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 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.

Except as permitted under U.S. Copyright Law, no part of this book may be reprinted, reproduced, transmitted, or
utilized in any form by any electronic, mechanical, or other means, now known or hereafter invented, ­including
­photocopying, microfilming, and recording, or in any information storage or retrieval system, without written
­permission from the publishers.

For permission to photocopy or use material electronically from this work, access www.copyright.com or contact the
Copyright Clearance Center, Inc. (CCC), 222 Rosewood Drive, Danvers, MA 01923, 978-750-8400. For works that are
not available on CCC please contact [email protected]

Trademark notice: Product or corporate names may be trademarks or registered trademarks and are used only for
identification and explanation without intent to infringe.

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 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−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 Introduction ..............................................................................................25
1.1.4.2 Configuration of the System.....................................................................26
1.1.4.3 Analysis and Discussion...........................................................................28
1.1.4.4 Conclusion................................................................................................28
References ............................................................................................................. 29

Chapter 1.1.5 Ultrafast Laser System Based on Noncollinear Optical Parametric

Amplification for Laser Spectroscopy .................................................................. 31
1.1.5.1 Introduction ............................................................................................ 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 Introduction
 ............................................................................................ 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 Conclusion.............................................................................................. 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 Introduction ............................................................................................ 51
1.2.1.2 Experimental Setup ................................................................................ 51
1.2.1.3 Experimental Results and Discussion .................................................... 52
1.2.1.4 Conclusion.............................................................................................. 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 Introduction ............................................................................................ 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 ZnGeP2................................................................. 85
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 CO2 Lasers.................................... 88
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 Generation and Optimization of Femtosecond Pulses by Four-Wave Mixing

(FWM) Process ..................................................................................................... 173
5.2.1 Introduction
 ............................................................................................... 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
x Contents

5.3.2 Theoretical Analysis .................................................................................. 194

5.3.2.1 FWM Process ............................................................................. 194
5.3.2.2 CFWM Process ........................................................................... 195
5.3.3 Experimental Characteristics of Multicolored Pulses ............................... 196
5.3.3.1 Experimental Setups ................................................................... 196
5.3.3.2 Spectra and Wavelength Tuning of Multicolored Sidebands...... 199
5.3.3.2.1 Tuning the Wavelength of Sidebands by
Changing Cross-Angle .............................................199
5.3.3.2.2 Tuning the Wavelength of Sidebands by
Changing Nonlinear Media ...................................... 199
5.3.3.3 Temporal Characteristics of Multicolored Pulses .......................200
5.3.3.4 Output Power/Energy of Multicolored Pulses ............................ 201
5.3.3.5 Multicolored Sidebands Generated with Low Threshold ...........203
5.3.4 2-D Multicolored Sidebands Arrays .......................................................... 205
5.3.5 Conclusion and Prospects ..........................................................................208
References .............................................................................................................208

Chapter 5.4 Mechanism Study of 2-D Laser Array Generation in a YAG Crystal Plate.......... 213
5.4.1 Introduction ............................................................................................... 213
5.4.2 Numerical Simulation Model .................................................................... 213
5.4.3 Results and Discussion .............................................................................. 215
5.4.4 Conclusion ................................................................................................. 217
References ............................................................................................................. 217

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......................... 221
6.1.1 Introduction ............................................................................................... 221
6.1.2 Experimental.............................................................................................. 221
6.1.3 Results and Discussion .............................................................................. 221
6.1.4 Conclusion ................................................................................................ 225
References ............................................................................................................. 225

Chapter 6.2 Generation of Broadband Two-Dimensional Multicolored Arrays in a

Sapphire Plate ........................................................................................................ 227
6.2.1 Experimental
 .............................................................................................. 227
6.2.2 Experimental Setup ................................................................................... 227
6.2.3 Experimental Results and Discussion ....................................................... 228
6.2.4 Conclusion ................................................................................................. 232
References ............................................................................................................. 232

Section 7 nLo Materials

Chapter 7.1 Sellmeier Dispersion for Phase-Matched Terahertz Generation in ZnGeP2 .......... 235
Contents xi

7.1.1 Introduction................................................................................................ 235

7.1.2 Derivation of the Sellmeier Dispersion...................................................... 236
7.1.3 Generation of Terahertz Radiation with a Nd:YAG Laser.......................... 237
7.1.4 Generation of Terahertz Radiation with CO2 Lasers.................................. 238
7.1.5 Discussion................................................................................................... 239
7.1.6 Conclusion.................................................................................................. 239
References..............................................................................................................240

Chapter 7.2 
Broadband Sum-Frequency Mixing (SFM) in Some Recently Developed
Nonlinear Optical Crystals..................................................................................... 241
7.2.1 Introduction................................................................................................ 241
7.2.2 Schematic of the Experimental Arrangement............................................. 242
7.2.3 Theoretical Background of Phase Matching and Broadband SFM............ 243
7.2.4 Results and Discussion...............................................................................244
7.2.5 Broadly Tunable Conventional SFM in a Thin Crystal..............................246
7.2.6 Conclusion.................................................................................................. 247
References.............................................................................................................. 249

Chapter 7.3 Optimal Te-Doping in GaSe for Nonlinear Applications....................................... 251

7.3.1 Introduction................................................................................................ 251
7.3.2 Crystal Growth and Characterization......................................................... 252
7.3.2.1 Growth Technology..................................................................... 252
7.3.2.2 Optical Properties........................................................................ 253
7.3.2.3 THz Generation via Optical Rectification................................... 256
7.3.3 Discussion................................................................................................... 257
7.3.4 Conclusion.................................................................................................. 258
References.............................................................................................................. 258

Chapter 7.4 
Widely Linear and Non-Phase-Matched Optical-to-Terahertz Conversion on
GaSe: Te Crystals.................................................................................................... 261
7.4.1 Introduction................................................................................................ 261
7.4.2 Experimental............................................................................................... 261
7.4.3 Results and Discussion............................................................................... 262
7.4.4 Conclusion.................................................................................................. 265
References.............................................................................................................. 265

Section 8 NLO Processes in Time-Resolved Spectroscopy

Chapter 8.1 
Elimination of Coherence Spike in Reflection-Type Pump-Probe
Measurements......................................................................................................... 269
8.1.1 Introduction................................................................................................ 269
8.1.2 Experiments................................................................................................ 269
8.1.3 Results and Discussion............................................................................... 270
8.1.4 Summary..................................................................................................... 273
References.............................................................................................................. 274
xii Contents

Chapter 8.2 Vibrational Fine Structures Revealed by the Frequency-to-Time Fourier

Transform of the Transient Spectrum in Bacteriorhodopsin ................................. 275
8.2.1 Introduction ............................................................................................... 275
8.2.2 Experimental Section................................................................................. 276
8.2.3 Results and Discussion .............................................................................. 276
8.2.4 Conclusions ............................................................................................... 281
References ............................................................................................................. 282

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 .......................................... 287
9.1.1.1 Introduction .......................................................................................... 287
9.1.1.2 Experiments.......................................................................................... 288
9.1.1.3 Results and Discussion......................................................................... 289
9.1.1.4 Conclusion............................................................................................ 295
References ........................................................................................................... 296

Chapter 9.1.2 Observation of an Excitonic Quantum Coherence in CdSe Nanocrystals ......... 299
9.1.2.1 Introduction .......................................................................................... 299
9.1.2.2 Experimental ........................................................................................ 299
9.1.2.3 Results and Discussion.........................................................................300
9.1.2.4 Conclusion............................................................................................307
Supporting Information .......................................................................................308
References ...........................................................................................................309

Section 9.2 1D cnt

Chapter 9.2.1 Coherent Phonon Generation in Semiconducting Single-Walled Carbon

Nanotubes Using a Few-Cycle Pulse Laser ........................................................ 313
9.2.1.1 Introduction .......................................................................................... 313
9.2.1.2 Experimental Details ............................................................................ 314
9.2.1.3 Results and Discussion......................................................................... 314
9.2.1.3.1 Stationary Absorption Spectrum of the Sample and
Laser Spectrum .................................................................. 314
9.2.1.3.2 Two-Dimensional (2D) Real-Time Spectra and Exact
Chirality Assignment ......................................................... 314
9.2.1.3.3 Probe Photon Energy Dependent Amplitude Profiles ........ 315
9.2.1.4 Conclusion............................................................................................ 319
References ........................................................................................................... 319
Contents xiii

Chapter 9.2.2 
Electronic Relaxation and Coherent Phonon Dynamics in Semiconducting
Single-Walled Carbon Nanotubes with Several Chiralities................................ 321
9.2.2.1 Introduction.......................................................................................... 321
9.2.2.2 Experiment........................................................................................... 323
9.2.2.2.1  Ultrafast Spectroscopy..................................................... 323
9.2.2.2.2  Sample Preparation.......................................................... 323
9.2.2.3 Results and Discussion......................................................................... 324
9.2.2.3.1  Stationary Absorption Spectrum...................................... 324
9.2.2.3.2  Electronic Relaxation and Thermalization of
Excited Population����������������������������������������������������������326
9.2.2.3.3  FT Spectra and Chirality Assignments............................. 328
9.2.2.3.4  CP Amplitudes of Chiral Systems.................................... 330
9.2.2.3.5  Raman Processes in a Classical Model............................ 331
9.2.2.3.6  Raman and Raman-Like Processes in a
Semiclassical Model�������������������������������������������������������332
9.2.2.3.7  Probe Photon Energy Dependence of the Vibrational
Amplitudes���������������������������������������������������������������������� 334
9.2.2.3.8  Fitting the Amplitude Spectrum with Contributions
from the Real and Imaginary Parts of the
Third-Order Susceptibility����������������������������������������������336
9.2.2.3.9  Size and Meaning of the Contribution from the Real
Part of the Third-Order Susceptibility�����������������������������338
9.2.2.3.10  RBMs Studied by the Moment Calculation.....................340
9.2.2.4 
Conclusions........................................................................................... 342
References............................................................................................................ 342
Supplemental Material.........................................................................................344
Supporting Information: Sample Morphology.....................................344

Chapter 9.2.3 
Coherent Phonon Coupled with Exciton in Semiconducting Single-Walled
Carbon Nanotubes Using a Few-Cycle Pulse Laser............................................ 345
9.2.3.1 Introduction.......................................................................................... 345
9.2.3.2 Experiment...........................................................................................346
9.2.3.3 Results and Discussion.........................................................................346
9.2.3.3.1  Electronic Relaxation and Thermalization of Excited
Population�������������������������������������������������������������������������346
9.2.3.3.2  Fourier-Transform (FT) Spectra and Chirality
Assignments���������������������������������������������������������������������� 347
9.2.3.3.3  Fitting the Amplitude Spectrum with Contributions
from the Real and Imaginary Parts of the Third-Order
Susceptibility���������������������������������������������������������������������348
9.2.3.4 Conclusions..........................................................................................348
Acknowledgments............................................................................................... 349
References........................................................................................................... 350

Chapter 9.2.4 
Real-Time Spectroscopy of Single-Walled Carbon Nanotubes for Negative
Time Delays by Using a Few-Cycle Pulse Laser................................................. 351
9.2.4.1 Introduction.......................................................................................... 351
9.2.4.2 Experimental Method........................................................................... 352
xiv Contents

9.2.4.2.1  Pump–Probe Experiment................................................... 352

9.2.4.2.2  Sample Preparation............................................................ 352
9.2.4.3 
Results and Discussion......................................................................... 352
9.2.4.3.1  Stationary Absorption Spectrum ....................................... 352
9.2.4.3.2  Two-Dimensional (2D) Real-Time Vibration Spectra........ 353
9.2.4.3.3  Electronic Phase Relaxation Time..................................... 356
9.2.4.3.4  Fourier Transform Power Spectra and Probe Photon
Energy-Dependent Amplitudes����������������������������������������� 359
9.2.4.4 
Conclusions.......................................................................................... 362
References........................................................................................................... 363

Section 9.3 1D Oligomers and Polymers

Chapter 9.3.1 
Fluorescence from Molecules and Aggregates in Polycrystalline Thin
Films of α-Oligothiophenes................................................................................. 369
9.3.1.1 Introduction.......................................................................................... 369
9.3.1.2 Experiment........................................................................................... 370
9.3.1.3 Results and Discussion......................................................................... 370
9.3.1.3.1  Absorption and Fluorescence Excitation Spectra............... 370
9.3.1.3.2  Fluorescence Spectra.......................................................... 372
9.3.1.3.3  Site-Selective Fluorescence Spectra................................... 374
9.3.1.3.4  Assignment of Fluorescence.............................................. 375
9.3.1.3.5  Time-Resolved Fluorescence Spectra................................ 376
9.3.1.4 Summary.............................................................................................. 379
References........................................................................................................... 380

Sequential Singlet Internal Conversion of IB–u → 3A–g → IB–u → 2A–g →

Chapter 9.3.2 
(IA–g Ground) in All-Trans-Spirilloxanthin Revealed by Two-Dimensional
Sub-5-fs Spectroscopy......................................................................................... 383
9.3.2.1 
Introduction.......................................................................................... 383
9.3.2.2 
Experimental........................................................................................ 385
9.3.2.3 
Results and Discussion......................................................................... 385
9.3.2.3.1  Characterization of Femtosecond Time-Resolved
Absorption Spectra: Identification of Sequential
Internal Conversion�����������������������������������������������������������385
9.3.2.3.1.1  Time-Resolved Absorption Spectra Near
Zero Delay Time������������������������������������������385
9.3.2.3.1.2  Time-Resolved Spectra with Positive
Delay Times�������������������������������������������������386
9.3.2.3.2  Analysis by SVD and Global-Fitting in the Framework
of a Sequential Model�������������������������������������������������������387
9.3.2.3.3  Comparison with the Previous Results of
Subpicosecond Time-Resolved Absorption Spectra���������389
References........................................................................................................... 390

Chapter 9.3.3 
Observation of Breather Exciton and Soliton in a Substituted Polythiophene
with a Degenerate Ground State.......................................................................... 391
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Title: An introductory lecture on archæology

Delivered before the University of Cambridge

Author: Churchill Babington

Release date: October 29, 2023 [eBook #71984]

Language: English

Original publication: Cambridge: Deighton, Bell, and Co, 1865

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*** START OF THE PROJECT GUTENBERG EBOOK AN

INTRODUCTORY LECTURE ON ARCHÆOLOGY ***
INTRODUCTORY LECTURE

ON

ARCHÆOLOGY.
 Cambridge:
PRINTED BY C. J. CLAY, M.A.
AT THE UNIVERSITY PRESS.
 AN

INTRODUCTORY LECTURE

ON

ARCHÆOLOGY

Delivered before the University of Cambridge.

BY

CHURCHILL BABINGTON, B.D., F.L.S.

DISNEY PROFESSOR OF ARCHÆOLOGY, SENIOR FELLOW OF
ST JOHN’S COLLEGE,
MEMBER OF THE ROYAL SOCIETY OF LITERATURE, OF THE
NUMISMATIC
AND SYRO-EGYPTIAN SOCIETIES, HONORARY MEMBER OF
THE
HISTORICO-THEOLOGICAL SOCIETY OF LEIPSIC, AND OF
THE ARCHÆOLOGICAL INSTITUTE OF ROME.

CAMBRIDGE:
DEIGHTON, BELL, AND CO.
LONDON: BELL AND DALDY.
1865.
 PREFACE.

The following Lecture was divided in the delivery into two parts;
illustrative specimens being exhibited after the conclusion of the
delivery of each portion. It has been suggested that I should add in
the form of notes a few books which may prove useful to the
students of particular branches of Archæology; my best thanks are
due to the Rev. T. G. Bonney and the Rev. W. G. Searle for their kind
and valuable assistance in drawing up certain of the lists. For ancient
art and archæology K. O. Müller’s Manual, so often referred to, will in
general sufficiently indicate the bibliography, and it is only in a few
departments, in numismatics more especially, that it has been
deemed necessary to add anything to his references. M. Labarte’s
Handbook, from which a great part of the concluding portion of this
lecture is derived, will do the same thing, though in a far less
complete manner, for medieval art.
 CONTENTS.

Plan of the Lecture, pp. 1-3.

Archæology defined, and the principal kinds of archæological
monuments specified, pp. 3-6.
Nature of the Disney Professorship of Archæology explained; its
comprehensive character; the advantages of this, pp. 6-13.
Sketch of the existing remains of Antiquity among different nations,
beginning with primeval man, pp. 13-21. The Egyptians, pp. 21-
26. The Babylonians, pp. 26, 27. The Assyrians, pp. 27, 28. The
Persians, pp. 28, 29. The Jews, pp. 29-31. The Phœnicians, pp.
31, 32. The Lycians, pp. 32, 33. The Greeks, pp. 33-41. The
Etruscans, p. 41. The Romans, pp. 42-46. The Celts, pp. 43, 44.
The Byzantine empire and the European nations during the
middle ages, pp. 46-61. Recapitulation, pp. 61, 62.
Qualifications necessary for an archæologist. He must be a collector
of facts and objects, and be able to reason on them. He must
also be a man of learning. Exact scholarship, an appreciation of
art, and a knowledge of natural history often useful or necessary
for the archæologist, pp. 63-68.
Pleasures and advantages which result from archæology. It
illustrates and is illustrated by ancient literature. Modern art
aided by archæology. Archæology deserving of cultivation for its
own sake, as an ennobling and delightful pursuit, pp. 68-74.
 INTRODUCTORY LECTURE

ON

ARCHÆOLOGY.
Following the example of my distinguished predecessor in
the Disney Professorship of Archæology, I open my first Course
of Lectures with an introductory Lecture on Archæology itself, so
far as the very limited time for preparation has allowed me to
attempt one.
I cannot indeed conceal from myself, and still less can I
conceal from you, that no introductory Lecture which I could give,
even if I were to take my own time in writing it, would bear any
comparison with the compositions of his elegant and learned
pen. It certainly does not proceed from flattery, and I hope not
from an undue partiality of friendship to say of him, that in his
power of grasping a complicated subject, of presenting it in a
clear light, of illustrating it with varied learning, and of expressing
himself in relation thereto in appropriate language, I have rarely
seen his equal. To how great a disadvantage then must I
necessarily appear, when I have had only six weeks’ time in
which to get ready this as well as five other Lectures, and have
been moreover compelled to devote a considerable part even of
that short time to other and not less important duties. A great
unwillingness however that the Academical year should pass
over without any Archæological Lectures being delivered by the
Disney Professor, has induced me to make the attempt more
quickly than would under other circumstances have been
desirable or even justifiable; and I venture to hope that when
allowance is made for the exigency of the case, I shall find in
you, who have honoured this Lecture by your presence, a
clement and even an indulgent audience.
In an introductory Lecture which deals with generalities, it is
hardly to be expected that I either can say or ought to try to say
much which is absolutely new to any of my hearers; and I shall
not affect to say anything peculiarly striking, but shall rather
attempt to bring before you in a plain way a view of the subject,
which aims at being concise and comprehensive; and in
connexion therewith respectfully to submit a few observations
which have relation to other Academical studies, as well as to
the character of this particular Professorship.
What I propose then to do is this, first to explain what
Archæology is; next to put in a clear light what the character of
this Professorship is; after that to attempt a general sketch of the
existing remains of Antiquity; then to point out the qualifications
necessary or desirable for an archæologist; and in conclusion, to
indicate the pleasure and advantage which flow from his
pursuits.
The field of Archæology is vast, and almost boundless; the
eye, even the most experienced eye, can hardly take in the
whole prospect; and those who have most assiduously laboured
in its exploration will be most ready to admit, that there are
portions, and those large portions, which are to them either
almost or altogether unknown.
For what is Archæology? It is, I conceive, the science of
teaching history by its monuments[1], of whatever character those
monuments may be. When I say history, I use the word not in the
limited sense of the history of dynasties or of governments.
Archæology does indeed concern itself with these, and
splendidly does it illustrate and illuminate them; but it also
concerns itself with every kind of monument of man which the
ravages of time have spared.
1. Perhaps it would be more correct to say ‘by its contemporary sensible
monuments,’ so as to exclude later copies of ancient writings, or the monumenta
litterarum, which fall more especially to the province of the scholar. A MS. of
Aristotle of the thirteenth century is an archæological monument of that century
only; it is a literary monument of the fourth century B.C. But a Greek epigram or
epitaph which occurs on a sepulchral monument of the same or any other century
B.C. is an archæological as well as a literary monument of that century.

Archæology concerns itself with the domestic and the social,

as well as with the religious, the commercial, and the political life
of all nations and of all tribes in the ages that have passed away.
All that men in ancient times have made, and left behind them, is
the farrago of our study.
The archæologist will consequently make observations and
speculations on the sites of ancient cities where men have dwelt;
on their walls and buildings, sacred and profane; on their altars
and their market-places; on their subterranean constructions,
whether sepulchres, treasuries, or drains. He will trace the roads
and the fosses along which men of the old world moved, and on
which men often still move; he will explore the routes of armies
and the camps where they have pitched, and will prowl about the
barrows in which they sleep;

Exesa inveniet scabra robigine pila,

Grandiaque effossis mirabitur ossa sepulchris.

He will also collect and classify every kind of object, which man
has made for use or for ornament in his own home, or in the city;
in the fields, or on the water. He will arrange the weapons of
offence and defence according to their material and age; whether
of stone, of bronze, of iron, or of steel; among which some are so
rude that a practised eye alone distinguishes them from the
broken flint stones lying in the field, others again so elaborate as
to rank among the most beautiful productions both of classical
and medieval art; he will not disdain to preserve the bricks and
the tiles, which have once formed parts of Asiatic cities or of
Roman farms; he will excavate the villas of the ancients; unearth
their mosaic pavements; clean their lamps and candelabra; he
will mend or restore their broken crockery, and glass; he will
even penetrate into the lady’s chamber, turn over her toilet,
admire her brooches and her bracelets, examine her mirrors and
her pins; and all this he will do in addition to studying the nobler
works of ancient art, such as engraved gems and medallions;
works chased, carved and embossed in the precious metals and
in ivory; frescoes and vase-paintings; bronzes and statues. He
will, likewise, familiarise himself with the alphabets of the ancient
nations, and exercise his ingenuity in deciphering their written
records, both public and private; whether these be contained in
inscriptions on stones or metal plates, or in papyrus-rolls, or
parchment books; or be scratched on walls or on statues; or be
painted on vases; or, in fine, surround the device of a coin.
I have now mentioned some of the principal objects of
archæology, which, as I have said, embraces within its range all
the monuments of the history and life of man in times past. And
this it does, beginning with the remains of primeval man, which
stretch far beyond the records of all literary history, and
descending along the stream of time till it approaches, but does
not quite reach time actually present. No sharp line of
demarcation separates the past from the present; you may say
that classical archæology terminates with the overthrow of the
Western Empire; you may conceive that medieval archæology
ceases with the reign of Henry the Seventh; but, be this as it
may, in a very few generations the objects of use or of ornament
to us will become the objects of research to the archæologist;
and, I may add, may be the subjects of lectures to my
successors.
For the founder of this Professorship, whose memory is never
to be named without honour, and the University which accepted
it, together with his valuable collection of ancient sculptures,
undoubtedly intended that any kind or class of antiquities
whatever might fitly form the theme of the Professor’s discourse.
I say this, because a misconception has undoubtedly prevailed
on this subject, from which even my learned predecessor himself
was not free. “Every nation of course,” says he, “has its own
peculiar archæology. Whether civilized or uncivilized, whether of
historic fame or of obscure barbarism, Judæa, Assyria, and
Egypt; Greece and Rome; India, China, and Mexico; Denmark,
Germany, Britain, and the other nations of modern Europe, all
have their archæology. The field of inquiry,” he continues, “is
boundless, and in the multitude of objects presenting themselves
the enquirer is bewildered. It has been wisely provided therefore
by the founder of this Professorship, that we shall direct our
attention more immediately to one particular class of Antiquities,
and that the noblest and most important of them all, I mean the
Antiquities of Greece and Rome[2].” Very probably such may
have been Mr Disney’s original intention; and if so, this will easily
explain and abundantly pardon the error of my accomplished
friend; but the actual words of the declaration and agreement
between Mr Disney and the University, which is of course the
only document of binding force, are as follows: “That it shall be
the duty of the Professor to deliver in the course of each
academical year, at such days and hours as the Vice-Chancellor
shall appoint, six lectures at least on the subject of Classical,
Mediæval and other Antiquities, the Fine Arts and all matters and
things connected therewith.” Whether he would have acted
wisely or not wisely in limiting the field to classical archæology,
he has in point of fact not thus limited it. And, upon the whole, I
must confess, I am glad that he has imposed no limitation. For
while there are but few who would deny that many of the very
choicest relics of ancient art and of ancient history are to be
sought for in the Greek and Roman saloons and cabinets of the
museums of Europe, yet it must at the same time be admitted
that there are other branches of archæology, which are far too
important to be neglected, and which have an interest, and often
a very high interest, of their own.
2. Marsden’s Introd. Lect. p. 5. Cambr. 1852.
 Let it be confessed, that the archæology of Greece has in
many respects the pre-eminence over every other. “It is to
Greece that the whole civilized world looks up,” says Canon
Marsden, “as its teacher in literature and in art; and it is to her
productions that we refer as the standard of all that is beautiful,
noble, and excellent. Greece excelled in all that she put her hand
to. Her sons were poets and orators and historians; they were
architects and sculptors and painters. The scantiest gleanings of
her soil are superior to that which constitutes the pride and boast
of others. Scarcely a fragment is picked up from the majestic
ruin, which does not induce a train of thought upon the
marvellous grace and beauty which must have characterized the
whole!

Quale te dicat tamen

Antehac fuisse, tales cum sint relliquiæ.”

These eloquent and fervid words proceed from a passionate

admirer of Hellenic art, and a most successful cultivator of its
archæology. Nor do I dare to say that the praise is exaggerated.
But at the same time, viewed in other aspects, the archæology of
our own country has even greater interest and importance for us.
What man is there, in whose breast glows a spark of patriotism,
who does not view the monuments of his country which are
everywhere spread around him, (in this place above most
places,) which connect the present with the remote past, and
with many and diverse ages of that past by a thousand
reminiscences, with feelings deeper and nobler than any exotic
remains of antiquity, how charming soever, could either foment or
engender? This love of national antiquities, seated in a healthy
patriotic feeling, has place in the speech of an apostle himself:
“Men and brethren, let me freely speak unto you of the patriarch
David, that he is both dead and buried; and his sepulchre is with
us unto this day.” The same feeling prompted Wordsworth thus
to express himself in reference to our ancient colleges and their
former occupants: