Advances In Multi-Photon Processes and Spectroscopy, Volume 14.

349 Pages·2000·12.628 MB·English

by  Gordon, R. J., Fujimura, Y.

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Volume 14
QUANTUM CONTROL OF
MOLECULAR REACTION DYNAMICS:
Proceedings of the US-Japan Workshop
held in Honolulu, USA
Edited by
R J Gordon
Y Fujirnura
World Scientific
ADVANCES IN MULTI-PHOTON PROCESSES AND SPECTROSCOPY
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QUANTUM CONTROL OF
MOLECULAR REACTION DYNAMICS:
Proceedings of the US-Japan Workshop
Honolulu, USA 12 -15 December 1999
Edited by
R J Gordon
University of IllinoisatChicago, USA
Y Fujimura
Tohoku University, JAPAN
World Scientific
PSingapore • New Jersey • London • Hong Kong
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ADVANCES IN MULTI-PHOTON PROCESSES AND SPECTROSCOPY -Vol. 14
Copyright ® 2001 by World Scientific PublishingCo. Pte. Ltd.
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PREFACE
The field of coherent control may be broadly defined as the utilization of
the quantum mechanical properties of matter to control the motion of electrons and
nuclei. Included within this definition are the control of chemical reactions , control
of the motion of charge carriers in solids, alignment of molecules in gases, liquids,
and thin films, and trapping and manipulation of the center of mass motion of atoms
and molecules.
Although first experiments in the control of atomic and molecular motion
were performed in the early seventies, coherent control of chemical reactions can be
traced to the mid-eighties, when Paul Brumer and Moshe Shapiro initiated the use of
quantum mechanical interference, and David Tannor and Stuart Rice initiated the
use of wave packets to control chemical processes. The field remained largely
theoretical until the early nineties, when experiments by Dan Elliot and Robert
Gordon implemented the Brumer-Shapiro theory, and Graham Fleming, Kent
Wilson, Gustav Gerber, and Philip Bucksbaum, among others, used the wave packet
method. Coherent control of a branching ratio was first demonstrated by Thomas
Baumert and Gustav Gerber in 1994 using the wave packet method and by Gordon
and coworkers in 1995 using the quantum mechanical interference method. Since
then there has been a flood of new experimental and theoretical developments.
Many key objectives, however, such as bond-selective photochemistry and the use
of tailored laser pulses to control electronic and nuclear motion, are still in their
infancy. The first international meeting devoted exclusively to laser control was
held in Neve Ilan, Israel, in May, 1996. A second international meeting was held in
Cancun in November, 1997, and the first Gordon Research Conference on Quantum
Control was held in August, 1999.
In recent years Japanese scientists have made significant contributions to
the field of coherent control. Some of their notable achievements include phase
control of the photoionization of large polyatomic molecules in the gas phase by
Kawasaki, the alignment of molecules with strong laser fields by Sakai, local
control theory applied to isomerization and dissociation reactions by Fujimura, and
a control theory based on the dressed state picture by Nakamura. Despite the
growing Japanese research effort, there has been relatively little interaction between
v
vi
Japanese and American workers in this field. In order to promote greater interaction
between these communities, we convened a workshop in Honolulu in December,
1999 that was attended by thirty-one scientists from both countries. As the
contributions to this volume attest, the workshop provided a forum for presenting
the leading edge issues in this field, which are continuing to be addressed by
researchers in both countries.
The main findings of this workshop (and the participants who presented
them) may be summarized as follows:
• Learning algorithms have opened the door to controlling many processes
(Bucksbaum and Stroud).
• Wave packet engineering has become a practical reality (Fujimura , Leone,
Kleiman, Bucksbaum, Stroud, Misawa).
• The Hamiltonian can be altered by dressing it in a strong field (Nakamura,
diMauro, Liu, Kono).
• Non-adiabatic transitions may be exploited for control (Nakamura, Ohmori).
• External degrees of freedom may be controlled (Sakai, Kawasaki, Dantus, Kasai).
• Progress is being made in understanding and controlling decoherence (Gruebele,
Makri, Leone, Petek, Lozovoy, Tominaga).
• Control in condensed phases is robust (Bucksbaum, Kleiman, Potz, Misawa,
Petek, Kobayashi).
• The phase lag is a powerful tool both for controlling dynamics and for discovering
properties of the continuum (Gordon, Khachatrian, Zhu, Nakajima, Lozovoy,
Scully).
• Useful applications of coherent control are envisioned (Bucksbaum, Stroud,
Fujimura, Scully).
This workshop was made possible by grants from the United States National
Science Foundation and the Japanese Society for the Promotion of Science. We
wish to acknowledge and thank these agencies for their generous support.
R. J. Gordon
Y. Fujimura
Contents
Preface v
Part I. Control of Wave Packets 1
Time-Shifting the Dynamics of Li2 Multistate Rovibrational Wave
Packets by State Selective Coherent Phase Control 3
ZoharAmitay, Radoslaw Uberna, and Stephen R. Leone
Strong Field Ultrafast Quantum Control with Learning Algorithms 15
Philip H. Bucksbaum
Quantum Control of Isomerization and Enantiomer Preparation 30
Y Fujimura, L. Gonzalez, K. Hoki, J. Manz, Y Ohtsuki,
and H. Umeda
Nonexponential Dephasing and Control of Molecular Quantum Systems 47
Martin Gruebele and Vance Wong
What Role Can Four-Wave Mixing Techniques Play in Coherent Control? 62
Vadim V Lozovoy, Emily J. Brown, Igor Pastirk,
Bruna I. Grimberg, and Marcos Dantus
Using Optical Collision to Control the Transition-Region Dynamics 80
Kenji Ohmori
Part II. Coherent Phase Control 97
What Have We Learned from the Phase Lag in Coherent Control
Experiments? 99
Robert J. Gordon, Jeanette A. Fiss, Ani Khachatrian,
Kaspars Truhins, Langchi Zhu, and Tamar Seideman
Phase-Sensitive Photoionization of Atoms and itsApplication 113
Takashi Nakajima
Coherent Control, Fano Interference, and Non-Hermitian Interactions 126
Marlan O. Scully
vii
Part III. Alignment 133
Alignment of Neutral Molecules by a Strong Nonresonant Laser Field 135
Hirofumi Sakai, Jakob Juul Larsen, C. P. Safvan, Ida Wendt-Larsen,
Karen Marie Hilligs0e, Kasper Hald, and Henrik Stapelfeldt
Effect of IR Laser Pulses on the UV Photodissociation of CH3I and OCS 151
A. Sugita, M. Mashino, M. Kawasaki, and Y. Matsumi
Part IV. Intense Fields 163.
Electronic Dynamics and Structure of Molecules in Intense Laser Fields 165
Hirohiko Kono and Isao Kawata
Light-Dressed States of H2O in Intense Laser Fields 189
Shilin Liu, Akiyoshi Hishikawa, Atsushi Iwamae, and
Kaoru Yamanouchi
Atomic Dynamics at Long Wavelengths 203
B. Sheehy, J. D. D. Martin, T Clatterbuck, Dalwoo Kim,
L. F. diMauro, K. J. Schafer, M. B. Gaarde, and K. C. Kulander
New Way of Controlling Molecular Processes by Lasers 215
Yoshiaki Teranishi, Kuninobu Nagaya, and Hiroki Nakamura
Part V. Condensed Phases 229
Coherent Control of Molecular Excitations in the Condensed Phase Using
Optical Heterodyne Detected Raman Induced Kerr Effect Spectroscopy 231
Valeria D. Kleiman, Dale McMorrow, and Joseph S. Melinger
Dynamical Intensity Borrowing in Porphyrin J-Aggregates Revealed by
Sub-5-fs Spectroscopy 242
Takayoshi Kobayashi, Hideaki Kano, and Takashi Saito
Sub-5fs Real-Time Spectroscopy of Geometrical Relaxation Processes
in Polydiacetylenes 256
Takayoshi Kobayashi and Akira Shirakawa
ix
Localization in Dissipative Tunneling Systems Driven by
Monochromatic Light 266
Nancy Makri
Excited- and Ground-State Wave Packet Dynamics in Organic Materials
Induced by Femtosecond Chirped Pulses 286
Kazuhiko Misawa and Takayoshi Kobayashi
Optical and Structural Control of Quantum Interference in Semiconductors 302
W. Potz and T Krivosheev
Spectroscopic Application of THz Radiation Generated by Ultrashort Pulses:
Static Far Infrared Absorption Measurements in Condensed Phases 317
Keisuke Tominaga, Hideyuki Ohtake, Nobuhiko Sarukura,
Ken-Ichi Saitow, Hiroaki Sasakawa, Atsuo Tamura,
Igor V Rubtsov, and Keitaro Yoshihara