Table Of ContentUltrashort 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
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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
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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
