sub-10-fs DUV Pulses Generated by Broadband Chirped-Pulse FWM
    1.2.3.4 Four-Wave Optical Parametric Amplification (FWOPA) in Bulk Media
    1.2.3.5 Conclusion and Prospects
    References
    Section 2 Generation of Ultrashort Pulses in Terahertz
    Chapter 2.1 Sellmeier Dispersion for Phase-Matched Terahertz Generation in Nonlinear Optical Crystal: An Example of ZnGeP[sub(2)].
    2.1.1 Introduction
    2.1.2 Derivation of the Sellmeier Dispersion
    2.1.3 Generation of Terahertz Radiation with a Nd:YAG Laser
    2.1.4 Generation of Terahertz Radiation with CO[sub(2)] Lasers
    2.1.5 Discussion
    2.1.6 Conclusion
    References
    Chapter 2.2 Saturation of the Free Carrier Absorption in ZnTe Crystals
    2.2.1 Introduction
    2.2.2 Experiments
    2.2.2.1 THz Generation in ZnTe Crystals
    2.2.2.2 Photoluminescence Radiated From ZnTe Crystals
    2.2.3 Discussion
    2.2.4 Conclusion
    References
    Chapter 2.3 Widely Linear and Non-Phase-Matched Optical-to-Terahertz Conversion on GaSe: Te Crystals
    2.3.1 Introduction
    2.3.2 Experimental
    2.3.3 Results and Discussions
    2.3.4 Conclusion
    References
    Chapter 2.4 THz Emission from Organic Cocrystalline Salt: An Example of 2, 6-Diaminopyridinium-4-Nitrophenolate-4-Nitrophenol
    2.4.1 Introduction
    2.4.2 Sample Preparation and THz Emission Experiments
    2.4.3 Results and Discussion
    2.4.4 Summary
    References
    Section 3 CEP (Octave-Span)
    Chapter 3.1 Quasi-Monocyclic Near-Infrared Pulses with a Stabilized Carrier-Envelope Phase Characterized by Noncollinear Cross-Correlation Frequency-Resolved Optical Gating
    3.1.1 Introduction
    3.1.2 Experimental
    3.1.3 Conclusion
    References
    Chapter 3.2 Self-Stabilization of the Carrier-Envelope Phase of an Optical Parametric Amplifier Verified with a Photonic Crystal Fiber
    3.2.1 Introduction
    3.2.2 Experimental
    3.2.3 Results and Discussion
    3.2.4 Conclusion
    References
    Chapter 3.3 Octave-Spanning Carrier-Envelope Phase Stabilized Visible Pulse with Sub-3-fs Pulse Duration
    3.3.1 Introduction
    3.3.2 Results and Discussion
    3.3.3 Conclusion
    References
    Chapter 3.4 Carrier-Envelope-Phase-Stable, Intense Ultrashort Pulses in Near Infrared
    3.4.1 Introduction
    3.4.2 Experimental
    3.4.3 Results and Discussion
    3.4.4 Conclusion
    References
    Section 4 Simple NLO Processes with a Few Colors
    Chapter 4.1 Three-Photon-Induced Four-Photon Absorption and Nonlinear Refraction in ZnO Quantum Dots
    4.1.1 Introduction
    4.1.2 Experimental
    4.1.3 Results and Discussion
    4.1.4 Conclusion
    References
    Chapter 4.2 Femtosecond Pulses Cleaning by Transient-Grating Process in Optical Media
    4.2.1 Introduction
    4.2.2 Experimental
    4.2.3 Results and Discussion
    4.2.4 Conclusion
    References
    Chapter 4.3 Non-Degenerate Two-Photon Absorption Enhancement for Laser Dyes by Precise Lock-in Detection
    4.3.1 Introduction
    4.3.2 Theory
    4.3.3 Experimental Procedures
    4.3.4 Results and Discussion
    4.3.5 Conclusion
    References
    Section 5 Multi-Color Involved NLO Processes
    Chapter 5.1 Generation of µJ-Level Multicolored Femtosecond Laser Pulses Using Cascaded Four-Wave Mixing
    5.1.1 Introduction
    5.1.2 Experimental Setup
    5.1.3 Experimental Results and Discussion
    5.1.4 Conclusion
    References
    Chapter 5.2 Generation and Optimization of Femtosecond Pulses by Four-Wave Mixing (FWM) Process
    5.2.1 Introduction
    5.2.2 Cascaded FWM in Bulk Media
    5.2.2.1 Principle of Cascaded Four-Wave Mixing (FWM)
    5.2.2.2 Generation of Wavelength-Tunable Self-Compressed Multicolored Pulses by Nondegenerate Cascaded FWM
    5.2.2.3 Pulse Cleaning by Degenerate Cascaded FWM
    5.2.3 UV Pulse Generation by FWM in Hollow Fiber
    5.2.3.1 Chirped-Pulse FWM in a Gas-Filled Hollow Waveguide
    5.2.3.2 Broadband Chirped-Pulse FWM
    5.2.3.3 Practical Issues in Broadband Chirped-Pulse FWM
    5.2.3.4 Sub-10-fs DUV Pulses Generated by Broadband Chirped-Pulse FWM
    5.2.4 FWOPA in Bulk Media
    5.2.5 Conclusion and Prospects
    References
    Chapter 5.3 Tunable Multicolored Femtosecond Laser Pulses Generation by Using Cascaded Four-Wave Mixing (CFWM) in Bulk Materials
    5.3.1 Introduction
    5.3.2 Theoretical Analysis
    5.3.2.1 FWM Process
    5.3.2.2 CFWM Process
    5.3.3 Experimental Characteristics of Multicolored Pulses
    5.3.3.1 Experimental Setups
    5.3.3.2 Spectra and Wavelength Tuning of Multicolored Sidebands
    5.3.3.2.1 Tuning the Wavelength of Sidebands by Changing Cross-Angle
    5.3.3.2.2 Tuning the Wavelength of Sidebands by Changing Nonlinear Media
    5.3.3.3 Temporal Characteristics of Multicolored Pulses
    5.3.3.4 Output Power/Energy of Multicolored Pulses
    5.3.3.5 Multicolored Sidebands Generated with Low Threshold
    5.3.4 2-D Multicolored Sidebands Arrays
    5.3.5 Conclusion and Prospects
    References
    Chapter 5.4 Mechanism Study of 2-D Laser Array Generation in a YAG Crystal Plate
    5.4.1 Introduction
    5.4.2 Numerical Simulation Model
    5.4.3 Results and Discussion
    5.4.4 Conclusion
    References
    Section 6 Broadband Ultrashort Pulse Generation
    Chapter 6.1 Broadband Coherent Anti-Stokes Raman Scattering Light Generation in BBO Crystal by Using Two Crossing Femtosecond Laser Pulses
    6.1.1 Introduction
    6.1.2 Experimental
    6.1.3 Results and Discussion
    6.1.4 Conclusion
    References
    Chapter 6.2 Generation of Broadband Two-Dimensional Multicolored Arrays in a Sapphire Plate
    6.2.1 Experimental
    6.2.2 Experimental Setup
    6.2.3 Experimental Results and Discussion
    6.2.4 Conclusion
    References
    Section 7 NLO Materials
    Chapter 7.1 Sellmeier Dispersion for Phase-Matched Terahertz Generation in ZnGeP[sub(2)]
    7.1.1 Introduction
    7.1.2 Derivation of the Sellmeier Dispersion
    7.1.3 Generation of Terahertz Radiation with a Nd:YAG Laser
    7.1.4 Generation of Terahertz Radiation with CO[sub(2)] Lasers
    7.1.5 Discussion
    7.1.6 Conclusion
    References
    Chapter 7.2 Broadband Sum-Frequency Mixing (SFM) in Some Recently Developed Nonlinear Optical Crystals
    7.2.1 Introduction
    7.2.2 Schematic of the Experimental Arrangement
    7.2.3 Theoretical Background of Phase Matching and Broadband SFM
    7.2.4 Results and Discussion
    7.2.5 Broadly Tunable Conventional SFM in a Thin Crystal
    7.2.6 Conclusion
    References
    Chapter 7.3 Optimal Te-Doping in GaSe for Nonlinear Applications
    7.3.1 Introduction
    7.3.2 Crystal Growth and Characterization
    7.3.2.1 Growth Technology
    7.3.2.2 Optical Properties
    7.3.2.3 THz Generation via Optical Rectification
    7.3.3 Discussion
    7.3.4 Conclusion
    References
    Chapter 7.4 Widely Linear and Non-Phase-Matched Optical-to-Terahertz Conversion on GaSe: Te Crystals
    7.4.1 Introduction
    7.4.2 Experimental
    7.4.3 Results and Discussion
    7.4.4 Conclusion
    References
    Section 8 NLO Processes in Time-Resolved Spectroscopy
    Chapter 8.1 Elimination of Coherence Spike in Reflection-Type Pump-Probe Measurements
    8.1.1 Introduction
    8.1.2 Experiments
    8.1.3 Results and Discussion
    8.1.4 Summary
    References
    Chapter 8.2 Vibrational Fine Structures Revealed by the Frequency-to-Time Fourier Transform of the Transient Spectrum in Bacteriorhodopsin
    8.2.1 Introduction
    8.2.2 Experimental Section
    8.2.3 Results and Discussion
    8.2.4 Conclusions
    References
    Section 9 Low Dimensional (D) Materials
    Section 9.1 0D
    Chapter 9.1.1 Superior Local Conductivity in Self-Organized Nanodots on Indium-Tin-Oxide Films Induced by Femtosecond Laser Pulses
    9.1.1.1 Introduction
    9.1.1.2 Experiments
    9.1.1.3 Results and Discussion
    9.1.1.4 Conclusion
    References
    Chapter 9.1.2 Observation of an Excitonic Quantum Coherence in CdSe Nanocrystals
    9.1.2.1 Introduction
    9.1.2.2 Experimental
    9.1.2.3 Results and Discussion
    9.1.2.4 Conclusion
    Supporting Information
    References
    Section 9.2 1D CNT
    Chapter 9.2.1 Coherent Phonon Generation in Semiconducting Single-Walled Carbon Nanotubes Using a Few-Cycle Pulse Laser
    9.2.1.1 Introduction
    9.2.1.2 Experimental Details
    9.2.1.3 Results and Discussion
    9.2.1.3.1 Stationary Absorption Spectrum of the Sample and Laser Spectrum
    9.2.1.3.2 Two-Dimensional (2D) Real-Time Spectra and Exact Chirality Assignment
    9.2.1.3.3 Probe Photon Energy Dependent Amplitude Profiles
    9.2.1.4 Conclusion
    References
    Chapter 9.2.2 Electronic Relaxation and Coherent Phonon Dynamics in Semiconducting Single-Walled Carbon Nanotubes with Several Chiralities
    9.2.2.1 Introduction
    9.2.2.2 Experiment
    9.2.2.2.1 Ultrafast Spectroscopy
    9.2.2.2.2 Sample Preparation
    9.2.2.3 Results and Discussion
    9.2.2.3.1 Stationary Absorption Spectrum
    9.2.2.3.2 Electronic Relaxation and Thermalization of Excited Population
    9.2.2.3.3 FT Spectra and Chirality Assignments
    9.2.2.3.4 CP Amplitudes of Chiral Systems
    9.2.2.3.5 Raman Processes in a Classical Model
    9.2.2.3.6 Raman and Raman-Like Processes in a Semiclassical Model
    9.2.2.3.7 Probe Photon Energy Dependence of the Vibrational Amplitudes
    9.2.2.3.8 Fitting the Amplitude Spectrum with Contributions from the Real and Imaginary Parts of the Third-Order Susceptibility
    9.2.2.3.9 Size and Meaning of the Contribution from the Real Part of the Third-Order Susceptibility
    9.2.2.3.10 RBMs Studied by the Moment Calculation
    9.2.2.4 Conclusions
    References
    Supplemental Material
    Supporting Information: Sample Morphology
    Chapter 9.2.3 Coherent Phonon Coupled with Exciton in Semiconducting Single-Walled Carbon Nanotubes Using a Few-Cycle Pulse Laser
    9.2.3.1 Introduction
    9.2.3.2 Experiment
    9.2.3.3 Results and Discussion
    9.2.3.3.1 Electronic Relaxation and Thermalization of Excited Population
    9.2.3.3.2 Fourier-Transform (FT) Spectra and Chirality Assignments
    9.2.3.3.3 Fitting the Amplitude Spectrum with Contributions from the Real and Imaginary Parts of the Third-Order Susceptibility
    9.2.3.4 Conclusions
    Acknowledgments
    References
    Chapter 9.2.4 Real-Time Spectroscopy of Single-Walled Carbon Nanotubes for Negative Time Delays by Using a Few-Cycle Pulse Laser
    9.2.4.1 Introduction
    9.2.4.2 Experimental Method
    9.2.4.2.1 Pump–Probe Experiment
    9.2.4.2.2 Sample Preparation
    9.2.4.3 Results and Discussion
    9.2.4.3.1 Stationary Absorption Spectrum
    9.2.4.3.2 Two-Dimensional (2D) Real-Time Vibration Spectra
    9.2.4.3.3 Electronic Phase Relaxation Time
    9.2.4.3.4 Fourier Transform Power Spectra and Probe Photon Energy-Dependent Amplitudes
    9.2.4.4 Conclusions
    References
    Section 9.3 1D Oligomers and Polymers
    Chapter 9.3.1 Fluorescence from Molecules and Aggregates in Polycrystalline Thin Films of α-Oligothiophenes
    9.3.1.1 Introduction
    9.3.1.2 Experiment
    9.3.1.3 Results and Discussion
    9.3.1.3.1 Absorption and Fluorescence Excitation Spectra
    9.3.1.3.2 Fluorescence Spectra
    9.3.1.3.3 Site-Selective Fluorescence Spectra
    9.3.1.3.4 Assignment of Fluorescence
    9.3.1.3.5 Time-Resolved Fluorescence Spectra
    9.3.1.4 Summary
    References
    Chapter 9.3.2 Sequential Singlet Internal Conversion of IB[sub(–)][sub(u)] → 3A[sub(–)][sub(g)] → IB[sub(–)][sub(u)] → 2A[sub(–)][sub(g)] → (IA[sub(–)][sub(g)] Ground) in All-Trans-Spirilloxanthin Revealed by Two-Dimensional Sub-5-fs Spectroscopy
    9.3.2.1 Introduction
    9.3.2.2 Experimental
    9.3.2.3 Results and Discussion
    9.3.2.3.1 Characterization of Femtosecond Time-Resolved Absorption Spectra: Identification of Sequential Internal Conversion
    9.3.2.3.1.1 Time-Resolved Absorption Spectra Near Zero Delay Time
    9.3.2.3.1.2 Time-Resolved Spectra with Positive Delay Times
    9.3.2.3.2 Analysis by SVD and Global-Fitting in the Framework of a Sequential Model
    9.3.2.3.3 Comparison with the Previous Results of Subpicosecond Time-Resolved Absorption Spectra
    References
    Chapter 9.3.3 Observation of Breather Exciton and Soliton in a Substituted Polythiophene with a Degenerate Ground State
    9.3.3.1 Introduction
    9.3.3.2 Experimental Descriptions
    9.3.3.3 Molecule Structure
    9.3.3.4 Quantum-Chemical Methodology
    9.3.3.5 Results and Discussion
    9.3.3.5.1 Electronic Relaxation and Molecular Vibration Dynamics
    9.3.3.5.2 Dynamics of Breather and Soliton
    9.3.3.6 Conclusions
    References
    Chapter 9.3.4 Ultrafast Electronic Relaxation and Vibrational Dynamics in a Polyacetylene Derivative
    9.3.4.1 Introduction
    9.3.4.2 Experimental
    9.3.4.2.1 Sample
    9.3.4.2.2 Ultrafast Spectroscopy
    9.3.4.3 Results and Discussion
    9.3.4.3.1 Delay Time Dependence of Difference Absorbance and Time-resolved Spectrum
    9.3.4.3.2 The Effect of the Electronic Transition Spectrum by Molecular Vibration
    9.3.4.3.3 Initial Phases of the Vibrational Modes Coupled to the Electronic Transition via Impulsive Excitation
    9.3.4.3.4 Vibrational-Energy Ladder Descending Process and Vibrational Phase Relaxation
    9.3.4.3.5 Electronic Phase Relaxation Obtained from the Data in the Negative Time Range
    9.3.4.4 Conclusions
    References
    Chapter 9.3.5 Ultrabroadband Time-Resolved Spectroscopy of Polymers
    9.3.5.1 Effect of Annealing on the Performance of P3HT: PCBM Solar Cells
    9.3.5.2 Conclusion and Perspectives
    References
    Section 9.4 2D Topological Materials
    Chapter 9.4.1 Ultrabroadband Time-Resolved Spectroscopy of Topological Insulators
    9.4.1.1 Introduction
    9.4.1.2 Broadband Time-Resolved Spectroscopy
    9.4.1.2.1 Development
    9.4.1.2.2 Femtosecond Light Sources
    9.4.1.2.2.1 Narrowband Optical Parametric Amplifier
    9.4.1.2.2.2 Broadband Optical Parametric Amplifier
    9.4.1.2.3 Pump–Probe Spectroscopy
    9.4.1.2.3.1 Fast-Scan Techniques
    9.4.1.2.3.2 Broadband Detection Techniques
    9.4.1.3 Ultrafast Dynamics in Novel Condensed Matter
    9.4.1.3.1 Spin-Valley Coupled Polarization in Monolayer MoS2
    9.4.1.4 Conclusion and Perspectives
    References
    Chapter 9.4.2 Phonon Dynamics in Cu[sub(x)]Bisub(2) and Bi[sub(2)]Se[sub(2)] Crystals Studied Using Ultrafast Spectroscopy
    9.4.2.1 Introduction
    9.4.2.2 Experimental
    9.4.2.3 Results and Discussion
    9.4.2.4 Conclusion
    References
    Chapter 9.4.3 Ultrafast Multi-Level Logic Gates with Spin-Valley Coupled Polarization Anisotropy in Monolayer MoS[sub(2)]
    9.4.3.1 Introduction
    References
    Chapter 9.4.4 Femtosecond Time-Evolution of Mid-Infrared Spectral Line Shapes of Dirac Fermions in Topological Insulators
    9.4.4.1 Introduction
    9.4.4.2 Experimental
    9.4.4.3 Results
    9.4.4.3.1 Ultra-Broadband MIR ΔR/R Spectra of FCA and SSTs in Topological Insulators
    9.4.4.3.2 Quantitative Analysis of the Ultra-Broadband MIR ΔR/R Spectra
    9.4.4.3.2.1 Ultrafast Time-Evolution of the Ultra-Broadband MIR ΔR/R Spectra
    9.4.4.4 Discussion
    References
    Section 10 Conductors and Superconductors
    Section 10.1 Super Conductors
    Chapter 10.1.1 Dichotomy of Photoinduced Quasiparticle on CuO[sub(2)] Planes of YB[sub(2)]Cu[sub(3)]O[sub(7)] Directly Revealed by Femtosecond Polarization Spectroscopy
    10.1.1.1 Introduction
    10.1.1.2 Experiment
    10.1.1.3 Results and Discussion
    References
    Chapter 10.1.2 Ultrafast Dynamics and Phonon Softening in Fe[sub(1+y)]Se[sub(1–x)]Te[sub(x)] Single Crystals
    10.1.2.1 Introduction
    10.1.2.2 Experiments
    10.1.2.3 Temperature-Dependent ΔR/R
    10.1.2.4 Electron–Optical Phonon Coupling Strength
    10.1.2.5 Acoustic Phonon Softening
    10.1.2.6 Summary
    References
    Chapter 10.1.3 Quasiparticle Dynamics in FeSe Superconductors Studied by Femtosecond Spectroscopy
    10.1.3.1 Introduction
    10.1.3.2 Experiments
    10.1.3.3 Results and Discussion
    10.1.3.4 Summary
    References
    Section 10.2 THZ, MIR Spectroscopy of Materials
    Chapter 10.2.1 Dirac Fermions Near the Dirac Point in Topological Insulators
    10.2.1.1 Introduction
    10.2.1.2 Results and Discussion
    10.2.1.3 Conclusion
    References
    Chapter 10.2.2 Helicity-Dependent Terahertz Emission Spectroscopy of Topological Insulator
    10.2.2.1 Introduction
    10.2.2.2 Experiments
    10.2.2.3 Results and Discussion
    10.2.2.4 Summary and Conclusions
    Appendix A: Sample Preparation and Terahertz Emission Measurement
    Appendix B: Time-Domain Fits for the Helicity-Dependent Terahertz Radiation at ϕ = 0° and 90°
    Appendix C: Dependence of Circular
    Appendix D: Time-Domain Decomposition and Recombination of the α-Dependent Terahertz Waveforms at ϕ = 90°
    Appendix E: Estimation of the Terahertz-Emission Spectra for Dirac Fermions by Using Photoemission Dynamics from Time-Resolved ARPES Measurements
    Appendix F: Helicity-Independent Terahertz Radiation from a <110>ZnTe Single Crystal
    References
    Chapter 10.2.3 Femtosecond Time-Evolution of Mid-Infrared Spectral Line Shapes of Dirac Fermions in Topological Insulators
    10.2.3.1 Results
    10.2.3.2 Discussion
    10.2.3.3 Methods
    References
    Chapter 10.2.4 Ultrafast Carrier Dynamics in Ge by Ultra-Broadband Mid-Infrared Probe Spectroscopy
    10.2.4.1 Experiments
    10.2.4.2 Results and Discussion
    10.2.4.3 Summary
    References
    Section 11 Chemical Reactions and Material Processing
    Section 11.1 Chemical Reactions
    Chapter 11.1.1 Transition State in a Prevented Proton Transfer Observed in Real Time
    11.1.1.1 Introduction
    11.1.1.2 Experimental
    11.1.1.3 Results and Discussion
    11.1.1.3.1 Investigation of Reaction Mechanisms of Proton Transfer (Theory)
    11.1.1.4 Direct Observation of Transition State (Methanol Solution of Indigodisulfonate Salt)
    11.1.1.5 Comparison Between Experimental Results and Theoretical Results TD-B3LYP/6-311++G//B3LYP/6311++G
    11.1.1.6 Conclusion
    Supporting Information
    References
    Chapter 11.1.2 Environment-Dependent Ultrafast Photoisomerization Dynamics in Azo Dye
    11.1.2.1 Introduction
    11.1.2.2 Experimental Section
    11.1.2.3 Results and Discussion
    11.1.2.4 Summary
    References
    Chapter 11.1.3 Direct Observation of Denitrogenation Process of 2,3-diazabicyclo [2.2.1] hept-2-ene (DBH) Derivatives, Using a Visible 5-fs Pulse Laser
    11.1.3.1 Introduction
    11.1.3.2 Experimental
    11.1.3.3 Results and Discussion
    11.1.3.3.1 Pump–Probe Experimental Results
    11.1.3.3.2 Spectrogram
    11.1.3.3.3 Denitrogenation Mechanism
    11.1.3.4 Conclusion
    References
    Chapter 11.1.4 Photo-Impulsive Reactions in the Electronic Ground State Without Electronic Excitation: Non-Photo, Non-Thermal Chemical Reactions
    11.1.4.1 Introduction
    11.1.4.2 Experimental
    11.1.4.2.1 Few-Optical-Cycle Ultraviolet Pulses
    11.1.4.2.2 Few-Optical-Cycle Visible Pulses
    11.1.4.2.3 Sample Cell
    11.1.4.2.4 Pump–Probe Measurement
    11.1.4.2.5 Quantum Chemical Calculation
    11.1.4.3 Results
    11.1.4.3.1 Vibrational Dynamics in the Reaction Under Few-Optical Cycle Ultraviolet Pulse Irradiation (See Figure 11.1.4.1a)
    11.1.4.3.2 Vibrational Dynamics in the Reaction Under Few-Optical Cycle Visible Pulse Irradiation (See Figure 11.1.4.1c)
    11.1.4.3.3 Theoretical Vibrational Dynamics of the Photo- and Thermal Reactions
    11.1.4.4 Discussion
    11.1.4.4.1 Photochemically-Allowed Claisen Rearrangement of Allyl Phenyl Ether by Few-Optical-Cycle Ultraviolet Pulse Irradiation
    11.1.4.4.2 Thermally-Allowed Claisen Rearrangement of Allyl Phenyl Ether by Few-Optical-Cycle Visible Pulse Irradiation
    11.1.4.4.3 Non-Photo, Non-Thermal Chemical Reaction
    11.1.4.5 Conclusions
    References
    Chapter 11.1.5 The Reaction Mechanism of Claisen Rearrangement Obtained by Transition State Spectroscopy and Single Direct-Dynamics Trajectory
    11.1.5.1 Introduction
    11.1.5.2 Results and Discussions
    11.1.5.2.1 Transition State Spectroscopy of the Claisen Rearrangement of Allyl Vinyl Ether
    11.1.5.2.2 Single Direct-Dynamics Trajectory
    11.1.5.3 Experimental
    11.1.5.3.1 Visible 5-fs Laser System
    11.1.5.3.2 "The Reaction in the Electronic Ground State", Triggered by the Visible 5-fs Pulse
    11.1.5.4 Conclusions
    References
    Chapter 11.1.6 A New Reaction Mechanism of Claisen Rearrangement Induced by Few-Optical-Cycle Pulses: Demonstration of Nonthermal Chemistry by Femtosecond Vibrational Spectroscopy
    11.1.6.1 Introduction
    11.1.6.2 Experimental
    11.1.6.2.1 Visible Few-Optical-Cycle Pulses
    11.1.6.2.2 Ultraviolet Few-Optical-Cycle Pulses
    11.1.6.2.3 Sample Cell
    11.1.6.2.4 Pump–Probe Measurement
    11.1.6.2.5 Theoretical Calculation
    11.1.6.3 Results and Discussion
    11.1.6.3.1 Claisen Rearrangement of Allyl Vinyl Ether
    11.1.6.3.2 Claisen Rearrangement of Allyl Phenyl Ether
    11.1.6.3.3 "Nonphoto Nonthermal Claisen Rearrangement" and Thermal Claisen Rearrangement
    11.1.6.4 Conclusion
    References
    Section 11.2 Material Processing
    Chapter 11.2.1 Magnetization Dynamics and the Mn[sup(3+)] d-d Excitation of Hexagonal HoMnO[sub(3)] Single Crystals Using Wavelength-Tunable Time-Resolved Femtosecond Spectroscopy
    11.2.1.1 Introduction
    11.2.1.2 Experiments
    11.2.1.3 Results and Discussion
    11.2.1.4 Summary
    References
    Chapter 11.2.2 Ultrafast Thermoelastic Dynamics of HoMnO[sub(3)] Single Crystals Derived from Femtosecond Optical Pump – Probe Spectroscopy
    11.2.2.1 Introduction
    11.2.2.2 Experiments
    11.2.2.3 Results and Discussion
    11.2.2.3.1 Temperature- and Wavelength-Dependent ΔR/R
    11.2.2.3.2 Attribution of the Negative Component in ΔR/R
    11.2.2.3.3 Attribution of the Oscillation Component in ΔR/R
    11.2.2.4 Conclusion
    References
    Chapter 11.2.3 Ultrafast Photoinduced Mechanical Strain in Epitaxial BiFeO[sub(3)] Thin Films
    11.2.3.1 Introduction
    11.2.3.2 Experimental
    11.2.3.3 Results and Discussion
    11.2.3.4 Conclusion
    References
    Chapter 11.2.4 Femtosecond Laser-Induced Formation of Wurtzite Phase ZnSe Nanoparticles in Air
    11.2.4.1 Introduction
    11.2.4.2 Experimental
    11.2.4.3 Results and Discussion
    11.2.4.4 Conclusion
    References
    Chapter 11.2.5 Controllable Subwavelength-Ripple and -Dot Structures on YBa[sub(2)]Cu[sub(3)]O[sub(7)] Induced by Ultrashort Laser Pulses
    11.2.5.1 Introduction
    11.2.5.2 Experiments
    11.2.5.3 Results and Discussion
    11.2.5.4 Summary
    References
    Section 12 Photobiological Reactions
    Chapter 12.1 Real-Time Vibrational Dynamics in Chlorophyll a Studied with a Few-Cycle Pulse Laser
    12.1.1 Introduction
    12.1.2 Materials and Methods
    12.1.3 Results and Discussion
    12.1.3.1 Stationary Absorption and Fluorescence Spectra and Time-Resolved Difference Absorption Spectrum
    12.1.3.2 Ultrafast Dynamics of Vibrational Modes
    12.1.4 Theory and Discussion
    12.1.5 Conclusions
    Supporting Material
    References
    Chapter 12.2 Time-Resolved Spectroscopy of Ultrafast Photoisomerization of Octopus Rhodopsin Under Photoexcitation
    12.2.1 Introduction
    12.2.2 Experimental Methods
    12.2.2.1 Femtosecond Spectroscopy Apparatus
    12.2.2.2 Octopus Rh
    12.2.3 Results and Discussion
    12.2.3.1 Electronic Dynamics
    12.2.3.2 Vibration Dynamics
    12.2.4 Conclusions
    References
    Chapter 12.3 Schiff Base Proton Acceptor Assists Photoisomerization of Retinal Chromophores in Bacteriorhodopsin
    12.3.1 Introduction
    12.3.2 Materials and Methods
    12.3.2.1 Chemicals Used in This Study
    12.3.2.2 Plasmid Constructions
    12.3.2.3 Primers Used for Mutant Constructions
    12.3.2.4 Protein Purification
    12.3.2.5 Flash-Laser-Induced Photocycle Measurement
    12.3.2.6 Fast-Scan Transient Absorption Spectroscopy
    12.3.2.7 Visible Broadband Sub-10-Fs Pulse
    12.3.2.8 Software Employed in This Study
    12.3.3 Results and Discussion
    12.3.3.1 Sequence Alignment of HwBR and Other BRs
    12.3.3.2 Protein Constructions, Expression, Purification, and Ultraviolet-Visible Maximum Absorbance of Wild-Type, D93N, and D104N
    12.3.3.3 Ground-State Photocycle of Wild-Type, D93N, and D104N
    12.3.3.4 Transient Absorption Spectroscopy of Wild-Type and Mutants of HwBR
    12.3.3.5 Global Fitting Using the Triple-Exponential Function
    12.3.3.6 Femtosecond 2D-CS
    12.3.3.7 Picosecond 2D-CS
    12.3.3.8 Transient Absorption Spectroscopy of Wild-Types of HwBR, HmBRI, and HmBRII
    12.3.3.9 Global Fitting Using the Triple-Exponential Function
    12.3.3.10 Femtosecond 2D-CS
    12.3.3.11 Picosecond 2D-CS
    12.3.4 Conclusions
    References


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