Ultrashort Pulse Lasers and Ultrafast Phenomena This book describes the basic physical principles and structure of the special technique used to obtain such ultrashort pulse lasers. It introduces the basics of non-linear optics that provides their generation and measurement and provides application examples of ultrafast spectroscopy to solid-state materials. The chapters explains the basic physical principles of ultrashort pulse laser construction and describes the detailed structure of the world's shortest visible laser and DUV lasers. Finally, it also provides several examples of the applications of ultrafast spectroscopy to solid-state materials. Ultrashort Pulse Lasers and Ultrafast Phenomena Takayoshi Kobayashi Designed cover image: Takayoshi Kobayashi First edition published 2023 by CRC Press 6000 Broken Sound Parkway NW, Suite 300, Boca Raton, FL 33487-2742 and by CRC Press 4 Park Square, Milton Park, Abingdon, Oxon, OX14 4RN CRC Press is an imprint of Taylor & Francis Group, LLC © 2023 Taylor & Francis Group, LLC Reasonable efforts have been made to publish reliable data and information, but the author and publisher cannot assume responsibility for the validity of all materials or the consequences of their use. The authors and p ublishers have attempted to trace the copyright holders of all material reproduced in this publication and apologize to copyright holders if permission to publish in this form has not been obtained. If any copyright material has not been acknowledged please write and let us know so we may rectify in any future reprint. 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ISBN: 978-0-367-18471-1 (hbk) ISBN: 978-1-032-41172-9 (pbk) ISBN: 978-0-429-19657-7 (ebk) DOI: 10.1201/9780429196577 Typeset in Times by codeMantra Contents Preface..........................................................................................................................................xxiii Author ............................................................................................................................................xxv Section 1 G eneration 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−1 Bandwidth ............................................................5 References ...............................................................................................................9 Chapter 1.1.2 Simultaneous Compression and Amplification of a Laser Pulse in a Glass Plate.............................................................................................................11 1.1.2.1 Introduction ............................................................................................11 1.1.2.2 Principle .................................................................................................11 1.1.2.3 Experimental Setup ................................................................................12 1.1.2.4 Experimental Results and Discussion ....................................................13 1.1.2.5 Conclusion..............................................................................................16 References .............................................................................................................16 Chapter 1.1.3 Pulse-Front-Matched Optical Parametric Amplification for Sub-10-fs Pulse Generation Tunable in the Visible and Near Infrared ..........................................19 1.1.3.1 Introduction ............................................................................................19 1.1.3.2 Experimental ..........................................................................................19 1.1.3.3 Results and Discussion ...........................................................................20 1.1.3.4 Conclusion..............................................................................................22 References .............................................................................................................23 Chapter 1.1.4 Visible 4 fs Pulse from Dispersion Control Optical Parametric Amplifier ..........25 1.1.4.1 I ntroduction ..............................................................................................25 1.1.4.2 Configuration of the System.....................................................................26 1.1.4.3 Analysis and Discussion ...........................................................................28 1.1.4.4 C onclusion................................................................................................28 References .............................................................................................................29 Chapter 1.1.5 Ultrafast Laser System Based on Noncollinear Optical Parametric Amplification for Laser Spectroscopy ..................................................................31 1.1.5.1 I ntroduction ............................................................................................31 1.1.5.2 Experimental ..........................................................................................32 1.1.5.3 Results and Discussion ...........................................................................32 v vi Contents 1.1.5.4 Conclusion..............................................................................................34 References .............................................................................................................35 Chapter 1.1.6 Development of Ultrashort Pulse Lasers for Ultrafast Spectroscopy ...................37 1.1.6.1 I ntroduction ............................................................................................37 1.1.6.2 Light Sources for Studying Ultrafast Processes .....................................38 1.1.6.3 Electronic Relaxation and Vibrational Dynamics ..................................38 1.1.6.4 Principles and Advantages of Broad-Band Ultrafast Spectroscopy .......39 1.1.6.5 Ultrashort Visible Pulse Generation Based on Non-Linear Optical Parametric Amplifier (NOPA) ................................................................40 1.1.6.6 Ultrashort Deep Ultraviolet Laser ..........................................................42 1.1.6.6.1 DUV Pulse Generation ........................................................42 1.1.6.6.2 Sub-10 fs DUV Laser Pulse Obtained by Broad-Band CPFWM ...............................................................................43 1.1.6.6.3 DUV Pulse Stability Optimization.......................................44 1.1.6.7 C onclusion..............................................................................................45 References .............................................................................................................45 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 ......................................................................................51 1.2.1.1 I ntroduction ............................................................................................51 1.2.1.2 E xperimental Setup ................................................................................51 1.2.1.3 Experimental Results and Discussion ....................................................52 1.2.1.4 C onclusion..............................................................................................57 References .............................................................................................................57 Chapter 1.2.2 Sub-10 fs Deep-Ultraviolet Pulses Generated by Chirped-Pulse Four-Wave Mixing ..................................................................................................................59 1.2.2.1 Introduction ............................................................................................59 1.2.2.2 Experimental ..........................................................................................60 1.2.2.3 Results and Discussion ...........................................................................60 1.2.2.4 Conclusion..............................................................................................62 References .............................................................................................................62 Chapter 1.2.3 Generation and Optimization of Femtosecond Pulses by Four-Wave Mixing Process ..................................................................................................................63 1.2.3.1 I ntroduction ............................................................................................63 1.2.3.2 Cascaded FWM in Bulk Media ..............................................................64 1.2.3.2.1 Principle of Cascaded FWM ................................................64 1.2.3.2.2 Generation of Wavelength-Tunable Self-Compressed Multicolored Pulses by Nondegenerate Cascaded FWM ....65 1.2.3.2.3 Pulse Cleaning by Degenerate Cascaded FWM ..................67 Contents vii 1.2.3.3 UV Pulse Generation by FWM in Hollow Fiber....................................70 1.2.3.3.1 Chirped-Pulse FWM in a Gas-Filled Hollow Waveguide ....71 1.2.3.3.2 Broadband Chirped-Pulse FWM ..........................................72 1.2.3.3.3 Practical Issues in Broadband Chirped-Pulse FWM ............73 1.2.3.3.4 Sub-10-fs DUV Pulses Generated by Broadband Chirped-Pulse FWM ............................................................74 1.2.3.4 Four-Wave Optical Parametric Amplification (FWOPA) in Bulk Media......................................................................................................75 1.2.3.5 Conclusion and Prospects ......................................................................77 References .............................................................................................................78 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 . ...............................................................85 2 2.1.1 Introduction .................................................................................................85 2.1.2 Derivation of the Sellmeier Dispersion .......................................................86 2.1.3 Generation of Terahertz Radiation with a Nd:YAG Laser ...........................87 2.1.4 Generation of Terahertz Radiation with CO Lasers ...................................88 2 2.1.5 Discussion ....................................................................................................89 2.1.6 Conclusion ...................................................................................................89 References ...............................................................................................................90 Chapter 2.2 Saturation of the Free Carrier Absorption in ZnTe Crystals ...................................91 2.2.1 Introduction .................................................................................................91 2.2.2 Experiments .................................................................................................91 2.2.2.1 THz Generation in ZnTe Crystals .................................................91 2.2.2.2 Photoluminescence Radiated from ZnTe Crystals ........................94 2.2.3 Discussion ....................................................................................................94 2.2.4 Conclusion ...................................................................................................97 References ...............................................................................................................98 Chapter 2.3 Widely Linear and Non-Phase-Matched Optical-to-Terahertz Conversion on GaSe: Te Crystals ..................................................................................................101 2.3.1 Introduction ..............................................................................................101 2.3.2 Experimental ..............................................................................................101 2.3.3 Results and Discussions ...........................................................................102 2.3.4 Conclusion ................................................................................................104 References .............................................................................................................105 Chapter 2.4 THz Emission from Organic Cocrystalline Salt: An Example of 2,6-Diaminopyridinium-4-Nitrophenolate-4-Nitrophenol ....................................107 2.4.1 Introduction ...............................................................................................107 2.4.2 Sample Preparation and THz Emission Experiments ................................107 2.4.3 Results and Discussion ..............................................................................108 2.4.4 Summary ....................................................................................................111 References .............................................................................................................111 viii Contents 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 .......................................................................................................115 3.1.1 Introduction ..............................................................................................115 3.1.2 Experimental ..............................................................................................115 3.1.3 Conclusion .................................................................................................118 References .............................................................................................................118 Chapter 3.2 Self-Stabilization of the Carrier-Envelope Phase of an Optical Parametric Amplifier Verified with a Photonic Crystal Fiber .................................................121 3.2.1 Introduction ..............................................................................................121 3.2.2 Experimental .............................................................................................122 3.2.3 Results and Discussion .............................................................................122 3.2.4 Conclusion .................................................................................................124 References .............................................................................................................124 Chapter 3.3 Octave-Spanning Carrier-Envelope Phase Stabilized Visible Pulse with Sub-3-fs Pulse Duration .........................................................................................127 3.3.1 Introduction ...............................................................................................127 3.3.2 Results and Discussion ..............................................................................127 3.3.3 Conclusion .................................................................................................130 References .............................................................................................................130 Chapter 3.4 Carrier-Envelope-Phase-Stable, Intense Ultrashort Pulses in Near Infrared ........133 3.4.1 Introduction ..............................................................................................133 3.4.2 Experimental ..............................................................................................134 3.4.3 Results and Discussion ..............................................................................134 3.4.4 Conclusion .................................................................................................136 References .............................................................................................................136 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 ...............................................................................................141 4.1.1 Introduction ...............................................................................................141 4.1.2 Experimental ..............................................................................................141 4.1.3 Results and Discussion ..............................................................................141 4.1.4 Conclusion .................................................................................................144 References .............................................................................................................145 Contents ix Chapter 4.2 Femtosecond Pulses Cleaning by Transient-Grating Process in Optical Media ...147 4.2.1 Introduction ...............................................................................................147 4.2.2 Experimental ..............................................................................................148 4.2.3 Results and Discussion ..............................................................................149 4.2.4 Conclusion .................................................................................................150 References .............................................................................................................150 Chapter 4.3 Non-Degenerate Two-Photon Absorption Enhancement for Laser Dyes by Precise Lock-in Detection .....................................................................................153 4.3.1 Introduction ...............................................................................................153 4.3.2 Theory ........................................................................................................154 4.3.3 Experimental Procedures ...........................................................................155 4.3.4 Results and Discussion ..............................................................................156 4.3.5 Conclusion .................................................................................................161 References .............................................................................................................162 Section 5 Multi-color involved nLo Processes Chapter 5.1 Generation of μJ-Level Multicolored Femtosecond Laser Pulses Using Cascaded Four-Wave Mixing .................................................................................167 5.1.1 Introduction ...............................................................................................167 5.1.2 Experimental Setup ...................................................................................167 5.1.3 Experimental Results and Discussion .......................................................168 5.1.4 Conclusion .................................................................................................171 References .............................................................................................................171 Chapter 5.2 G eneration and Optimization of Femtosecond Pulses by Four-Wave Mixing (FWM) Process .....................................................................................................173 5.2.1 I ntroduction ...............................................................................................173 5.2.2 Cascaded FWM in Bulk Media .................................................................174 5.2.2.1 Principle of Cascaded Four-Wave Mixing (FWM) ....................174 5.2.2.2 Generation of Wavelength-Tunable Self-Compressed Multicolored Pulses by Nondegenerate Cascaded FWM ...........175 5.2.2.3 Pulse Cleaning by Degenerate Cascaded FWM .........................177 5.2.3 UV Pulse Generation by FWM in Hollow Fiber .......................................180 5.2.3.1 Chirped-Pulse FWM in a Gas-Filled Hollow Waveguide ..........180 5.2.3.2 Broadband Chirped-Pulse FWM ................................................182 5.2.3.3 Practical Issues in Broadband Chirped-Pulse FWM ..................183 5.2.3.4 Sub-10-fs DUV Pulses Generated by Broadband Chirped-Pulse FWM ...................................................................184 5.2.4 FWOPA in Bulk Media .............................................................................185 5.2.5 Conclusion and Prospects ..........................................................................186 References .............................................................................................................187 Chapter 5.3 Tunable Multicolored Femtosecond Laser Pulses Generation by Using Cascaded Four-Wave Mixing (CFWM) in Bulk Materials ...................................193 5.3.1 Introduction ...............................................................................................193