Laser Control and Manipulation of Molecules

378 Pages·2002·38.09 MB·English

by  A. D. Bandrauk

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In Laser Control and Manipulation of Molecules; Bandrauk, A., et al.;
ACS Symposium Series; American Chemical Society: Washington, DC, 2002.
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In Laser Control and Manipulation of Molecules; Bandrauk, A., et al.;
ACS Symposium Series; American Chemical Society: Washington, DC, 2002.
ACS SYMPOSIUM SERIES 821
Laser Control and
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acs.001 Manipulation of Molecules
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http://pub02-0821.f
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4, 20121/bk- A. D. Bandrauk, Editor
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n Se02 | Y. Fujimura, Editor
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American Chemical Society, Washington, DC
In Laser Control and Manipulation of Molecules; Bandrauk, A., et al.;
ACS Symposium Series; American Chemical Society: Washington, DC, 2002.
Library of Congress Cataloging-in-Publication Data
Laser control and manipulation of molecules / A. D. Bandrauk, editor, Y. Fujimura,
editor, R. J. Gordon, editor.
p. cm.—(ACS symposium series ; 821)
Includes bibliographical references and index.
ISBN 0-8412-3786-7
g 1. Lasers in chemistry—Congresses. 2. Laser manipulation (Nuclear physics)—
acs.or001 Congresses. 3. Molecular dynamics—Congresses.
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n Se02 | Copyright © 2002 American Chemical Society
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In Laser Control and Manipulation of Molecules; Bandrauk, A., et al.;
ACS Symposium Series; American Chemical Society: Washington, DC, 2002.
Foreword
The ACS Symposium Series was first published in 1974 to provide a
org mechanism for publishing symposia quickly in book form. The purpose
acs.001 of the series is to publish timely, comprehensive books developed from
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In Laser Control and Manipulation of Molecules; Bandrauk, A., et al.;
ACS Symposium Series; American Chemical Society: Washington, DC, 2002.
Preface
This volume is dedicated to the memory of Kent Wilson, who was a
pioneer in the rapidly growing field of coherent control of chemical reactions.
The chapters in this volume were presented at a symposium at the 2000
g International Chemical Congress of Pacific Basin Societies ("PacifiChem
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cs.01 2000") held in Honolulu, Hawaii, December 14-19, 2000. This symposium
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pubs.21.pr dWeaillst onw iatnhd thheis mstuadneipnutsla htiaovne mofa dlieg hmt awnyit hs emmainttaelr ,c oan ftrieibldu tiionn ws. hich Professor
http://02-08 Kent Wilson had an open-mindedness about people and ideas, which
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4, 221/ Philadelphia, Pennsylvania. This experiment in communal living helped Kent
10
er 0.1 develop a passion for free thinking. Kent's childhood experiments with moon­
ptembdoi: 1 Kshiisnteia aknodw fsikreyw's orlkasb oervaetonrtyu alalyt lHeda rhviamr dt o Cdool luengdee. rgTrhaed ugatree arteesseta rcinhf liune nGceeo rogne
43 on Se1, 2002 | KHeernstc'sh bsacciehn. tiKfice ngt rjoowintehd wHaesr shcihs bgarcahd'su agtreo uapn dw phoesnt -tdhoec tiodreaal omf eunstionrg, cDrousdsleedy
2.1e 2 molecular beams to study the chemical reactions of isolated molecules was in
15un its infancy. Kent's doctoral research dealt with the transition from rebound to
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o in 1964 was the development of the technique of photofragment spectroscopy.
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His experiments were among the first applications of laser radiation to probe
the structure and dynamics of molecules. His paper with Busch (2) on the re­
bound model for the partitioning of energy among molecular fragments has
been cited hundreds of times and is still valuable today.
The years that followed were a period of remarkable creativity in such
diverse fields as air pollution, chemical archeology, and the imaging of human
brain anatomy. An example of Wilson's interdisciplinary vision is his study of
the sources of metal used in ancient Nigerian bronzes. It was previously
believed that the lead used in these 15th to 19th century sculptures came from
northern Africa, but a statistical, isotopic analysis performed by Goucher et al.
xi
In Laser Control and Manipulation of Molecules; Bandrauk, A., et al.;
ACS Symposium Series; American Chemical Society: Washington, DC, 2002.
(3) proved that it came from Germany, possibly by a triangular trade route. In
the meanwhile, Kent's continuing interest in molecular reaction dynamics led
him to study the theory of chemical reactions in the liquid phase.
A hallmark of Kent's scholarship was his merging of science, art, and
showmanship. Numerous film productions by his undergraduate Senses
Bureau inspired a generation of young scientists. His film on protein synthesis,
which incorporates modern dance, rock-jazz, and poetry, is still shown in uni­
versities today, 30 years after its making. Wilson's conference presentations
were usually attended by standing-room-only crowds, many of whom came for
the pleasure of experiencing Kent's magical blend of science and art.
Kent's final decade, marked by his entry into the field of coherent
g control, was perhaps his most creative. At a workshop in Telluride in 1991, he
cs.or01 conceived of the idea of using a computer to tailor the properties of a light
a0 pulse, which could in turn be used to control the behavior of a wave packet (4).
ubs.1.pr In the following four years, Wilson's group laid much of the theoretical
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12 | k-20 calculating the optimal weak laser field for producing the best overlap of a
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4, 221/ wave packet with a given target in phase space. They illustrated the theory by
10 calculating the field needed to produce a "molecular cannon" wave packet fo­
ber 10.1 cused to a specified position and momentum, an incoming "reflectron" wave
ptemdoi: packet, and a bound, zero-momentum wave packet focused at a turning point
Se2 | of the trajectory. In later papers the Wilson group extended the theory to
143 on 21, 200 pstarpoenrgs fdieelsdcsr ibane da d misseitphaotdiv efo sry sstceumlps.t ingT wRoy dobtheerrg gwroavuen dpbarcekaektisn g( 6th) eaonredt icthael
52.ne generation of a molecular ft-pulse for total inversion of an electronic state
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w on to use this device to generate frequency-chirped laser pulses, which they
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excited I (9). In succeeding experiments over the next three years they ex­
2
tended their experiments to condensed phases (10), working with molecules as
complex as the green fluorescent protein (11). In still another landmark exper­
iment, the Wilson group used a genetic algorithm in a feedback loop to "teach"
the laser how to optimize the fluorescence of a laser dye in solution (12).
One of the great engineering accomplishments of the Wilson group
was to build an ultrahigh intensity laser, compact enough to fit on a single
table and simple enough to be operated by students (13). This instrument was
capable of generating intensities in excess of 1020 W/cm2, at which relativistic
effects become important. Using this device, Wilson was able to fulfill a lifelong
xii
In Laser Control and Manipulation of Molecules; Bandrauk, A., et al.;
ACS Symposium Series; American Chemical Society: Washington, DC, 2002.
dream of using ultra-short X-ray pulses to monitor atomic and molecular motion in
real time. In his final years, Wilson developed an ultra-fast X-ray laser that allowed
him to observe atomic motion (14) and a laser microscope that allowed him to
obtain very high-resolution images of living cells.
In 1998 Kent discovered that he had inoperable prostate cancer. Until
the very end of his life, Kent's curiosity about science was unabated. In his
final experimental endeavor, he worked with a team of biochemists and
physicians to develop new therapies for suppressing the cancer growth in his
own body, to which he finally succumbed in March 2000 (15). Shortly before
his death, a special issue of The Journal of Physical Chemistry A celebrating
Kent's work was published. In that issue, Kent wrote a poignant and in­
spirational account of his values and accomplishments (16).
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acs.001 experimental and theoretical methods of controlling matter with light, as
ubs.1.pr evident from an examination of the chapters in this volume. The book is
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12 | k-20 (nonperturbative) regimes and the manipulation of molecules in space. These
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er 0.1 The first section of this book deals with the coherent control of
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ptemdoi: molecular processes in weak fields. The opening chapter by Rabitz discusses
Se2 | the use of closed loop learning algorithms to control a variety of quantum and
43 on 1, 200 tnhoantl iwneaas r foirpstt icdaelm pohnesntoramteedn a bwy iWthoilusto knn'so wgrloeudpg ei no fc tohnet rHoallminiglt othnei anfl,u ao rsetrsacteengcye
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2.e of a dye. In th£ following chapter by Rice and co-workers, a multi-pulse
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Do vibrational, and rotational coherences, and in Jones' pump-dump control of
Rydberg wave packets. The use optimal control theory to design the "best"
laser pulse is generalized in the chapter by Cao et al. Chirped pulses, a central
idea in much of Wilson's wave packet experiments, are used by Yamashita et
al .to control chemical reactions and by Nakamura et al. to control non-adi-
abatic transitions. The impact of Wilson's pioneering work on vibrational
wave packets is evident in the paper by Ohmori et al. on the interaction of two-
wave packets in a complex and in the paper by Kobayashi et al., which deals
with real-time vibrational spectroscopy. Hoki and Fujimura discuss selective
preparation of pure enantiomers from an equal mixture of left-handed and
right-handed preoriented enantiomers, using a theory based on the density
xiii
In Laser Control and Manipulation of Molecules; Bandrauk, A., et al.;
ACS Symposium Series; American Chemical Society: Washington, DC, 2002.
matrix formalism with a dressed state representation. The photodissociation of
preoriented enantiomers has its antecedents in the early work of Busch and
Wilson on the photofragmentation of aligned molecules with linearly polarized
light. Finally, coherent phase control in the molecular analogue of Young's
two-slit experiment discussed by Gordon and co-workers and by Nakajima is
complementary to the time domain experiments pioneered by Wilson.
The second section of the book deals with intense field effects. The
leading chapters by Gerber and co-workers and by Levis et al. extend the usage
of learning algorithms to the strong field regime, where dressed state effects are
important. Structural deformation of molecules in intense fields is discussed in
the papers by Nguyen-Dang et al., by Yamanouchi, and by Kono and Koseki.
Intense field control of the interaction of electron and nuclear dynamics is treated
g
or in the chapter by Bandrauk et al.
acs.001 The final section of the book deals with the manipulation and
ubs.1.pr alignment of molecules with laser fields. Again, the dipole (or induced dipole)
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12 | k-20 developed by Cai and Friedrich, Sakai et al., and Mathur et al. is that the dipole
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ptemdoi: cally.
Se2 | At the close of his paper on "Controlling the Future of Matter" (17),
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52.ne into the future. Realistically, some of these dreams will come true, and others
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Do References
1. Wilson, K. R.; Kwei, G. H.; Norris, J. A.; Herm, R. R.; Birely, J. H.;
Herschbach, D. R. J. Chem. Phys. 1964, 41, 1154.
2. Busch, G. E.; Wilson, K. R. J. Chem. Phys. 1972, 56, 3626.
3. Goucher, C. L.; Teilhet, J. H.; Wilson, K. R.; Chow, T. J. Nature (London)
1976, 262, 130.
4. Gordon, R. J. private communication.
5. Krause, J. L.; Whitnell, R. M.; Wilson, K. R.; Yan, Y. J.; Mukamel, S. J.
Chem. Phys. 1993, 99, 6562.
xiv
In Laser Control and Manipulation of Molecules; Bandrauk, A., et al.;
ACS Symposium Series; American Chemical Society: Washington, DC, 2002.