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Springer Series in Chemical Physics 116

Kaoru Yamanouchi
Wendell T. Hill III
Gerhard G. Paulus Editors

Progress in
Ultrafast Intense
Laser Science XIII
Springer Series in Chemical Physics

Volume 116

Series editors
A.W. Castleman Jr., University Park, USA
J.P. Toennies, Göttingen, Germany
K. Yamanouchi, Tokyo, Japan
W. Zinth, München, Germany
The Springer Series in Chemical Physics consists of research monographs in basic
and applied chemical physics and related analytical methods. The volumes of this
series are written by leading researchers of their fields and communicate in a
comprehensive way both the basics and cutting-edge new developments. This series
aims to serve all research scientists, engineers and graduate students who seek
up-to-date reference books.

More information about this series at http://www.springer.com/series/11752

Kaoru Yamanouchi ⋅ Wendell T. Hill III
Gerhard G. Paulus
Editors

Progress in Ultrafast Intense

Laser Science XIII

123
Editors
Kaoru Yamanouchi Gerhard G. Paulus
Department of Chemistry Institute of Optics and Quantum Electronics
The University of Tokyo Friedrich Schiller University Jena
Tokyo Jena, Thüringen
Japan Germany

Wendell T. Hill III

University of Maryland, College Park
College Park, MD
USA

ISSN 0172-6218
Springer Series in Chemical Physics
Progress in Ultrafast Intense Laser Science
ISBN 978-3-319-64839-2 ISBN 978-3-319-64840-8 (eBook)
https://doi.org/10.1007/978-3-319-64840-8
Library of Congress Control Number: 2017954485

© Springer International Publishing AG 2017

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Preface

We are pleased to present the thirteenth volume of Progress in Ultrafast Intense

Laser Science. As the frontiers of ultrafast intense laser science rapidly expand ever
outward, there continues to be a growing demand for an introduction to this
interdisciplinary research field that is at once widely accessible and capable of
delivering cutting-edge developments. Our series aims to respond to this call by
providing a compilation of concise review-style articles written by researchers at
the forefront of this research field, so that researchers with different backgrounds as
well as graduate students can easily grasp the essential aspects.
As in previous volumes of PUILS, each chapter of this book begins with an
introductory part, in which a clear and concise overview of the topic and its sig-
nificance is given, and moves onto a description of the authors' most recent research
results. All chapters are peer-reviewed. The articles of this thirteenth volume cover
a diverse range of the interdisciplinary research field, and the topics may be grouped
into four categories: atoms, molecules, and clusters interacting in an intense laser
field (Chaps. 1–5); high-order harmonics generation and its applications (Chaps. 6
and 7); photoemission at metal tips (Chap. 8); and advanced laser facilities (Chaps.
9 and 10).
From the third volume, the PUILS series has been edited in liaison with the
activities of the Center for Ultrafast Intense Laser Science at the University of
Tokyo, which has also been responsible for sponsoring the series and making the
regular publication of its volumes possible. From the fifth volume, the Consortium
on Education and Research on Advanced Laser Science, the University of Tokyo,
has joined this publication activity as one of the sponsoring programs. The series,
designed to stimulate interdisciplinary discussion at the forefront of ultrafast intense
laser science, has also collaborated since its inception with the annual symposium
series of ISUILS (http://www.isuils.jp/), sponsored by JILS (Japan Intense Light
Field Science Society).
We would like to take this opportunity to thank all of the authors who have kindly
contributed to the PUILS series by describing their most recent work at the frontiers
of ultrafast intense laser science. We also thank the reviewers who have read the
submitted manuscripts carefully. One of the coeditors (KY) thanks Ms. Mihoshi Abe

v
vi Preface

for her help with the editing processes. Last but not least, our gratitude goes out to
Dr. Claus Ascheron, Physics Editor of Springer-Verlag at Heidelberg, for his kind
support.
We hope this volume will convey the excitement of ultrafast intense laser sci-
ence to the readers and stimulate interdisciplinary interactions among researchers,
thus paving the way to explorations of new frontiers.

Tokyo, Japan Kaoru Yamanouchi

College Park, USA Wendell T. Hill III
Jena, Germany Gerhard G. Paulus
January 2017
Contents

1 Strong-Field S-Matrix Series with Coulomb Wave Final State .... 1

F.H.M. Faisal
1.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1
1.2 Three-Interaction Formalism . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
1.3 Coulomb–Volkov Hamiltonian and Propagator . . . . . . . . . . . . . . 6
1.4 Coulomb-Volkov S-Matrix Series . . . . . . . . . . . . . . . . . . . . . . . 9
1.5 Strong-Field S-Matrix for Short-Range Potentials . . . . . . . . . . . . 11
1.6 Concluding Remarks . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
2 Multiconfiguration Methods for Time-Dependent Many-Electron
Dynamics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. 15
Erik Lötstedt, Tsuyoshi Kato and Kaoru Yamanouchi
2.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. 15
2.2 Basics of Time-Dependent Multiconfiguration Methods . . . . . .. 17
2.3 Time-Dependent Multiconfiguration Methods
with Time-Independent Orbitals . . . . . . . . . . . . . . . . . . . . . . . .. 21
2.3.1 Time-Dependent Configuration Interaction
with Single Excitations . . . . . . . . . . . . . . . . . . . . . . . . .. 22
2.3.2 Time-Dependent Restricted-Active-Space
Configuration-Interaction . . . . . . . . . . . . . . . . . . . . . . .. 23
2.3.3 Time-Dependent R-Matrix Theory . . . . . . . . . . . . . . . .. 25
2.4 Time-Dependent Multiconfiguration Methods
with Time-Dependent Orbitals . . . . . . . . . . . . . . . . . . . . . . . . .. 26
2.4.1 Multiconfiguration Time-Dependent Hartree-Fock . . . . .. 28
2.4.2 Time-Dependent Complete Active-Space
Self-Consistent Field . . . . . . . . . . . . . . . . . . . . . . . . . . . 31
2.5 Factorized CI . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 32
2.6 Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 35
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 37

vii
viii Contents

3 Controlling Coherent Quantum Nuclear Dynamics in LiH by

Ultra Short IR Atto Pulses . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. 41
Astrid Nikodem, R.D. Levine and F. Remacle
3.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. 42
3.2 Electronic Structure of LiH and Quantum Dynamics . . . . . . . . .. 43
3.3 Control of the Fragmentation Yields in the Σ Manifold by the
CEP of Pulse . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. 49
3.4 Effect of the Non Adiabatic Coupling in the Σ Manifold . . . . . .. 51
3.5 Probing the Dynamics for a Superposition of Σ and Π States by
Transient Absorption . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. 54
3.6 Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. 61
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. 61
4 Probing Multiple Molecular Orbitals in an Orthogonally
Polarized Two-Color Laser Field . . . . . . . . . . . . . . . . . . . . . . . . .. 67
Hyeok Yun, Hyung Taek Kim, Kyung Taec Kim
and Chang Hee Nam
4.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 68
4.2 Two-Dimensional High-Harmonic Spectroscopy of Molecules . . . 69
4.2.1 HHG in an Orthogonally Polarized Two-Color Field . . . . 69
4.2.2 HHG from Linear Molecules . . . . . . . . . . . . . . . . . . . . . 72
4.3 Resolving High-Harmonics from Multiple Orbitals . . . . . . . . . . . 74
4.3.1 Qualitative Approach . . . . . . . . . . . . . . . . . . . . . . . . . . . 74
4.3.2 Theoretical Calculation . . . . . . . . . . . . . . . . . . . . . . . . . . 76
4.3.3 Experimental Demonstration . . . . . . . . . . . . . . . . . . . . . . 79
4.4 Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 82
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 83
5 Tracing Nonlinear Cluster Dynamics Induced by Intense XUV,
NIR and MIR Laser Pulses . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. 85
Bernd Schütte
5.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 85
5.2 Ionization Dynamics of Clusters . . . . . . . . . . . . . . . . . . . . . . . . 87
5.2.1 XUV Multistep Ionization of Clusters . . . . . . . . . . . . . . . 87
5.2.2 Controlled Ignition of NIR Avalanching in Clusters . . . . . 89
5.2.3 MIR Strong-Field Ionization of Clusters Using
Two-Cycle Pulses . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 92
5.3 Expansion and Recombination Dynamics of Clusters . . . . . . . . . 94
5.3.1 Cluster Fragmentation . . . . . . . . . . . . . . . . . . . . . . . . . . 94
5.3.2 Frustrated Recombination . . . . . . . . . . . . . . . . . . . . . . . . 96
5.3.3 Reionization of Excited Atoms from Recombination . . . . 97
5.4 Autoionization and Correlated Electronic Decay . . . . . . . . . . . . . 101
5.4.1 Autoionization in Expanding Clusters . . . . . . . . . . . . . . . 102
5.4.2 Correlated Electronic Decay . . . . . . . . . . . . . . . . . . . . . . 104
Contents ix

5.5 Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 107

References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 108
6 Molecules in Bichromatic Circularly Polarized Laser Pulses:
Electron Recollision and Harmonic Generation . . . . . . . . . . . . . . . 111
André D. Bandrauk, François Mauger and Kai-Jun Yuan
6.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 112
6.2 Bicircular Recollision Dynamics . . . . . . . . . . . . . . . . . . . . . . . . 114
6.3 Polarization of Molecular HHG . . . . . . . . . . . . . . . . . . . . . . . . . 122
6.4 Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 125
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 127
7 High Harmonic Phase Spectroscopy Using Long Wavelengths . . . . 129
Antoine Camper, Stephen B. Schoun, Pierre Agostini
and Louis F. DiMauro
7.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 129
7.2 Reconstruction of the Attosecond Beating by Interference of
Two-Photon Transitions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 130
7.3 High Harmonic Spectroscopy of Argon Cooper Minimum . . . . . 133
7.4 High Harmonic Spectroscopy of Aligned Nitrogen . . . . . . . . . . . 137
7.5 Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 141
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 142
8 Strong-Field-Assisted Measurement of Near-Fields and Coherent
Control of Photoemission at Nanometric Metal Tips . . . . . . . . . . . . 143
M. Förster, T. Paschen, S. Thomas, M. Krüger and P. Hommelhoff
8.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 143
8.2 Experimental Setup . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 145
8.3 Measurement of the Field Enhancement Factor at the Tip Apex
by Rescattering Electrons . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 146
8.4 Coherent Control of Photoemission . . . . . . . . . . . . . . . . . . . . . . 149
8.5 Summary and Outlook . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 153
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 154
9 Advanced Laser Facilities and Scientific Applications . . . . . . . . . . . 157
Luis Roso
9.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 157
9.2 Different Approaches for a PW . . . . . . . . . . . . . . . . . . . . . . . . . 160
9.3 Bottlenecks . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 163
9.4 Applications of PW Lasers . . . . . . . . . . . . . . . . . . . . . . . . . . . . 168
9.5 Hard Laser Light . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 172
9.6 Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 176
9.7 Appendix: The VEGA Laser . . . . . . . . . . . . . . . . . . . . . . . . . . . 177
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 178
x Contents

10 The Extreme Light Infrastructure—Attosecond Light Pulse

Source (ELI-ALPS) Project . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 181
Dimitris Charalambidis, Viktor Chikán, Eric Cormier, Péter Dombi,
József András Fülöp, Csaba Janáky, Subhendu Kahaly,
Mikhail Kalashnikov, Christos Kamperidis, Sergei Kühn,
Franck Lepine, Anne L’Huillier, Rodrigo Lopez-Martens,
Sudipta Mondal, Károly Osvay, László Óvári, Piotr Rudawski,
Giuseppe Sansone, Paris Tzallas, Zoltán Várallyay and Katalin Varjú
10.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 183
10.2 The Mission and Structure of ELI-ALPS . . . . . . . . . . . . . . . . . . 184
10.3 Lasers . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 185
10.3.1 The High Repetition Rate (HR) Laser System . . . . . . . . . 186
10.3.2 The Single-Cycle Laser System (SYLOS) . . . . . . . . . . . . 187
10.3.3 The High-Field (HF) Laser System . . . . . . . . . . . . . . . . . 189
10.3.4 The MIR System . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 191
10.4 Secondary Sources . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 192
10.4.1 The GHHG Beamlines . . . . . . . . . . . . . . . . . . . . . . . . . . 193
10.4.2 The Surface High Harmonic Generation (SHHG)
Development Beamlines . . . . . . . . . . . . . . . . . . . . . . . . . 202
10.4.3 The THz Beamlines . . . . . . . . . . . . . . . . . . . . . . . . . . . . 207
10.4.4 The Electron Acceleration Beamlines . . . . . . . . . . . . . . . 209
10.5 Research Perspectives . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 211
10.6 Outlook . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 214
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 215
Index . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 219
Contributors

Pierre Agostini Department of Physics, The Ohio State University, Columbus,

OH, USA
André D. Bandrauk Computational Chemistry & Molecular Photonics, Labora-
toire de Chimie Théorique, Faculté des Sciences, Université de Sherbrooke,
Sherbrooke, Québec, Canada
Antoine Camper Department of Physics, The Ohio State University, Columbus,
OH, USA
Dimitris Charalambidis FORTH-IESL, Heraklion, Greece; ELI-ALPS, ELI-Hu
Kft, Szeged, Hungary
Viktor Chikán Kansas State University, Manhattan, USA; ELI-ALPS, ELI-Hu
Kft, Szeged, Hungary
Eric Cormier University of Bordeaux, CEA, CNRS, CELIA, UMR 5107,
Talence, France; ELI-ALPS, ELI-Hu Kft, Szeged, Hungary
Louis F. DiMauro Department of Physics, The Ohio State University, Columbus,
OH, USA
Péter Dombi Wigner RCP, Budapest, Hungary; ELI-ALPS, ELI-Hu Kft, Szeged,
Hungary
F.H.M. Faisal Fakultaet Fuer Physik, Universitaet Bielefeld, Bielefeld, Germany;
Optical Sciences Center, University of Arizona, Tucson, AZ, USA
M. Förster Lehrstuhl für Laserphysik, Friedrich-Alexander-Universität Erlangen-
Nürnberg, Erlangen, Germany
József András Fülöp University of Pécs, Pécs, Hungary; ELI-ALPS, ELI-Hu Kft,
Szeged, Hungary
P. Hommelhoff Lehrstuhl für Laserphysik, Friedrich-Alexander-Universität
Erlangen-Nürnberg, Erlangen, Germany

xi
xii Contributors

Csaba Janáky University of Szeged, Szeged, Hungary; ELI-ALPS, ELI-Hu Kft,

Szeged, Hungary
Subhendu Kahaly ELI-ALPS, ELI-Hu Kft, Szeged, Hungary
Mikhail Kalashnikov MBI, Berlin, Germany; ELI-ALPS, ELI-Hu Kft, Szeged,
Hungary
Christos Kamperidis ELI-ALPS, ELI-Hu Kft, Szeged, Hungary
Tsuyoshi Kato Department of Chemistry, School of Science, The University of
Tokyo, Tokyo, Japan
Hyung Taek Kim Center for Relativistic Laser Science, Institute for Basic Sci-
ence, Gwangju, Korea; Advanced Photonics Research Institute, Gwangju Institute
of Science and Technology, Gwangju, Korea
Kyung Taec Kim Center for Relativistic Laser Science, Institute for Basic Sci-
ence, Gwangju, Korea; Department of Physics and Photon Science, Gwangju
Institute of Science and Technology, Gwangju, Korea
M. Krüger Weizmann Institute of Science, Rehovot, Israel
Sergei Kühn ELI-ALPS, ELI-Hu Kft, Szeged, Hungary
Franck Lepine UMR 5306 CNRS Univ. Lyon 1, Villeurbanne Cedex, France;
ELI-ALPS, ELI-Hu Kft, Szeged, Hungary
R.D. Levine The Fritz Haber Center for Molecular Dynamics and Institute of
Chemistry, The Hebrew University of Jerusalem, Jerusalem, Israel; Crump Institute
for Molecular Imaging and Department of Molecular and Medical Pharmacology,
David Geffen School of Medicine and Department of Chemistry and Biochemistry,
University of California, Los Angeles, CA, USA
Anne L’Huillier Lund University, Lund, Sweden
Rodrigo Lopez-Martens LOA, UMR 7639, Palaiseau, France; ELI-ALPS,
ELI-Hu Kft, Szeged, Hungary
Erik Lötstedt Department of Chemistry, School of Science, The University of
Tokyo, Tokyo, Japan
François Mauger Department of Physics and Astronomy, Louisiana State
University, Baton Rouge, LA, USA
Sudipta Mondal ELI-ALPS, ELI-Hu Kft, Szeged, Hungary
Chang Hee Nam Center for Relativistic Laser Science, Institute for Basic Science,
Gwangju, Korea; Department of Physics and Photon Science, Gwangju Institute of
Science and Technology, Gwangju, Korea
Astrid Nikodem Département de Chimie, B6c, Université de Liège, Liège,
Belgium
Contributors xiii

Károly Osvay University of Szeged, Szeged, Hungary; ELI-ALPS, ELI-Hu Kft,

Szeged, Hungary
László Óvári University of Szeged, Szeged, Hungary; ELI-ALPS, ELI-Hu Kft,
Szeged, Hungary
T. Paschen Lehrstuhl für Laserphysik, Friedrich-Alexander-Universität Erlangen-
Nürnberg, Erlangen, Germany
F. Remacle Département de Chimie, B6c, Université de Liège, Liège, Belgium;
The Fritz Haber Center for Molecular Dynamics and Institute of Chemistry, The
Hebrew University of Jerusalem, Jerusalem, Israel
Luis Roso Centro de Láseres Pulsados (CLPU), Villamayor, Salamanca, Spain
Piotr Rudawski Lund University, Lund, Sweden
Giuseppe Sansone Politecnico di Milano, Milan, Italy; ELI-ALPS, ELI-Hu Kft,
Szeged, Hungary
Stephen B. Schoun Department of Physics, The Ohio State University, Columbus,
OH, USA
Bernd Schütte Max-Born-Institut, Berlin, Germany
S. Thomas Lehrstuhl für Laserphysik, Friedrich-Alexander-Universität Erlangen-
Nürnberg, Erlangen, Germany
Paris Tzallas ELI-ALPS, ELI-Hu Kft, Szeged, Hungary
Katalin Varjú University of Szeged, Dóm tér 9, 6720 Szeged, Hungary;
ELI-ALPS, ELI-Hu Kft, Szeged, Hungary
Zoltán Várallyay ELI-ALPS, ELI-Hu Kft, Szeged, Hungary
Kaoru Yamanouchi Department of Chemistry, School of Science, The University
of Tokyo, Tokyo, Japan
Kai-Jun Yuan Computational Chemistry & Molecular Photonics, Laboratoire de
Chimie Théorique, Faculté des Sciences, Université de Sherbrooke, Sherbrooke,
Québec, Canada
Hyeok Yun Center for Relativistic Laser Science, Institute for Basic Science,
Gwangju, Korea
Chapter 1
Strong-Field S-Matrix Series with Coulomb
Wave Final State

F.H.M. Faisal

Abstract Despite its long-standing usefulness for the analysis of various processes
in intense laser fields, it is well-known that the KFR or strong-field approximation
(SFA) does not account for the final-state Coulomb interaction for ionisation. Var-
ious ad hoc attempts have been made in the past to face this problem within the
SFA, however, till now no systematic S-matrix expansion accounting for it has been
found. To overcome this long standing limitation of SFA we present here a systematic
series expansion of the strong-field S-matrix that could accounts for the final-state
Coulomb interaction in all orders.

1.1 Introduction

Over the past several decades the well-known strong-field approximation in the form
of the so-called KFR or SFA ansatz [1–3] has provided much fruitful insights into
the highly non-perturbative processes in intense laser fields. However, it is also well-
known that SFA does not account for the Coulomb interaction in the final state that is
specially significant for the ubiquitous ionisation process in strong fields. Due to this
problem, many authors in the past decades have made various heuristic corrections to
the SFA. Thus, for example, attempts to account for the Coulomb effect appear within
early ionisation models [4–6]. Other approaches include WKB-like approximations
[7, 8], semi-clssical and/or “quantum trajectory” approach [9–11], semi-analytic R-
matrix approach [12], and more recently an approach employing ansätze with phase
correction plus inhomogeneous differential equation [13]. Until now, however, no
systematic strong-field S-matrix theory could be found that unlike the usual plane-
wave SFA would be able to account for the laser plus Coulomb interaction in the
final state to all orders.

F.H.M. Faisal (✉)

Fakultaet Fuer Physik, Universitaet Bielefeld, 33501 Bielefeld, Germany
e-mail: ffaisal@physik.uni-bielefeld.de
F.H.M. Faisal
Optical Sciences Center, University of Arizona, Tucson, AZ 85721, USA

© Springer International Publishing AG 2017 1

K. Yamanouchi et al. (eds.), Progress in Ultrafast Intense Laser Science XIII,
Springer Series in Chemical Physics 116, https://doi.org/10.1007/978-3-319-64840-8_1
2 F.H.M. Faisal

Here we present a strong-field S-matrix theory that overcomes this long standing
problem and derive a systematic all order S-matrix series explicitly incorporating
the laser plus Coulomb interaction in the final state. To this end we shall use be-
low a three-interaction formalism developed earlier in connection with the so-called
intense-field S-matrix theory or IMST (see, e.g. review [14] or, original references
cited therein).

1.2 Three-Interaction Formalism

In this section we briefly indicate the three-interaction technique suitable for the
problem at hand. The Schroedinger equation of the interacting atom+ laser field is

𝜕
(iℏ − H(t))|𝛹 (t)⟩ = 0 (1.1)
𝜕t

where H(t) is the total Hamlltonian of the system,

H(t) = Ha + Vi (t) (1.2)

For example, for an effective one electron atomic system interacting with a laser
field, we may take

𝐩op 2 Ze2
Ha = ( − + Vs.r. (𝐫)) (1.3)
2m r

where Z is the core charge and Vs.r. (𝐫) is a short-range potential that goes to zero for
asymptotically large r faster than the Coulomb potential.
The laser-atom interaction is assumed here in the minimal coupling gauge (in
“dipole approximation”)

e e2 A2 (t)
Vi (t) = (− 𝐀(t) ⋅ 𝐩op + ) (1.4)
mc 2mc2

where 𝐀(t) is the vector potential of the laser field, and 𝐩op ≡ −iℏ∇.
Since all information of the interacting system is contained in the full wavefunc-
tion 𝛹 (t) and in general this is not known explicitly, we shall consider a more useful
formal expression of the full wavefunction in terms of the appropriate partial in-
teractions among the sub-systems and, the associated sub-propagators (or Green’s
functions). The latter objects may be already known, or could be found, to expand
the total wavefunction in terms of them.
Thus, first, we may formally define the full propagator, G(t, t′ ), associated with
the total Hamiltonian H(t), by the inhomogeneous equation
1 Strong-Field S-Matrix Series with Coulomb Wave Final State 3

𝜕
(iℏ − H(t))G(t, t′ ) = 𝛿(t − t′ ). (1.5)
𝜕t
The solution of the Schroedinger equation (1.1) can then be expressed as

|𝛹 (t)⟩ = |𝜙i (t)⟩ + G(t, t1 )Vi (t1 )|𝜙i (t1 )⟩dt1 (1.6)
∫

where |𝜙i (t)⟩ is a given initial state. We may note here already that due to the implicit
presence of the Heaviside theta-function in all the propagators (see, for example, the
Volkov propagator given in the sequel) the time integration limits are always from
a given initial time ti to a given final time tf since the limits of the intermediate
time-integrations are automatically controlled by the propagators at the appropriate
positions by themselves. Usually the interaction time interval tf − ti is taken to be
long, e.g., from −∞ to +∞. Note, however, that there is no difficulty in using the
theory for interactions with any finite laser pulse, for during the rest of the time, from
and to the long-time limits, the pulse could be assumed to be vanishingly small.
In general, as for the full wavefunction, we do not have explicit knowledge of
the full propagator G(t, t′ ). Therefore, we intend to express it in terms of certain
most relevant sub-propagators. Clearly, the two most relevant states in any quantum
mechanical transition process are the initial state, in which the system is prepared,
and the final state, in which the system is detected. Since in any ionisation process
the final state interaction is governed by the long-range Coulomb interaction of the
outgoing electron and the residual ion-core, it is highly desirable that the final state
incorporates the long-range Coulomb interaction from the beginning.
Let us define a final reference Hamiltonian Hf (t) that incorporates the final-state
Coulomb interaction in the presence of the laser field. Hf , and the corresponding
final-state interaction Vf (t) are related to each other by the total Hamiltonian, H(t),

H(t) = Hf (t) + Vf (t) (1.7)

Formally, the final state propagator is then defined as usual by

𝜕
(iℏ − Hf (t))Gf (t, t′ )(t) = 𝛿(t − t′ ) (1.8)
𝜕t

Assuming for a moment that a suitable Hf (t) and Gf (t, t′ ) for the present purpose
could be found, the total G(t, t′ ) can be re-expressed in terms of Gf (t, t′ ) as

G(t, t′ ) = Gf (t, t′ ) + Gf (t, t1 )Vf (t1 )G(t1 , t′ )dt1 (1.9)

∫

Substituting this in |𝛹 (t)⟩ above we get a closed form expression of the full state
vector in the form
4 F.H.M. Faisal

|𝛹 (t)⟩ = |𝜙i (t)⟩ + dt1 Gf (t, t1 )Vi (t1 )|𝜙i (t1 )⟩

∫

+ dt2 dt1 Gf (t, t2 )Vf (t2 )G(t2 , t1 )Vi (t1 )|𝜙i (t1 )⟩ (1.10)
∫

This formally closed form of the wavefunction of the interacting system has been
originally derived and discussed in connection with non-sequential double ionization
processes (see, review [14]). Here we shall make use of it for the problem at hand.
In fact, the transition amplitude (or the S-Matrix element Sfi ) from an initial state,
|𝜙i (t)⟩, to a final state |𝜓f (t)⟩ of the system is given, by definition, by the projection
of the final state on to the total wavefunction evolving from the initial state. Thus,
using the above form of |𝛹 (t)⟩, we get

Sfi = ⟨𝜓f (t)|𝛹 (t)⟩

= ⟨𝜓f (t)|𝜙i (t)⟩ + dt1 ⟨𝜓f (t1 )|Vi (t1 )⟩|𝜙i (t1 )⟩ +
∫

+ dt2 dt1 ⟨𝜓f (t2 )|Vf (t2 )G(t2 , t1 )Vi (t1 )|𝜙i (t1 )⟩ + ... (1.11)
∫

This is a specially convenient general form of a transition amplitude from which

to generate the desired expansion of the ionisation amplitude. Now, G(t, t′ ) may be
expanded in terms of any suitable intermediate sub-propagator and the correspond-
ing intermediate interaction (without affecting the choice of the initial and the final
states and the respective rest-interactions). This generates a series expansion of the
strong-field S-matrix element of interest.
Before proceeding to derive the strong-field S-matrix series of present interest,
we may pause here briefly to make a few observations on the general character of
such series. Generally speaking, the strong-field S-matrix series are not perturbation
series based on a “small parameter”. Thus, for example, the usual plane wave SFA
expansion involves both the laser-atom interaction and the atomic potential. Indeed,
most of its useful applications using the first and the second order terms have been
for cases in which the laser field strength F had been weaker than the strength of
(eFa0)
the atomic potential or (Ze 2 ∕a0)
< 1, Z = nuclear charge; this is contrary to the view
sometimes held that SFA is a perturbative expansion where the “small parameter”
corresponds to the strength of the atomic potential (in comparison with the laser field
strength).
More appropriately viewed, strong-field S-matrix series are iterative series, where
each successive order of iteration corresponds to an additional intermediate
interaction-event or “collision” (involving the active electron and, either the atomic
potential or the laser-field, or both). With each increasing iteration order, the number
of intermediate “collisions” to occur also increases and hence the probability of its
significance for a given final event tends to decrease. Independent of this general but
qualitative expectation, the final results can be tested for quantitative accuracy only
a posteriori e.g. by comparison with accurate simulations (when feasible) and/or
1 Strong-Field S-Matrix Series with Coulomb Wave Final State 5

with experimental data (when available). Another physically significant usefulness

of such series is that they allow a systematic exploration of hypothesised mechanisms
behind a strong-field phenomenon. This is possible due to the ability of the S-matrix
series to systematically generate Feynman-like diagrams that can help to visualise
the underlying mechanism(s)suggested by the diagrams, as well as to estimate their
relative significance (see, e.g. [14]).
To continue with the problem at hand, we choose the strong-field Volkov propa-
gator GVol (t, t′ ) to expand the full G appearing in (1.11). The Volkov Hamiltonian is
given by the interaction of the free-electron with the laser field only, or

𝐩2op e e2 A2
HVol (t) = ( − 𝐀(t) ⋅ 𝐩 + ) (1.12)
2m mc 2mc2
The solutions of the corresponding Schroedinger equation are easily found
2
t pt′′
i
dt′′
𝜓𝐩 (𝐫, t) = ⟨𝐫|𝐩⟩e− ℏ ∫t′ 2m (1.13)

i
where 𝐩t ≡ (𝐩 − ec 𝐀(t)) and ⟨𝐫|𝐩⟩ = e ℏ 𝐩⋅𝐫 is a plane wave of momentum 𝐩.
The Volkov propagator GVol (t, t′ ) is the solution of the inhomogeneous equation

𝜕 𝐩2op e e2 A2
(iℏ − ( − 𝐀(t) ⋅ 𝐩 + ))GVol (t, t′ ) = 𝛿(t − t′ ). (1.14)
𝜕t 2m mc 2mc2
which is therefore given explicitly by:

i ∑ i t p2′′
dt′′
GVol (t, t′ ) = − 𝜃(t − t′ ) |𝐩⟩e− ℏ ∫t′
t
2m ⟨𝐩| (1.15)
ℏ 𝐩

Using the Volkov propagator we can expand

G(t, t′ ) = GVol (t, t′ ) + GVol (t, t1 )V0 (t1 )GVol (t1 , t′ )dt1 + ⋯ . (1.16)
∫

The intermediate interaction operator V0 (t) is accordingly defined by

V0 (t) = H(t) − HVol (t)

Ze2
= (− + Vs.r. (𝐫)) (1.17)
r
(which is time independent in the present case).
Since the initial state belongs to the atomic Hamiltonian Ha , therefore, the initial
rest-interaction Vi (t) is, as indicated earlier, simply
6 F.H.M. Faisal

Vi (t) = H(t) − Ha
e e2 A2
= (− 𝐀(t) ⋅ 𝐩op + ) (1.18)
mc 2mc2
For the final state, we intend to take account of the long-range Coulomb interac-
tion explicitly. One such state is the so-called “Coulomb-Volkov” state. It has been
introduced a long time ago [15, 16] by taking the usual stationary Coulomb-wave
and augmenting it heuristically by the time-dependent Volkov-phase:
2
t pt ′
−ℏ ∫i
dt′
𝛷𝐩 (𝐫, t) = 𝜙(−)
𝐩 (𝐫) × e
2m (1.19)

The stationary Coulomb waves, 𝜙(−)

𝐩 (𝐫), belong to the asymptotic atomic (or hydro-
genic) Hamiltonian HCou :

HCou = Ha − Vs.r. (𝐫)

𝐩2op Ze2
=( − ) (1.20)
2m r
They are given by [17]

1 𝜋 i i
𝜙(−)
𝐩 (𝐫) = e 2 𝜂p 𝛤 (1 + i𝜂p )e ℏ 𝐩⋅𝐫 1 F1 (−i𝜂p , 1, − (pr + 𝐩 ⋅ 𝐫)) (1.21)
L
3
2
ℏ

We have assumed them to be normalised in a large volume L3 with the understand-

∑ L 3
ing that, limit L → ∞, 𝐬 (⋯) ≡ ( 2𝜋 ) ∫ d3 s(⋯); 𝐩op ≡ −iℏ∇, and 𝜂p ≡ aZℏp is the
0
ℏ 2
so-called Sommerfeld parameter; a0 = Bohr radius = me 2
. Note that the “minus”
Coulomb wave is chosen above, which is appropriate for the ionisation final state. We
note in passing that for the laser assisted scattering problems the “plus” wave is also
of interest; they are related to each other by the transformation 𝜙(+) (−)∗
𝐩 (𝐫) = 𝜙−𝐩 (𝐫).
To determine the associated final-state interaction we need to know the appropri-
ate time-dependent Coulomb-Volkov Hamiltonian (call it HCV (t)). If it exists, HCV (t)
should be such, that the above defined Coulomb-Volkov state (1.19) should be a
member of the complete set of linearly independent fundamental solutions of the
associated Schroedinger equation.

1.3 Coulomb–Volkov Hamiltonian and Propagator

To determine the Hamiltonian HCV (t) to which the Coulomb-Volkov state belongs,
we introduce a vector operator defined by
1 Strong-Field S-Matrix Series with Coulomb Wave Final State 7
∑
𝜋c ≡ |𝜙𝐬 ⟩𝐬⟨𝜙𝐬 | (1.22)
𝐬

where |𝜙𝐬 ⟩ stands for the Coulomb wave (“+” or “-”) with momentum 𝐬, cf. (1.21).
Consider next the exponential operator

T(𝜋c ) = ei𝛼(t)⋅𝜋c (1.23)

t
where 𝛼(t) = mce
∫ 𝐀(t′ )dt′ . By expanding the exponential as a power series and
using the projection operator nature of the individual terms, it can be reduced to the
simple form
∑
T(𝜋c ) = 1 − |𝜙𝐬 ⟩(1 − ei𝛼(t)⋅𝐬 )⟨𝜙𝐬 | (1.24)
𝐬

We can write the Coulomb-Volkov Hamiltonian HCV (t) with the help of the op-
erator 𝜋c ,

𝐩2op Ze2 e2 A2 (t) e

HCV (t) = − + − 𝐀(t) ⋅ 𝜋c (1.25)
2m r 2mc2 mc

The corresponding Schroedinger equation is

𝜕 𝐩2op Ze2 e2 A2 (t) e

iℏ 𝛷j (t) = ( − + − 𝐀(t) ⋅ 𝜋c )𝛷j (t) (1.26)
𝜕t 2m r 2mc2 mc

The complete set of linearly independent solutions of (1.26) is

t 2 A2 (t′ )
i
(Ej + e )dt′ + ℏi 𝛼(t)⋅𝜋c
|𝛷j (t)⟩ = e− ℏ ∫ 2mc2 |𝜙j ⟩ (1.27)

where j ≡ 𝐩, stands for the momentum 𝐩 of the Coulomb wave state |𝜙(−) 𝐩 ⟩ and j ≡ D
stands for the discrete indices of the bound states |𝜙D ⟩ of the attractive Coulomb
potential. To establish that (1.27) indeed satisfies (1.26), let us first consider the case
{j ≡ 𝐩} and use (1.24) to calculate,
i
e ℏ 𝛼(t)⋅𝜋c |𝜙𝐩 ⟩ = T(𝜋c )|𝜙𝐩 ⟩
∑ i
= |𝜙𝐩 ⟩ − |𝜙𝐬 ⟩(1 − e ℏ 𝛼(t)⋅𝐬 )⟨𝜙𝐬 |𝜙𝐩 ⟩
𝐬
i
= |𝜙𝐩 ⟩ − |𝜙𝐩 ⟩(1 − e ℏ 𝛼(t)⋅𝐩 )
i
= e ℏ 𝛼(t)⋅𝐩 |𝜙𝐩 ⟩ (1.28)

Also we have
8 F.H.M. Faisal

e e
− 𝐀(t) ⋅ 𝜋c |𝜙𝐩 ⟩ = − 𝐀(t) ⋅ 𝐩|𝜙𝐩 ⟩ (1.29)
mc mc
Thus, substituting (1.27) in (1.26) for the continuum case, we get on the left hand
side
i t
(Ep + e
2 A2 (t′ )
)dt′ −𝛼(t)⋅𝐩) e2 A2 (t)
l.h.s. = e− ℏ (∫ 2mc2 (Ep + − 𝛼(t)
̇ ⋅ 𝐩)|𝜙𝐩 ⟩ (1.30)
2mc2
and on the right hand side,

i t
(Ep + e
2 A2 (t′ )
)dt′ −𝛼(t)⋅𝐩)
𝐩op 2 Ze2 e2 A2 (t′ ) e
r.h.s. = e− ℏ (∫ 2mc2 (( − )+ − 𝐀(t) ⋅ 𝐩)|𝜙𝐩 ⟩
2m r 2mc 2 mc
(1.31)

p 2
e
Noting that 𝛼(t)
̇ = mc 𝐀(t) and HCou |𝜙𝐩 ⟩ = Ep |𝜙𝐩 ⟩, where, Ep = 2m , one easily finds
from above that the l.h.s = r.h.s and hence the given solution is exactly fulfilled.
In a similar way it is easily seen that
∑ i
T(𝜋c )|𝜙D ⟩ = |𝜙D ⟩ − |𝜙𝐬 ⟩(1 − e ℏ 𝛼(t)⋅𝐬 )⟨𝜙𝐬 |𝜙D ⟩
𝐬
= |𝜙D ⟩ + 0
(1.32)

since, the overlap integral between the discrete and the continuum eigenstates of the
Coulomb Hamiltonian vanish by orthogonality, ⟨𝜙𝐬 |𝜙D ⟩ = 0. Hence, on substituting
(1.27) in (1.26) in the discrete case we get

i t
(ED + e
2 A2 (t′ )
dt′ +0) e2 A2 (t)
l.h.s. = e− ℏ ∫ 2mc2 (ED + + 0)|𝜙D ⟩ (1.33)
2mc2
and

i t
(ED + e
2 A2 (t′ )
)dt′ +0)
𝐩op 2 Ze2 e2 A2 (t′ )
r.h.s. = e− ℏ (∫ 2mc2 (( − )+ + 0)|𝜙D ⟩ (1.34)
2m r 2mc2
𝐩2 2
Moreover, ( 2m
op
− Zer )|𝜙D ⟩ = ED |𝜙D ⟩ and, therefore, the l.h.s = r.h.s and the verifi-
cation is complete.
To summarise, the complete set of solutions of the CV-Schroedinger equation
defined by (1.26) is given explicitly for the continuum case by
t p2
−ℏ ∫ i
( 2m + 12 A(t′ )2 − ec 𝐀(t′ )⋅𝐩)dt′
𝛷𝐩(−) (𝐫, t) = 𝜙(−)
𝐩 (𝐫)e
2c (1.35)

and for the discrete case by

1 Strong-Field S-Matrix Series with Coulomb Wave Final State 9

t p2
i
( 2m + 12 A(t′ )2 )dt′
𝛷D (𝐫, t) = 𝜙D (𝐫)e− ℏ ∫ 2c (1.36)

where we may recall that [17]

1 𝜋𝜂p i i
⟨𝐫|𝜙(−)
𝐩 ⟩ = e 2 𝛤 (1 + i𝜂p )e ℏ 𝐩⋅𝐫 1 F1 (−i𝜂p , 1, − (pr + 𝐩 ⋅ 𝐫)) (1.37)
L3∕2 ℏ
Zℏ
with 𝜂p = pa0
, and the well known hydrogenic bound states,

𝜙D≡(n,l,m) (𝐫) = Nnl Rnl (r)Ylm (𝜃, 𝜙)

Rnl (r) = (2𝜅n r)l e−𝜅n r F1 (−n + l + 1, 2l + 2, 2𝜅n r)
√
(2𝜅n )3∕2 𝛤 (n + l + 1)
Nnl = (1.38)
𝛤 (2l + 2) 2n𝛤 (n − l)
√
−2mED
with 𝜅n ≡ naZ = ℏ2
.
0
Having thus found the explicit form of both HCV (t), (1.25), and the complete set of
solutions [(1.27) or, (1.35) and (1.36)] of the Coulomb-Volkov Schroedinger equa-
tion, (1.26), we may now write down the associated Coulomb-Volkov propagator
GCV (t, t′ ) explicitly,

i
GCV (t, t′ ) = − 𝜃(t − t′ )
ℏ
∑ i t (𝐩− ec 𝐀(t′′ )2
dt′′
× { |𝜙𝐩 ⟩e− ℏ ∫t′ 2m ⟨𝜙𝐩 |
𝐩
∑ i t e2 A2 (t′′ )
)dt′′
+ |𝜙nlm ⟩e− ℏ ∫t′ (Enl + 2mc2 𝜙nlm |} (1.39)
nlm

1.4 Coulomb-Volkov S-Matrix Series

We are now in a position to obtain the desired S-matrix amplitude. From the knowl-
edge of HCV (t) obtained above the rest-interaction in the final-state turns out to be,

VCV (t) = H(t) − HCV (t)

e
= (− 𝐀(t) ⋅ (𝐩𝐨𝐩 − 𝜋𝐜 ) + Vs.r. (𝐫)) (1.40)
mc
Therefore, substitutions of the initial and the final rest-interactions as well as the
expansion of G(t, t′ ) in terms of the Volkov propagator and the intermediate rest-
2
interaction V0 (𝐫) = (− Zer + Vs.r (𝐫)) into the amplitude expression (1.11), immedi-
ately yield:
10 F.H.M. Faisal

Sfi =⟨𝛷𝐩 (t)|𝜙i (t)⟩

i
− dt ⟨𝛷 (t )|V (t )|𝜙 (t )⟩
ℏ∫ 1 𝐩 1 i 1 i 1
i e
− dt dt ⟨𝛷 (t )|(− 𝐀(t2 ) ⋅ (𝐩op − 𝜋c ) + Vs.r. (𝐫2 ))×
ℏ∫ 2 1 𝐩 2 mc
×GVol (𝐫2 , t2 ; 𝐫1 , t1 )Vi (t1 )|𝜙i (t1 )⟩
⋯ (1.41)

Thus, finally, we have arrived at the desired systematic S-matrix series for the strong-
field ionisation amplitude, which systematically accounts for the final state long
range Coulomb interaction through the Coulomb-Volkov state in all orders. We quote
the first three terms more explicitly and, give the rule of construction for all the higher
order terms of the series:
∞
∑
Sfi = Sfi(n) (1.42)
n=0

where,
Sfi(0) = ⟨𝛷𝐩 (𝐫, t)|𝜙i (𝐫, t)⟩ (1.43)

i e e2 A2 (t1 )
Sfi(1) = − dt1 ⟨𝛷𝐩 |(𝐫1 , t1 )(− 𝐀(t1 ) ⋅ 𝐩op + )|𝜙i (𝐫1 , t1 )⟩ (1.44)
ℏ∫ mc 2mc2

i e
Sfi(2) = − dt dt ⟨𝛷 (𝐫 , t )|(− 𝐀(t2 ) ⋅ (𝐩op − 𝜋c ) + Vs.r. (𝐫2 ))GVol (𝐫2 , t2 ; 𝐫1 , t1 )
ℏ∫ 2 1 𝐩 2 2 mc
e e2 A2 (t1 )
× (− 𝐀(t1 ) ⋅ 𝐩op + )|𝜙i (𝐫1 , t1 )⟩ (1.45)
c 2mc2

i e
Sfi(3) = − dt dt dt ⟨𝛷 (𝐫 , t )|(− 𝐀(t3 ) ⋅ (𝐩op − 𝜋c ) + Vs.r. (𝐫3 ))
ℏ∫ 3 2 1 𝐩 3 3 mc
Ze2
×GVol (𝐫3 , t3 ; 𝐫2 , t2 )(− + Vs.r. (𝐫2 ))GVol (𝐫2 , t2 ; 𝐫1 , t1 )
r2
e e2 A2 (t1 )
×(− 𝐀(t1 ) ⋅ 𝐩op + )|𝜙i (𝐫1 , t1 )⟩
mc 2mc2
… (1.46)

where the angle brackets stand for the integration with respect to the space coordi-
nates and “⋯” stands for the higher orders terms. The higher order terms can be
written down easily, if required, for they follow the same pattern as the third order
term but are to simply extended by an extra intermediate factor GVol V0 and an extra
time integration for each successive order, to all orders.
1 Strong-Field S-Matrix Series with Coulomb Wave Final State 11

1.5 Strong-Field S-Matrix for Short-Range Potentials

Before ending this report it is interesting to consider the S-matrix expansion of the
strong-field amplitude in the presence of an asymptotically short range potential.
This can be obtained simply by taking the limit Z = 0 in the result derived above. In
i
this limit the Coulomb waves 𝜙𝐩 (𝐫) reduce to the plane waves e ℏ 𝐩⋅𝐫 and the Coulomb-
Volkov state 𝛷𝐩 (𝐫, t) (1.19) reduces to the Volkov state (1.13). This implies that
the factor with the final state interaction in all terms, beginning with the second
order term, reduces to the short range potential Vs.r. (𝐫) only, due to the following
simplification
e e
⟨𝐩|(− 𝐀(t) ⋅ (𝐩op − 𝜋c ) + Vs.r. (𝐫)) = (− 𝐀(t) ⋅ (𝐩 − 𝐩)⟨𝐩| + ⟨𝐩|Vs.r. (𝐫))
mc mc
= ⟨𝐩|Vs.r. (𝐫) (1.47)

Also, the intermediate interaction V0 in all terms (from the second order term on-
wards) for Z = 0 reduces to the short-range potential Vr.s. (𝐫) only. Hence, in general,
for Z ≡ 0, the Coulomb-Volkov S-matrix series, (1.41), goes over to the simpler se-
ries

Sfi (Z = 0) = ⟨𝜓𝐩 (t)|𝜙i (t)⟩

i
− dt ⟨𝜓 (t )|V (t)|𝜙i (t)⟩
ℏ∫ 1 𝐩 1 i
i
− dt dt ⟨𝜓 (t )|V (𝐫 )G (𝐫 , t ; 𝐫 , t )V (t )|𝜙 (t)⟩
ℏ ∫ 2 1 𝐩 2 s.r. 2 Vol 2 2 1 1 i 1 i
i
− dt dt dt ⟨𝜓 (t )|V (𝐫 )G (𝐫 , t ; 𝐫 , t )V (𝐫 )
ℏ ∫ 3 2 1 𝐩 3 s.r. 3 Vol 3 3 2 2 s.r. 2
× GVol (𝐫2 , t2 ; 𝐫1 , t1 )Vi (t1 )|𝜙i (t1 )⟩
+ …. (1.48)

Equation (1.48) provides a strong-field S-matrix expansion when there is no long-

range Coulomb interaction preset asymptotically. This occurs with all asymptotically
neutral systems with effective core charge Z = 0 (as seen by the ejected electron) e.g.
for the case of electron-detachment from negative ions. Equation (1.48) is apparently
analogous in structure to the usual SFA with the plane-wave Volkov final state. Note,
however, that in (1.48) the plane-wave Volkov final state and the short-range potential
Vs.r. , appear self-consistently together.

1.6 Concluding Remarks

We may end this report with a few short remarks.

12 F.H.M. Faisal

(a) For the sake of concreteness we have presented the result starting with the
Schroedinger equation of the interacting system in the minimal coupling gauge (so-
called velocity gauge). A similar result can be derived in the same way (or by a
gauge transformation) starting from the Schroedinger equation in the so-called length
gauge. This and the issue of gauge invariance of the theory will be presented and
discussed elsewhere.
(b) It is expected that the present theory would be helpful in clarifying a number
of issues of much current interest in strong-field physics involving (i) the shape of the
so-called “low energy structure” (LES) [18], (ii) the number of peaks associated with
the “very low energy structures” (VLES) [19, 20], (iii) origin of the “zero energy
structure” (ZES) [21], and (iv) possible existence of an as yet unknown “threshold
law” for the energy dependence of the strong-field ionization probability. Most or
all of these issues possibly depend crucially on the role of the long-range final state
Coulomb interaction specially in the low energy regime (e.g. c.f. [22]).
(c) The explicit expression of the Coulomb-Volkov propagator (or Green’s func-
tion) GCV (t, t′ ) given here suggests that the theory also would be useful for strong-
field processes involving excitation of the discrete states, either as a final state, or as
intermediate mediating states, or both, for example, in connection with the so-called
“frustrated ionization” (e.g. [23]) in strong fields.
(d) We may point out for that the terms of the S-matrix series (1.42), for example,
the amplitudes Sif(1) and Sif(2) , could be evaluated by a combination of stationary phase
method and numerical evaluation, provided the coordinates dependent Coulomb in-
tegrals can be evaluated analytically, for example by Norsieck’s method [24]. The
Coulomb integral of the first order amplitude (and of the first factor of the second
order amplitude) are of the form

(1) e
M𝐩,i = 𝜙(−)∗
𝐩 (𝐫)(− 𝐀(t) ⋅ 𝐩op )e−𝜅r d3 r (1.49)
∫ mc
Zℏ
where 𝜂(p) ≡ pa0
. The second Coulomb integral of the 2nd order amplitude is of the
form

(2) e
M𝐩,𝐤 = 𝜙(−)∗
𝐩 (𝐫)(− 𝐀(t) ⋅ (𝐩op − 𝜋c ))ei𝐤⋅𝐫 d3 r
∫ mc
e
= (− 𝐀(t) ⋅ (𝐤 − 𝐩)) 𝜙(−)∗ (𝐫)ei𝐤⋅𝐫 d3 r
mc ∫ 𝐩
(1.50)

They have the same form as of the following two prototypical integrals which we
give explicitly below:

I1 = e−i𝐬⋅𝐫 1 F1 (i𝜂s , 1, i(sr + 𝐬 ⋅ 𝐫))(𝜀 ⋅ 𝐩op )e−𝜅r d3 r

∫
= 8𝜋ℏ𝜅(1 + i𝜂s )(𝜀 ⋅ 𝐬)∕((𝜅 + is)(2−i𝜂s ) (𝜅 − is)(2+i𝜂s ) ) (1.51)
1 Strong-Field S-Matrix Series with Coulomb Wave Final State 13

I2 = (𝜀 ⋅ (𝐤 − 𝐬)) × Lim.𝜆→0 e−i𝐬⋅𝐫 1 F1 (i𝜂s , 1, i(sr + 𝐬 ⋅ 𝐫)ei𝐤⋅𝐫 e−𝜆r d3 r

∫
8𝜋s𝜂s q2
= (𝜀 ⋅ 𝐪) × ( 2 )i𝜂s (1.52)
q2 (q2+ 2𝐪 ⋅ 𝐬) q + 2𝐪 ⋅ 𝐬
Z
where, 𝐪 ≡ 𝐤 − 𝐬, 𝜂s = sa0 , and 𝜀 stands for an unit vector. The additional integra-
tion over the intermediate momentum 𝐤 can be performed e.g. by the stationary
phase method (or otherwise), and the first time-integration can be done either ana-
lytically or by the stationary phase method, while the second time-integration can be
done e.g. numerically. (Application of the theory to the observed low energy struc-
tures/phenomena [18–21] with more details of the calculations and discussions of
the results will be presented elsewhere).

References

1. L.V. Keldysh, Sov. Phys. JETP 20, 1307 (1965)

2. F.H.M. Faisal, J. Phys. B: At. Mol. Opt. Phys. 6, L89 (1973)
3. H.R. Reiss, Phys. Rev. A 22, 1786 (1980)
4. A.I. Nikishov, V.I. Ritus, Sov. Phys. JETP 23, 168 (1966)
5. A.M. Perelomov et al., Sov. Phys. JETP 50, 1393 (1966)
6. V.S. Popov, Phys. Usp. 42, 733 (1999)
7. M. Klaiber et al., Phys. Rev. A 87, 023417 (2013)
8. V.P. Krainov, J. Opt. Soc. Am. B 14, 425 (1997)
9. S.V. Popruzhenko et al., Phys. Rev. A 77, 053409 (2008)
10. T.-M. Yan et al., Phys. Rev. Lett. 105, 253002 (2010)
11. X.-Y. Lai et al., Phys. Rev. A 92, 043407 (2015)
12. L. Torlina, O. Smirnova, Phys. Rev. A 86, 043408 (2012)
13. A. Galstyan et al., Phys. Rev. A 93, 023422 (2016)
14. A. Becker, F.H.M. Faisal, J. Phys. B: At. Mol. Opt. Phys. 38, R1 (2005)
15. M. Jain, N. Tzoar, Phys. Rev. A 18, 538–45 (1978)
16. C. Leone et al., Nuouo Cimento D 9, 609 (1987)
17. L.D. Landau, E.M. Lifshitz, Quantum Mechanics (Pergamon Press, Oxford, 1965)
18. C.I. Blaga et al., Nature Phys. 5, 335 (2008)
19. W. Quan et al., Phys. Rev. Lett. 103, 093001 (2009)
20. C. Wu et al., Phys. Rev. Lett. 109, 043001 (2012)
21. J. Dura et al., Nature Sci. Rep. 3, 2675 (2013)
22. F.H.M. Faisal, Nature Phys. 5, 319 (2009)
23. T. Nubbemeyer et al., Phys. Rev. Lett. 101, 233001 (2008)
24. A. Nordsieck, Phys. Rev. 93, 785 (1954)
Chapter 2
Multiconfiguration Methods
for Time-Dependent
Many-Electron Dynamics

Erik Lötstedt, Tsuyoshi Kato and Kaoru Yamanouchi

Abstract A concise overview of time-dependent multiconfiguration methods for the

approximate solution of the time-dependent Schrödinger equation for many-electron
systems in intense laser fields is presented. In all the methods introduced, the total
wave function of the system is written as a linear combination of Slater determinants.
The methods can be divided into two classes, one class in which the orbitals used to
construct the Slater determinants are time-independent, and the other class in which
the orbitals are time-dependent. The key ideas of these two classes are reviewed,
focusing on the scheme used for reducing the number of Slater determinants in the
expansion of the wave function. Also described is our recent proposal, in which
the number of Slater determinants is not reduced, but the matrix of configuration-
interaction coefficients is approximated by a product of three smaller matrices.

2.1 Introduction

A common theme in theoretical chemistry is to develop efficient procedures for

describing electron-electron interaction in atoms and molecules. Starting with the
Hartree-Fock approximation, which includes the electron-electron interaction only
on a mean-field level, researchers have proposed a variety of methods such as config-
uration interaction (CI) and coupled-cluster (CC) theory [1] to solve approximately
the Schrödinger equation (SE)
H𝛹 = E𝛹 , (2.1)

E. Lötstedt (✉) ⋅ T. Kato ⋅ K. Yamanouchi

Department of Chemistry, School of Science, The University
of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-0033, Japan
e-mail: lotstedt@chem.s.u-tokyo.ac.jp
T. Kato
e-mail: tkato@chem.s.u-tokyo.ac.jp
K. Yamanouchi
e-mail: kaoru@chem.s.u-tokyo.ac.jp

© Springer International Publishing AG 2017 15

K. Yamanouchi et al. (eds.), Progress in Ultrafast Intense Laser Science XIII,
Springer Series in Chemical Physics 116, https://doi.org/10.1007/978-3-319-64840-8_2
16 E. Lötstedt et al.

where H is the Hamiltonian, E is the eigenenergy, and 𝛹 is the wave function. The
non-relativistic ground state energy levels E0 of many-electron molecules (where the
number of electrons N ≤ 15) can be obtained to about 0.01 eV accuracy using the CI
method [2] or the CC method [3]. For small systems like He [4, 5] and H2 [6], the
exact eigenenergies of the bound states can be calculated. It remains a challenge to
obtain reliable estimates of the energies of highly excited states [7–9].
Much less effort has been spent on developing methods for obtaining solutions to
the time-dependent Schrödinger equation (TDSE),

𝜕𝛹 (t)
iℏ = H(t)𝛹 (t), (2.2)
𝜕t

where the Hamiltonian H(t) depends on time. The time-dependence of the Hamil-
tonian usually arises from the coupling with a laser field. Equation (2.2) describes
an initial-value problem, where we provide the initial wave function 𝛹 (t = 0) = 𝛹0 ,
which is the lowest energy solution to (2.1), and we seek an approximation to the
wave function 𝛹 (t) for 0 ≤ t ≤ T for some finite time T. To compute 𝛹 (t) could be a
significantly more difficult problem than solving the time-independent SE (2.1). The
reason is that we require a method that describes well the electron correlation not
only in the initial state 𝛹 (0) but also at later time t. Particularly in the case of intense
laser-molecule and laser-atom interactions, the wave function is strongly perturbed
by the laser field so that 𝛹 (t) becomes in general very different compared to the ini-
tial state 𝛹 (0). After the interaction with the laser field, the wave function becomes
a superposition of the initial state and more than a few excited states, which may
include singly excited states, doubly excited states, Rydberg states, and continuum
states representing ionization. Ideally, a theoretical method we develop can describe
all of these components equally well.
On the experimental side, a variety of phenomena have been observed, the mech-
anisms of which need to be explored theoretically. The best studied example is the
correlated motion of the two electrons in helium, leading to non-sequential double
ionization [10, 11] and the creation of wave packets consisting of doubly-excited
states [12]. Signatures of correlated electron dynamics can also be seen in high-
harmonic spectra of molecules [13, 14] and atoms [15], and in molecular dissocia-
tion [16, 17].
In the first part of this chapter, Sect. 2.2, we introduce the basics of multicon-
figuration-based wave function approaches to the approximate solution of the TDSE
(2.2). A multiconfiguration wave function is a wave function which consists of
several or many Slater determinants. The simplest wave function of this kind, in
which only one Slater determinant is included, is called the Hartree-Fock (HF)
wave function. Adding more Slater determinants gives a better description of the
dynamics of the system. Since the inclusion of all possible Slater determinants
is computationally unfeasible for any system having more than two electrons, the
essential point of a multiconfiguration method is to find a way of effectively reduc-
ing the number of Slater determinants. In Sect. 2.3, we review three approaches for
reducing the number of Slater determinants: the time-dependent configuration inter-
Another random document with
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The Project Gutenberg eBook of Refraction and
muscular imbalance, as simplified through the
use of the ski-optometer
This ebook is for the use of anyone anywhere in the United States
and most other parts of the world at no cost and with almost no
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Title: Refraction and muscular imbalance, as simplified through the

use of the ski-optometer

Author: Daniel Woolf

Release date: August 29, 2023 [eBook #71517]

Language: English

Original publication: New York: Theodore S. Holbrook, 1921

Credits: deaurider and the Online Distributed Proofreading Team at

https://www.pgdp.net (This file was produced from images
generously made available by The Internet Archive)

*** START OF THE PROJECT GUTENBERG EBOOK

REFRACTION AND MUSCULAR IMBALANCE, AS SIMPLIFIED
THROUGH THE USE OF THE SKI-OPTOMETER ***
 Ski-optometer Master Model 215
Embodying in a Single Instrument, in Convenient Form,
Cylindrical and Spherical Lenses, in Combination
with Appliances for Testing and Correcting
Muscular Imbalance.

Refraction and
Muscular Imbalance
 As Simplified Through the Use
of the Ski-optometer

By

DANIEL WOOLF
WOOLF INSTRUMENT CORPORATION
New York: 516 Fifth Avenue

Copyright 1921
By WOOLF INSTRUMENT CORPORATION

Published by
Theodore S. Holbrook
New York
 CONTENTS
Page
Chapter I
Ski-optometer Construction 1
Convex Spherical Lenses 2
Operates and Indicates Automatically 6
Concave Spherical Lenses 7

Chapter II
Cylindrical Lenses 10
Obtaining Correct Focus 11
Why Concave Cylinders Are Used Exclusively 14
Transposition of Lenses 14

Chapter III
How the Ski-optometer Assists in Refraction 17
The Use of the Ski-optometer in Skioscopy 17
A Simplified Skioscopic Method 20
Employing Spheres and Cylinders in Skioscopy 22
Use of the Ski-optometer in Subjective Testing 23
A Simplified Subjective Method 24
Procedure for Using Minus Cylinders Exclusively 26
Constant Attention Not Required 29

Chapter IV
Important Points in Connection with the
Use of the Ski-optometer 30
Elimination of Trial-Frame Discomfort 30
Rigidity of Construction 31
How to Place the Ski-optometer in Position 32
Cleaning the Lenses 33
Accuracy Assured in Every Test 34
Built to Last a Lifetime 35
 Chapter V
Condensed Procedure for Making Sphere and
Cylinder Test with the Ski-optometer 37
Subjective Distance Test 37
Subjective Reading Test 40

Chapter VI
Muscular Imbalance 41
The Action of Prisms 42
The Phorometer 43
The Maddox Rod 44
Procedure for Making the Muscle Test 45
Binocular and Monocular Test 47

Chapter VII
The Binocular Muscle Test 48
Made with the Maddox Rod and Phorometer 48
Esophoria and Exophoria 50
Making Muscle Test Before and After Optical Correction 52
When to Consider Correction of Muscular Imbalance 53
Four Methods for Correction of Muscular Imbalance 54
The Rotary Prism 54
Use of the Rotary Prism in Binocular Muscle Tests 56

Chapter VIII
The Monocular Duction Muscle Test 58
Made with Both Rotary Prisms 58
Locating the Faulty Muscle 58
Adduction 59
Abduction 61
Superduction 62
Subduction 63
Procedure for Monocular Muscle Testing 64
Diagnosing a Specific Muscle Case 65
 Chapter IX
First Method of Treatment—Optical Correction 70
Esophoria 70
Treatment for Correcting Esophoria in Children 72
How Optical Correction Tends to Decrease 6°
Esophoria in a Child 74

Chapter X
Second Method of Treatment—Muscular Exercise 75
Made with Two Rotary Prisms and Red Maddox Rod 75
Exophoria 75
An Assumed Case 78
Effect of Muscular Exercise 80
Home Treatment for Muscular Exercise—
Square Prism Set Used in Conjunction with
the Ski-optometer 82

Chapter XI
Third Method of Treatment—Prism Lenses 84
When and How Employed 84
Prism Reduction Method 85

Chapter XII
A Condensation of Previous Chapters on the Procedure
for Muscle Testing with the Ski-optometer 87
Four Methods of Treating an Imbalance Case when
the Preceding One Fails 90
Prisms 92
Cyclophoria 92

Chapter XIII
Cyclophoria 93
Made with Maddox Rods and Rotary Prisms 93

Chapter XIV
Cycloduction Test 99
Made with the Combined Use of the Two Maddox Rods 99
Treatment for Cyclophoria 102

Chapter XV
Movements of the Eyeballs and their Anomalies 105
Monocular Fixation 105
Binocular Fixation 106
Orthophoria 107
Heterophoria 107
Squint 108
Varieties of Heterophoria and Squint 109

Chapter XVI
Law of Projection 114
Suppression of Image 115
Monocular Diplopia 115
Table of Diplopia 116
Movement of Each Eye Singly 117
Subsidiary Actions 118
Field of Action of Muscles 120
Direction of the Gaze 120
Primary Position—Field of Fixation 121
Binocular Movements 121
Parallel Movements 122
Lateral Rotators 123
Eye Associates 124
Movements of Convergence 125
Movements of Divergence 125
Vertical Divergence 126
Orthophoria 126
Heterophoria 126
Subdivisions 126

Chapter XVII
Symptoms of Heterophoria 128
Treatment 130
Destrophoria and Laevophoria 132
The demands of the day for maximum efficiency in
the refracting world are largely accountable for the
inception, continuous improvement and ultimate
development of the master model Ski-optometer.
The present volume, dealing with the instrument’s
distinctive operative features, has been prepared not
only for Ski-optometer users, but also for those
interested in the simplification of refraction and
muscular imbalance.
The author is indebted for invaluable counsel, to

Louis J. Ameno, M.D., New York.

E. LeRoy Ryer, O.D., New York.
Jos. D. Heitger, M.D., Louisville, Ky.
W. B. Needles, N.D., Kansas City, Mo.
 INTRODUCTORY

W
hile in a measure the conventional trial-case still serves its
purpose, so much of the refractionist’s time is consumed
through the mechanical process of individually transferring the
trial-case spheres and cylinder lenses, that far too little thought is
given to muscular imbalance, notwithstanding its importance in all
refraction cases.
Dr. Samuel Theibold, of Johns Hopkins University, in a recent
address before the American Medical Association, stated that the
average refractionist was inclined to devote an excess of time to
general refraction, completely overlooking the important test and
correction of muscular imbalance. If the latter is to be at all
considered, general refraction must be simplified—without impairing
its accuracy—a result that is greatly facilitated through the use of the
Ski-optometer.
One must admit that tediously selecting the required trial-case
lens—whether sphere, cylinder or prism—watching the stamped
number on the handle—continual wiping and inserting each
individual lens in a trial-frame is a time-consuming practise. This is
readily overcome, however, through the employment of the Ski-
optometer.
In a word, the Ski-optometer is practically an automatic trial-case,
bearing the same relation to the refracting room as the accepted
labor and time-saving devices of the day bear to the commercial
world.
The present volume has accordingly been published, not alone in
the interest of those possessing a Ski-optometer, but also for those
interested in attaining the highest point of efficiency in the work of
refraction and muscular imbalance.
Ski-optometer Lens Battery (almost actual size)
showing how sphere and cylinder lenses are
procured.
After obtaining FINAL results, your prescription is
automatically registered,
ALL READY for you to transcribe.
Fig. 1—The three time-saving moves necessary in
the operation of the Ski-optometer.
 Chapter I
SKI-OPTOMETER CONSTRUCTION

A
far better understanding of the instrument will be secured if the
refractionist possessing a Ski-optometer will place it before him,
working out each operation and experiment step by step in its
proper routine.
The three moves as outlined in Fig. 1 should first be thoughtfully
studied and the method of obtaining the spheres and cylinders
carefully observed.
 Fig. 2—To Obtain Plano.
1—Set spherical indicator at “000” as illustrated above.
2—Set cylinder indicator to “0”.
3—Set pointer of supplementary disk at “open”.
The instrument should then be set at zero or “plano,” a position
indicated by the appearance of the three “0 0 0” at the spherical
register, in conjunction with one “0” or zero, for the cylinder at its
register, marked “CC Cyl.”
After this move, the supplementary disk’s pointer should be set at
“open” (Fig. 2).
 Fig. 3—To obtain sphericals, turn this
Single Reel as shown by dotted finger. This
assures an automatic and simultaneous
registration at sphere indicator of focus of
lens appearing at sight opening.

Convex Spherical Lenses

A careful study will show that the Ski-optometer’s spherical lenses
are obtained by merely turning the smaller reel (Fig. 3). The first
outward turn of this reel, toward the temporal side of the instrument,
draws into position in regular order the spherical lenses +.25, +.50,
+.75, and +1.D., as shown in Fig. 3a.
3-A—Outer spherical reel containing Cx. sphericals
from .025 to 1.00D and a blank.
 3-B—Inner spherical disk containing Cx. sphericals,
automatically turns within 3-A.

3-C—Supplementary spherical disk.

By means of a concealed tooth gear, an inner disk is automatically
picked up, placing its first lens +1.25D in position (Fig. 3b). This
+1.25D spherical lens remains stationary while the outer disk again
revolves, adding to it the original +.25, +.50, +.75 and +1.D., the latter
totalling +2.25D. At this point, the instrument again automatically picks
up its inner disk, thereby placing its second lens, +2.50D, in position.