Atomic, Molecular, Optical Physics Workshop: Final Report

Atomic, Molecular, and
Optical Physics
Workshop
Final Report
of the workshop held

September 21-24, 1997
in
Chantilly, Virginia
Sponsored by:
The Division of Chemical Sciences
Office of Basic Energy Sciences
Office of Energy Research
U.S. Department of Energy
Washington, D.C.
Table of Contents
Preface ...................................................................................................................................................................... iii
FORWARD ................................................................................................................................................................ v
Panel A: Interaction of Atoms and Molecules with Photons - Low Field ................................................................ 7
Panel B: Interactions of Atoms and Molecules with Photon - High Field ............................................................. 18
Panel C: Surface Interactions With Photons, Electrons, Ions, Atoms, and Molecules ............................................ 31
Panel D: Theory of Structure and Dynamics ........................................................................................................... 45
Panel E: Nano- and Mesoscopic Structures ............................................................................................................. 57
This document was produced under contract number DE-AC05-76OR00033 between the U.S. Department of Energy and Oak Ridge Associated Universities.
Table of Contents ii
PREFACE
This document contains the final reports from the five panels that comprised a Workshop held to explore future
directions, scientific impacts and technological connections of research in Atomic, Molecular and Optical Phys-
ics. This workshop was sponsored by the Department of Energy, Office of Basic Energy Sciences, Chemical
Sciences Division and was held at the Westfields International Conference Center in Chantilly, Virginia on
September 21-24, 1997. The workshop was chaired by Lloyd Armstrong, Jr., University of Southern California
and the five panels focused on the following topics:
Panel A: Interactions of Atoms and Molecules with Photons - Low Field

Daniel Kleppner (Massachusetts Institute of Technology), chair
Panel B: Interactions of Atoms and Molecules with Photons - High Field

Phil Bucksbaum (University of Michigan), chair
Panel C: Surface Interactions with Photons, Electrons, Ions, Atoms and Molecules
J. Wayne Rabalais (University of Houston), chair
Panel D: Theory of Structure and Dynamics

Chris Greene (University of Colorado), chair
Panel E: Nano- and Mesocopic Structures

Paul Alivisatos (Lawrence Berkeley National Laboratory), chair
The choice of focus areas reflects areas of significant interest to DOE/BES but is clearly not intended to span all
fields encompassed by the designation of atomic, molecular and optical physics, nor even all areas that would be
considered for review and funding under DOE’s AMOP program. In a similar vein, not all research that might be
suggested under these topics in this report would be appropriate for consideration by DOE’s AMOP program. The
workshop format included overview presentations from each of the panel chairs, followed by an intensive series
of panel discussion sessions held over a two-day period. The panels were comprised of scientists from the U. S.
and abroad, many of whom are not supported by DOE’s AMOP Program. This workshop was held in lieu of the
customary “Contractors Meeting” held annually for those scientists currently receiving support from the DOE
AMOP Program. The current DOE principal investigators attended the workshop, presented posters on their
current research, and engaged in discussions with the panel members. Thus, the reports contained in this docu-
ment reflect their active participation.
The workshop and this report are intended to stimulate and provoke the thinking of those interested in research in
AMOP. Anyone who would like to submit a proposal (Grant Application) for consideration and review can do so
at any time. This document as well as the annual Summaries of Research in the Chemical Sciences should be
useful reference materials to consider. Both are available either as hard copy or on our website at:
http://www.er.doe.gov/production/bes/chm/chmhome.html
iii Preface
The web version of the FY 1997 summaries of research can be easily searched by several criteria including both
scientific discipline and relevant technologies. Those considering submitting a proposal are encouraged to
prepare a brief preproposal prior to preparing and submitting a full proposal. Preproposals can be submitted and
discussed with staff in the Chemical Sciences Division. All relevant information, including phone numbers and e-
mail addresses, for all Division staff is available on our website and in the hardcopy version of the research
summaries. Preproposals should be addressed to the Division Director with copies to the appropriate Team
Leader and Program Manager. This will ensure full and timely consideration.
Patricia Dehmer
Associate Director of Energy Research for the
Office of Basic Energy Sciences
U. S. Department of Energy
Preface iv
FORWARD
Recent years have seen a virtual explosion of activity and advances in the fields of atomic, molecular and
optical physics. Development of new instrumentation and new experimental techniques has proceeded at an
unusually rapid rate, leading to discovery of many new phenomena and much improved characterization of
previously known phenomena. New theoretical approaches have enabled higher levels of understanding of
old problems, helped to provide explanations for newly discovered phenomena, and pointed out directions
for new exploration.
The Department of Energy Office of Basic Energy Sciences held a workshop on Atomic, Molecular, and
Optical (AMO) Physics on September 21-24, 1997, to review advances in selected areas of AMO physics
and to consider the impact of these changes on the closely allied fields of surface interactions and
nanostructures. Emphasis was placed on identifying future directions in all of these areas that are ripe for
exploitation. The papers that follow describe the conclusions of the AMO panels that reviewed high-field
and low-field regimes and the theory of structure and dynamics, as well as of the panels that looked at
surface interactions and nanostructures and their relations with AMO physics.
One of the central themes running through all of these reports is that many of these new developments enable
or should in the future enable a great expansion in our ability to control broad classes of physical phenomena.
Control of novel photon and atom states, of quantum dynamics of collisions and chemical bonds, of atoms on
surfaces, of chaotic behavior in nonseparable dynamical systems, of size, shape and properties of
nanostructures is increasingly possible. Control of these and other similar phenomena promises to open up
new and exciting fields of research, and to lead to the creation of powerful new experimental and theoretical
techniques for further exploration. Achieving this increased level of control and of the understanding of
these complex systems that this control implies could enable very significant advances in many important
areas of research. For example, understanding and control of the quantum dynamics of collisions and
chemical bonds is fundamental to the control and manipulation of chemical reactions.
Another important interconnecting theme is that of the continuing rapid evolution of probes, in particular
those that utilize light. Developments in lasers are leading rapidly to ever higher intensity, ultrafast pulses of
defined shape, shorter wavelength, greater stability and narrower lines. Third generation synchrotron light
sources are providing unprecedented resolution and sensitivity in the high-energy photon range. New
approaches to the production of photon beams having nonclassical properties have the potential to enable
spectroscopic sensitivity beyond the standard quantum limit. These and other new probes enable important
new experiments not only in AMO research, but in many other fields supported by the Office of Basic
Energy Sciences as well.
Several of the reports discuss recently created novel states of matter or matter and field. The ultimate utility
and application of these states is unknown, but many seem to have great potential for significant impact.
Bose Einstein condensates (BEC) are one of these. Already, researchers have been able to use BEC to create
“atom lasers” that display phase coherence between beams of atoms, raising the possibility of, for example,
v Forward
greatly increased capabilities in lithography. In other work, new states are being created in which matter and
field form systems with unusual properties. Among these at one end of the energy spectrum are entangled
states, created in micromaser cavities with a small number of photons and atoms; at the other end are states in
which external field strengths are comparable to the strength of the binding fields of the matter.
The papers on nanostructures and surface physics clearly show the very significant impact of existing AMO
technologies and theories on these fields. In addition, as workers in these fields look to the future, they find
numerous examples where developing AMO technologies should be of considerable importance in enabling
the fields to move ahead. This theme of AMO as an enabling science is found throughout all of the reports,
with each paper discussing areas outside of AMO where new technologies, instrumentation and theories being
developed to advance the physics of AMO might find applications. Numerous potential important enabling
applications of AMO technologies to other areas of interest to DOE and in particular BES are indicated
throughout the reports.
Since the emphasis of this meeting was on future directions, it is not surprising that there are many obstacles
to full realization of the potential of most of the areas of research discussed in these reports. In many, such as
the matter-field states in which external field and binding field strengths are comparable, there are serious
theoretical and computational difficulties that must be overcome in order to achieve understanding and
predictability. In others, the experimental techniques and instrumentation are just now reaching a level of
sophistication that enables “proof of principle” experiments, and considerable development will be required
before real investigations and exploitation of the field can occur.
Overall, the picture that emerged from this workshop was of fields that are extremely dynamic and exciting,
and critical to the development of many other fields of science. Important new phenomena, new theories,
new techniques, new understanding were to be found in all of the areas that were discussed. Development is
moving at an unprecedented rate in many of these areas. The challenges, the opportunities, and the
excitement were clearly described by the participants, and well captured by the contributions contained in
this volume.
Lloyd Armstrong, Jr., Chair
Forward vi
Atomic, Molecular, and Optical Physics Workshop Report
Panel A: Interaction of Atoms and Molecules

with Photons - Low Field
Chair:
Daniel Kleppner (Massachusetts Institute of Technology)
Panelists:
Uwe Becker (Fritz Haber Institut der MPG)
Nora Berrah (Western Michigan University)
William Cooke (College of William and Mary)
Robert Field (Massachusetts Institute of Technology)
Wallace Glab (Texas Tech University)
Wendell Hill (University of Maryland)
Eric Horsdal-Pedersen (Aarhus University)
Stephen Leone (University of Colorado, JILA)
Marsha Lester (University of Pennsylvania)
Stephen Lundeen (Colorado State University)
Cheuk-Yiu Ng (Iowa State University)
Erwin Poliakoff (Louisiana State University)
Stephen Pratt (Argonne National Laboratory)
William Stwalley (University of Connecticut)
Michael White (Brookhaven National Laboratory)
Outline Summary
1. Atomic and Molecular Manipulation and Control
2. Advanced Spectroscopies with New Light Sources
3. Quantum Dynamics of Interacting Systems
7 Panel A
Summary include studies of the basic physics of photon-

matter interactions, new investigations of the
Laser cooling and trapping techniques, synchrotron light
many-body problem, studies of the product
sources, advanced imaging methods and other
distributions from photo-initiated dissociation, and
innovations have opened frontiers for research in atomic
studies of the structure and dynamics of highly
and molecular physics. Opportunities encompass
charged ions. The studies are germane to
fundamental studies of structure and dynamics, the
problems ranging from the origin of radiation
development of knowledge and data for other disciplines
damage in cells to hot plasmas in stars. Ultrashort
and for industry, and the development of new
optical pulses can be tailored to study atomic and
technologies. We describe opportunities in three
molecular wavepacket dynamics. Tailored pulses
categories.
can be used to control molecular dynamics and the
products of chemical reactions, and can provide
1. Atomic and Molecular Manipulation and
new diagnostics for identifying atoms and
Control
molecules in hostile environments.
Light force techniques make it possible to cool
atoms to sub-microkelvin temperatures and to 3. Quantum Dynamics of Interacting Systems
study ultra cold collisions and new types of
Understanding chemical reactivity requires
molecular association. They have led to the
understanding the quantum dynamics of
creation of matter-wave optics and to Bose-
interacting systems. Scattering, including photo
Einstein condensation in an atomic gas. These
scattering and photo ejection, is the chief
developments have created opportunities for the
experimental tool for studying quantum dynamics.
study of Bose-Einstein condensates, the creation
The development of novel photon sources and
of new condensate systems, the development of
time- and position-sensitive imaging and co-
atom lasers, and new studies of fundamental
incidence methods opens the way to study the
symmetries. The cooling methods may be
mechanisms of energy exchange within a
extended to molecular systems to create new types
molecule. Reactions between simple systems can
of spectroscopy and studies of dynamical
be observed with a detail approaching complete
processes. Applications for the research exist in
quantum specification. There are opportunities for
areas ranging from biology to nanotechnology. In
extending these experiments to more complex
addition, new techniques to control and
systems and for developing visualization
manipulate ions, including ion storage rings, can
techniques for interpreting the voluminous data.
be employed to study molecular ionic systems that
In addition to elucidating the basic processes of
are important in the atmosphere and in low energy
chemical reactivity, such studies are important to
plasmas.
astrophysics, plasma physics and materials
science.
2. Advanced Spectroscopies with New Light
Sources
Two developments have stimulated the creation of
new spectroscopies and new methods for the
quantum control of atomic and molecular
processes. These are the creation of third
generation light sources and practical methods for
generating ultrashort optical pulses. Research
opportunities with third generation light sources
Panel A 8
1. ATOMIC AND MOLECULAR Within the past decade a revolution in atomic

MANIPULATION AND CONTROL control has been precipitated by the development
of light force techniques. The significance of this
1A. Introduction revolution was dramatized by the award of the
1997 Nobel Prize in physics for the development
The underlying goal for much of the research in
of atomic light force methods. The essence of the
atomic, molecular and optical physics (AMOP) is
advance is this: In the past, translational motion
to understand atomic, molecular and optical
had to be treated classically, and kinetic energy
processes with the ultimate clarity that quantum
was unquantized. Today, the ultimate limit in
mechanics allows. Achieving this goal
translational control has been achieved; it is now
experimentally requires tools for preparing atomic
possible to put atoms into a single translational
and molecular samples in specific states, and for
quantum state and to observe their behavior in
controlling their motion. Recently there has been
complete detail.
a revolution in techniques for controlling not only
the internal states of atoms but also their
The new methods employ laser techniques for
translational states, providing qualitatively new
slowing, cooling, and manipulating atoms, and
levels of control. These methods have opened
optical and magnetic traps for confining them. The
frontiers of research, generated strong links to
traps can hold large numbers of atoms at sub-
other areas of science, provided new opportunities
microkelvin temperatures. These methods make it
for metrology, and are starting to have an impact
possible to witness the photo-association of free
on technology.
atoms into unusual molecular states; to study
ultracold collisions in which the dynamics can be
1B. Light Forces—Manipulating Matter by
controlled by electric, magnetic, and laser fields;
Light
to observe phenomena such as Bloch
Motion is an impediment to the study of atomic, oscillations—collective oscillations in a periodic
molecular and ionic structure and dynamics. Motion potential—and to realize the quantum kicked
blurs spectral lines and obscures structure. It limits rotor—a paradigm in the study of nonlinear
observation time, degrades the control of collision dynamics.
kinetics and introduces undesirable complexities
into observations. For this reason, experimental The observation of Bose-Einstein condensation
progress in AMOP has often been propelled by (BEC) in an atomic gas is the most dramatic
progress in controlling atomic and molecular achievement of the light-force techniques. The
motion. Early efforts to control motion employed clarity with which the Bose condensates can be
effusive atomic beams and mechanical velocity observed and the exquisite control by which they
selectors. Supersonic beams were developed that can be manipulated, as well as the novelty of the
further reduced thermal effects in atoms and phenomena, have generated a new field of study
molecules, creating a new arena for studying atomic that has attracted enormous interest in AMOP by
and molecular dynamics and also the science of condensed matter scientists, chemists, and others.
clusters, including the discovery of the fullerenes— The phase transition, the collective motions and
honored by the 1996 Nobel Prize in chemistry. In a transport and relaxation processes of the
parallel development, the creation of ion traps led to condensate, have all been studied. A study of the
essentially total control of ionic motion and opened phase coherence of the condensate resulted in the
the way to advances in spectroscopy, collision creation of an atom laser.
dynamics, plasma processes, and metrology.
9 Panel A
Closely related to these developments is the • Developing light force and trapping
creation of the field of matter wave optics. techniques for molecules. Trapped molecule
Several types of atom-wave interferometers have methods would provide new ways to study
been demonstrated and optical elements such as molecular structure, chemical reactions, and
mirrors, lenses, gratings, beam splitters, and interatomic and inter- molecular interactions
hollow guiding fibers, have been developed. The that may ultimately yield BEC of state-
interferometers have been employed to measure selected molecules, and molecule lasers.
atomic and molecular properties, to investigate the
• Applying low temperature molecular
decoherence in quantum systems, to measure
spectroscopy to new studies in molecular
fundamental constants, and to create ultrasensitive
and biological physics. For example, low
accelerometers. Atom-optics methods are being
frequency torsional modes in biopolymers
applied to new types of lithography, and have
can be cooled to ultralow temperatures,
already been used to create length standards for
perhaps yielding new insights into protein
scanning microscopies.
folding.
Scientific opportunities and applications include: • Developing light force techniques for other
applications. A notable example is the early
• Addressing fundamental questions on BEC
development of optical tweezers, which are
including transport, condensate dynamics,
used in polymer studies, biology, and other
coherent collisions, compound condensates,
applications. These tweezers are able for the
and interactions with light. The condensates
first time to directly manipulate matter
may make possible new studies in quantum
within a living cell and to stretch and even
entanglement.
break an individual polymer or DNA
• Exploring new condensates and developing molecule.
methods for increasing the size of BEC
condensates. Such methods could be 1C. Fundamental Studies
applied to much more intense atom lasers.
Closely related in spirit to the study of light forces
• Developing the atom laser as a scientific is a body of research in AMOP centered on the
tool, and exploring its applications to nano- study of fundamental symmetries and other
technology. fundamental phenomena. The goal is to deepen
our basic understanding of physics, but in
• Extending photoassociative spectroscopy of
accomplishing this the research has often pushed
submillikelvin atoms to study long range
forward the frontiers of experimental control, and
molecular states of other atoms (for instance
of metrology.
the hyperfine-free alkaline earths, and
metastable rare gases) and also to study
Among the most precise studies in AMOP are a
atom-molecule and molecule-molecule
series of experiments on parity
photoassociation. Such studies provide
nonconservation (PNC) effects in atoms. These
parameters such as scattering lengths,
have contributed new information to the Standard
dissociation energies, and spin-flip cross
Model and they have led to the discovery of a new
sections. These are critical for
type of nuclear current—the anapole moment.
understanding very low temperature
Laser power buildup cavities for these experiments
dynamics and BEC.
have advanced laser mirror technology in
developments that led to cavity ring-down
Panel A 10
spectroscopy and that have been taken up by Opportunities include:

industry. New opportunities for this line of research
• Exploiting atom trapping and cooling
have been opened by advances in light force
techniques for tests of PNC interactions and
techniques and in the trapping of radioactive atoms.
other fundamental tests.
Atomic studies of the fundamental symmetries • Developing new methods for the
probe the basic forces that govern the interactions spectroscopy of short lived atomic species.
in nature and search for new types of fundamental
• Applying optical methods to polarize atomic
particles. Such investigations range from the
nuclei to create polarized beams and targets
extremely high precision spectroscopy of neutral
for nuclear and particle physics. Recent
and ionic atoms and molecules to the creation of
studies on the spin structure of the neutron
exotic atoms and antimatter. These experiments
through electron scattering from polarized
generally push the frontiers of experimental
helium-3 nuclei provide a notable example.
techniques and are a source of new technology for
other sciences and for applications. Studies of • Finding more efficient methods for
QED in atoms are spurring methods to measure polarizing rare gas nuclei. The production
optical frequencies that have potential applications of these nuclei have led to the development
in communication and control. Searches for of an important new medical diagnostic
electric dipole moments of fundamental particles technology—magnetic resonance imaging
have led to the development of magnetometers and with polarized rare gases—with greatly
improved methods for measuring and controlling enhanced sensitivity and resolution.
electric and magnetic fields. Investigations of
• Investigating the behavior of atomic systems
antimatter atoms have been instrumental in the
in nonclassical light fields to understand
development of ion trapping.
altered lineshapes and decay rates, nonlinear
mixing, and new types of lasing behavior.
In a different domain, new types of light have been
created with unique quantum properties. These • Studying entangled atomic states using the
include squeezed light, correlated photon beams, methods of cavity quantum electrodynamics
and quantum solitons. A common feature is that to obtain new techniques with potential
the fluctuations lie below the so-called standard applications in the general area of quantum
quantum limit associated with the vacuum state of computing and quantum cryptography.
the electromagnetic field. In addition to their
fundamental interest, such nonclassical light 1D. Molecular Control
sources may have spectroscopic applications.
Molecular spectra can be vastly simplified, and
Nonclassical light has enhanced spectroscopic
new types of molecular states accessed by
sensitivity beyond the standard quantum limit. If
methods such as multiple optical-optical and
this technique can be made practical, it offers
optical-RF resonance techniques, polarization
opportunities for advances in ultrasensitive
labeling spectroscopy, multiphoton ionization,
detection and it may increase the sensitivity of
laser-induced fluorescence, and stimulated Raman
gravity wave detectors such as LIGO. Closely
adiabatic rapid passage. Beyond these, molecular
related to these developments are the creation of
spectra can be greatly simplified by cooling the
new types of photon and atomic states using the
molecules. Spectroscopy has been carried out to
methods of cavity quantum electrodynamics.
temperatures as low as 1K using seeded
11 Panel A
supersonic molecular beams or solid rare gas Ions that can be conveniently studied include O2+
matrices. More recently, temperatures as low as and N2+, which are relevant to the physics and
0.4K have been achieved, for example by studying chemistry of the Earth’s atmospheres (N2+ is also
species in helium-4 clusters. important on Mars), and H2+, which is important
to the chemistry of the interstellar space.
Opportunities include:
• Extending methods for manipulating and
controlling the vibrational populations of • Producing state-selected molecular ions
molecules to their rotational and electronic directly from ultracold atoms by
states. Such control would provide new photoassociative ionization.
pathways to the studies of collision
• Manipulating ions in storage rings by laser
dynamics and chemical reactions.
light, providing a new control over reaction
• Developing methods for cooling and dynamics.
trapping molecules. These methods could
provide new levels of resolution and vastly
simplify molecular spectroscopy and 2. ADVANCED SPECTROSCOPIES
provide a new arena for the study of WITH NEW LIGHT SOURCES
collisions and reactions.
Two developments are stimulating the creation of
• Controlling detrimental loss processes in
new forms of spectroscopy and new methods for
traps by controlling collision dynamics.
the quantum control of atomic and molecular
processes. These are the creation of third
1E. The Control of Ions
generation light sources to extend the power and
Ions can be manipulated and controlled with traps resolution of spectroscopy in the UV and short x-
for collision studies, ultrahigh precision ray regimes, and the development of practical
spectroscopy, studies of ion crystals and strongly methods for generating tailored ultrashort optical
coupled plasmas, and for applications to quantum pulses. Additional opportunities due to free
logic gates and quantum computing. Ion trap electron laser light sources are discussed by the
methods have also been used to observe Panel on Interactions of Atoms and Molecules
vibrational relaxation of molecular ions, and with Photons: High Energy.
dissociative and dielectronic recombination at very
low energies. Because dissociative recombination 2A. Third Generation Synchrotron Sources
can play an essential role in determining the
The photon beams now available from third
distributions of free radicals in low energy
generation synchrotron light sources developed at
plasmas, this research can have important
Berkeley (ALS) and Argonne (APS) offer new
applications in materials processing and etching.
opportunities to study radiation-matter interactions
that require very high energies, spatial resolution,
In heavy ion storage rings molecular ions can be
spectral resolution, or polarization. The low
stored at MeV energies for several seconds,
emittance of third generation storage rings makes
allowing them to cool rotationally and
it possible to employ undulator or wiggler devices
vibrationally. Reaction products from dissociative
that can provide radiation into the hard x-ray
recombination and branching ratios for electronic
region with unprecedented intensities and spatial
states can be identified using imaging techniques.
collimation. In atomic and molecular physics,
Panel A 12
these developments open new avenues for • Identifying nascent product distributions of
studying multi-electron excitation and inner-shell atomic and molecular fragments, resulting
photoionization. For example, high brightness from reactive scattering, electron
undulators in the UV can be used for “universal” attachment, and photo-initiated dissociation,
detection of neutral product species via one- ionization, detachment and desorption.
photon ionization with sensitivities rivaling
• Studying endothermic reactions with low cross
conventional electron-impact sources, but without
sections and other processes that result in
the associated difficulties of unwanted dissociative
difficult to detect, low-yield neutral products.
ionization and a hot source region.
• Combining ultra-high resolution capabilities
Complex atomic, molecular and ionic processes can of small aperture monochromators with the
be studied by combining third generation beams from undulators to produce narrow-
synchrotron radiation with high resolution detection band UV and soft x-ray radiation to study
techniques that simultaneously detect and analyze photoionization of atoms, molecules, clusters
every possible outcome channel. These methods also and ions, possibly with complete quantum
make it possible to image the fragments emitted in state specification and kinematic imaging.
photoprocesses-ions, electrons, neutral, and
• Employing high resolution photoelectron-
photons—and to detect their coincidences. Because
photoion coincidence techniques, to prepare
polyatomic molecular species can exit in different
atomic and molecular ions with specified
chemical isomers with distinctly different chemical
quantum states for scattering and
properties and energetics, the detailed understanding
spectroscopic experiments. Neutral atoms
of photodissociation, electron dissociation, and
(O, N, and C, etc.) and radicals (OH, CN,
reaction processes is possible only with such an
CH3, and C2H, etc.) can be prepared by
identification of nascent product chemical structures.
photodissociation of appropriate precursor
molecules using the high flux VUV
synchrotron radiation.
• Testing the basic assumptions that have been
• Employing light from third generation
used traditionally to interpret photon-matter
synchrotron sources to create new species;
interactions; for instance, the independent
for example, “hollow” atoms in which the
particle, impulse, and dipole
core electrons are simultaneously excited to
approximations.
high-lying states. Such atoms provide a new
• Conducting quantum mechanically complete arena for observing many-electron systems
experiments that determine the alignment and testing theories of highly correlated
and orientation parameters for atomic and electron motion.
molecular targets, using circularly or
• Studying the structure and dynamics of
elliptically polarized light from helical
highly charged ions by combining radiation
undulators.
from third generation synchrotron sources
• Advancing our understanding of the many- with targets of highly charged ions. These
body problem, one of the central problems studies will provide precision data on ionic
in atomic, nuclear and condensed matter structure and electron-correlation effects,
physics, through negative ion spectroscopy, benchmarks for theoretical studies of
as suggested by theoretical studies. multielectron interactions and data for
plasma modeling and ion-beam lithography.
13 Panel A
2A-2. Related Science and Applications between collisions in a dense gas, make possible
new ways for manipulating and interrogating the
X-ray absorption spectroscopy with third-
internal dynamics of molecules. Several groups
generation synchrotrons can provide element-
have employed shaped optical pulses to generate
specific and chemical state-specific detection of
atomic and molecular wave-packets. These
trace contaminants in biological materials, soils
techniques may be able to provide such precise
and groundwater. The spectroscopy can be
control over internal interactions that the final
applied to understand radiation damage in
products of chemical reactions can be selected by
complex molecules such as DNA, for the damage
suitably arranging a sequence of shaped pulses. In
originates in core excitations that are
related control experiments, interference between
fundamentally atomic processes. A real
two optical excitation pathways has been used to
understanding of radiation damage is possible only
control the branching ratios between
through studies of the complex decay processes in
photoionization and photodissociation in hydrogen
isolated atoms and simple molecules.
iodide, and interference between one- and two-
photon excitations has been used to control the
Studies in the structure and dynamics of highly
photoionization angular distribution and the
charged ions is vital for understanding hot plasmas
direction of the flow of current in solid state
in stars, in fusion reactors, and also in x-ray lasers.
devices.
The energetic, spectroscopic and dynamical

In a somewhat different context, new types of
information from molecular studies with third
wave-packets have been created in Rydberg atoms
generation synchrotron sources can be important
by employing combinations of laser light,
to combustion chemistry, plasma science, and
microwave fields and time-varying electric and
environmental and atmospheric chemistry. For
magnetic fields. The electronic current can be
instance, cation spectroscopic studies can yield
stationary and highly localized, as in a “circular”
invaluable spectroscopic and geometric
Rydberg state, and the electron can even be
information on the neutral ground state.
localized in a stationary wave packet, as in a
Rotationally resolved photoionization and
coherent elliptic state. Such atomic states have
photoelectron spectroscopic studies of reactive
already been employed in studies of quantum
intermediates, such as CH, CH2, NH, NH2, HCO,
optics, high resolution spectroscopy, and
CH3O, and C2H, are important in combustion,
scattering. They have also been employed to study
plasmas, and atmospheric chemistry.
the physics of the semiclassical regime, a problem
which is of deep interest in molecular physics
2B. Ultrafast Lasers and Wave Packet
where semiclassical approximations are often
Dynamics
appropriate.
Sub-picosecond laser systems have become
practical laboratory instruments. Their Opportunities include:
development has generated an explosion of new
• Extending these tailored pulse techniques by
research on the control of elementary
combining several shaped, multicolor
photochemical and photophysical processes by
pulses.
using sequences of ultrafast pulses with precisely
shaped spectral and temporal profiles. The pulses, • Investigating wave packet dynamics by
which are shorter than the period of typical experimentally executing algorithms created
molecular vibrations and rotations, or the time with optimal control theory.
Panel A 14
• Employing short-pulsed, multi-step events can be observed, the variety of systems that
excitation to create a new collision-free tool have become accessible, and the range in
for identifying atoms or molecules, even in dynamical variables with which they can be
hostile environments such as plasmas or studied, have expanded enormously.
flames.
3A. Complete Scattering Experiments
• Investigating the possibility of preparing
species in wave packets to control the As its name suggests, a complete scattering
dynamics of interactions, i.e., of controlling experiment provides all the information about a
molecular reactions. scattering event that quantum dynamics allows us to
know. Instead of an average transition rate, one talks
• Developing new methods for creating and
of the quantum mechanical amplitude for passing
studying the physics of localized atomic
from one quantum state of the collision partners to
states, and for applying these states to
another. Such an experiment requires precise
scattering problems and studies of
measurement and control of the incoming and
semiclassical physics.
outgoing momenta of the scattering partners, and also
their polarization, alignment, and orientation. With
3. QUANTUM DYNAMICS OF such measurements one can obtain both the
INTERACTING SYSTEMS magnitudes and phases of the scattering amplitudes
for targets and projectiles such as atoms, ions,
Understanding the fundamentals of chemical
photons, electrons, and simple molecules.
reactivity demands understanding the quantum
dynamics of interacting systems. Such an
Although a complete scattering experiment
understanding would contribute not only to
remains an ideal, even in cases where it cannot be
fundamental chemical dynamics but to essentially
fully achieved the concept can nevertheless be
every area of chemistry and related disciplines
employed to distinguish the important degrees of
such as atmospheric science, combustion,
freedom in complex systems. Techniques
astrophysics, plasmas, and materials science. The
employed in complete scattering experiments
quantum dynamics of interacting systems holds
include polarized beams and targets, spin resolved
the key to controlling and manipulating reactions.
electron detection, and laser-selected molecular
It is difficult to overestimate the power that such
state preparation and detection. The research has
control would provide.
been propelled by the recent development of time-
and position-sensitive imaging methods that
Just as spectroscopy is the chief experimental tool
provide what are known as 4 π detection, detectors
for studying the structure of atomic and molecular
in which every scattering partner in a collision is
systems, scattering—including photon scattering
observed and fully measured. Their high
and half-scattering (photo ejection processes)—is
collection efficiency can make coincidence
the primary experimental tool for studying
experiments feasible. These detectors have been
dynamics at the quantum level. Spectroscopy is
applied to photo fragmentation (“half collisions”)
also an important tool for studying dynamical
and particle-induced reactions involving atoms
processes such as photoassociation and
and simple molecules, for instance, to the
photoionization, and it can provide essential
photodissociation of molecular hydrogen. Other
diagnostics for scattering experiments. And just as
advances include photofragment imaging and
spectroscopy has undergone a revolution, so too
multiphoton ionization of neutral products.
has scattering, for the clarity with which scattering
15 Panel A
Scientific opportunities and applications include: In some cases, a subset of the coordinates can be
employed in a reduced dimension visualization
• Extending complete scattering studies to
scheme. An example is the femto-chemists’
more complex systems such as polyatomic
picture of a wave packet moving on a potential
molecules, radicals and ions. These
surface. This sort of picture aids in the design of
experiments, with their full specification of
experiments and in the identification of physically
initial and final quantum states, can reveal
plausible coupling mechanisms. Non-separable,
the mechanisms for energy exchange
nonperturbative systems are often separable for a
between electronic, vibrational, rotational
short time after a short pulse preparation of a
and translational degrees of freedom. Such
localized excitation. In some cases the first stages
experiments have been carried out on
of an interaction can be separated into active and
reactions between atoms and simple
passive degrees of freedom. In such cases the
diatomic molecules, for instance deuterium
reduced dimension representation of the evolving
and molecular hydrogen, and on the
system can show the evolution within a system of
competition between autoionization and
a well understood subsystem that has been
predissociation in highly excited small
previously studied in isolation.
molecules.
• Extending these techniques to clusters. In high resolution frequency domain spectroscopy,

Collision experiments with complete a spectrum can consist of entangled patterns arising
specificity are not yet possible due to the from different values of a conserved observable.
high density of final quantum states in a By comparing different spectra in which the
cluster, but much can be learned from entangled patterns appear with different relative
collisions with electrons, atoms, and ions, in weights, the dynamically independent pieces of the
experiments employing mass spectrometry spectrum may be separated. For example, data on
and time-of-flight energy analysis. Such threshold double ionization of helium presented in
experiments can reveal, for instance, the terms of the momentum vector of the relative
mass distribution of photofragments, motion of the two electrons revealed a simple
information that is essential for dynamical pattern that was essentially invisible
understanding cluster-cluster and cluster- when presented in terms of the conventional
surface interactions. laboratory frame momentum vectors.
3B. Visualization of Quantum States and Scientific opportunities include:

Dynamics
• Developing reduced-dimension visualization
A serious problem in interpreting data from methods for optimally representing a
complete scattering experiments and comparing complex system in terms of weakly
the results with theory is that even relatively interacting subsystems. It is essential to find
simple systems require complex multidimensional when such representation are appropriate,
representations. It is essential to find methods to for they can introduce major simplifications.
view this information in ways that yield insights
• Developing pattern recognition techniques
into the essential degrees of freedom, time scales,
that can recognize an unspecified and
and the various competing mechanisms. The
unknown patterns in a large, high quality
particular way in which the results are presented is
data set.
crucial in determining whether or not the essential
processes can even be recognized.
Panel A 16
• Developing methods that reveal correlations important. In addition, a quantitative

in the internal relative momenta in multi- understanding of binary ion-ion and photon-ion
dimensional velocity space. Such methods interactions is needed for numerous plasma
are needed for understanding experiments in diagnostic techniques.
which the momentum vectors of all final
reaction products are determined c. Understanding theoretically and experimentally
individually event by event. the transition of scattering characteristics as a
function of collision energy where the collision
• Investigating the use of collective, Jacobi, or
evolves from molecular characteristics (e.g.,
other appropriate internal momentum
molecular wave functions, potential curves, etc.)
coordinates, to reveal patterns that reveal the
to that of proceeding via atomic characteristics
roles of two-body or collective interactions.
(e.g., impulsive interactions, atomic states, etc.) is
important to basic physics and for applications.
3C. Cross-Disciplinary Connections
Advancing our understanding of the quantum

mechanics of interacting systems has broad
ramifications and the impact of the research is not
easily summarized. Nevertheless, it is of value to
note some of these.
a. Comprehensive sets of dynamical parameters of

atomic collision and half-collision processes
provide information needed to derive partial cross-
sections, angular distributions, and spin
parameters of a large variety of atoms and
molecules that are important in astrophysics,
plasma physics, and materials science.
b. The interaction of highly charged atomic ions

with atomic, molecular, electronic and ionic
targets occupies a special place in the study of
quantum dynamics of interacting systems because
of their importance in high temperature plasmas.
Such plasmas occur in such fusion plasma devices
and laser-produced plasmas in both ICF and x-ray
laser work. Opacities, charge-state equilibria and
equations of state of such plasmas, as well as
energy flow rates through short lived plasmas, can
be calculated if relevant recombination, electron
transfer, and ionization rates are known.
Interactions involving ions in states appropriate to
plasmas with electronic temperatures of a few
hundred eV to over 100 keV are particularly
17 Panel A
Panel B: Interactions of Atoms and Molecules
with Photon - High Field
Chair:
Phil Bucksbaum (University of Michigan)
Panelists:
Louis Dimauro (Brookhaven National Laboratory)
Richard Freeman (Lawrence Livermore National Laboratory)
Anthony Johnson (New Jersey Institute of Technology)
Robert Jones (University of Virginia)
Jeffrey Kimble (California Institute of Technology)
Wolfgang Sandner (Max Born Institute/Berlin)
Carlos Stroud (University of Rochester)
I. Executive Summary dynamics of atoms and molecules, since the time for
scattering between a relativistic particle and an atom is
In “high-field” interactions applied field energies equal on this timescale.
or exceed the energy density of matter, so that the field
controls the shape and dynamics of atoms, molecules, High-field laser-atom interactions have recently
or other material systems. Using modern tools of high- yielded intense coherent radiation at wavelengths as
field and ultrafast physics, one no longer merely short as 27 Angstroms, which is short enough for
observes nature, but can reshape and redirect atoms, biological imaging of femtosecond dynamics in the
molecules, particles, or radiation. This new drive “water window.” These light sources are major
towards harnessing quantum dynamics is enormously complements to synchrotron sources, delivering
important to future developments in fundamental shorter pulses and greater control over coherence, on
physics and applied energy science. platforms that can be as small as a single table top.
Still shorter wavelength sources have been
This document explores some of the ramifications and demonstrated by scattering high intensity laser pulses
future fertile directions in this field. We divide the from relativistic electon beams, or gating synchrotron
paper into three “grand visions,” which are broad radiation using laser-driven material switches. These
interconnected areas of AMO science. We begin with advances bring kilovolt, megavolt, or even gigavolt
an executive summary: photons into reach for laser-based time-resolved
science of materials, chemistry, atomic physics, and
I.A. Frontiers of Time, Intensity, and possibly even particle physics.
Wavelength
We now control not only the wavelength, intensity, and
The first vision is the technical frontier of high fields
duration of intense fields, but also their detailed shape,
and ultrafast optical pulses. The lasers that produce
often down to the single-cycle limit. Pulse shaping is
the intense fields are themselves designed and built
a major enabling element of the second “grand vision,”
using the principles of this new science of
which we call:
manipulating matter.
I.B. Harnessing Quantum Dynamics

The past decade has seen a thousand-fold
improvement in the peak power of solid-state lasers, Quantum dynamics in an atom or a molecular bond
and the future holds challenges for scaling to higher involves atomic-size fields (volts/angstrom), times
power with both solid-state and proposed free-electron (picoseconds and below), and frequencies (terahertz
sources. This progress will enable a wide range of [1012 hertz] to exahertz [1018 hertz]). Our challenge
science: new methods for more efficient inertial is to achieve the technical ability to manipulate these
confinement fusion; compact laser-driven electron states, the knowledge of how to design new
accelerators; sources of femtosecond (10-15 seconds) “sculpted” states, and the wisdom of which new states
gamma radiation are some of the prospects. will best accomplish our goals of new insight and
useful applications.
Pulses will also become shorter, opening new areas of
scientific inquiry previously undreamed. Femtosecond Some of the frontier areas are fundamental, such as
pulses, which were frontier research projects ten years nonclassical properties of entangled states of the fields
ago, have been commercialized. Attosecond (10-18 and matter, or the control of chaotic behavior in
seconds) pulses are actively investigated, and their nonseparable dynamical systems. Others challenges
control and measurement is a major challenge. lie at the interface between basic knowledge and
Attosecond science will certainly center on the technology. For example, adaptive feedback could
19 Panel B
permit the newly formed quantum state to “teach” the The high intensity can be converted to high pressure in
external field how to alter its own shape. Sometimes solid-density targets, to produce conditions usually
this adaptive feedback is built into the quantum only observed in astrophysical objects or in
system, such as in relativistic plasma channeling or thermonuclear reactions. Possible applications are
electromagnetically-induced transparency. An even advanced x-ray sources, or creating initial conditions
more exciting vision for the future, however, is using for inertial confinement fusion.
fast computers and pulse shapers to alter intense fields
according to instructions given by the quantum state, New nonlinear effects occur when the work done on
in order to optimize the state for a particular purpose. an electron during one optical cycle exceeds the
Some of the possible challenging applications of field- electron rest mass (intensities exceeding one exawatt
sculpted matter are: per square centimeter). Optical propagation in
plasmas becomes dominated by the oscillating
• Bond-selective chemistry, in which a strong relativistic mass of the electrons. This coherent
programmed optical field creates a rovibrational motion creates extreme charge-density gradients in
or electronic wavepacket in a molecule, which plasmas, which can support fields of gigavolts per
induces a specific change in unimolecular centimeter. Nonlinear Compton scattering in this
chemistry; regime creates harmonics from the relativistic motion
of the electrons. Photoionization into such a
• Coherent collisions, where target or projectile
relativistic continuum has not been studied.
are prepared in wavepacket states to control
specific inelastic channels or select impact
At still higher fields, near the material limits for focused
parameters;
laser light in the laboratory but well beyond what has
• Quantum encoding, the encrypting of been demonstrated, electrons can be driven so violently
information into the amplitude and phase of that they emit electron-positron pairs through the
nonstationary states. A strong programmed field process of coherent nonlinear Compton scattering.
pulse can key the return of the information as a
quantum echo; Still higher intensities can be achieved in the center of
momentum frame by back-scattering laser light from a
• Altering bulk properties, to control Bragg
relativistic electron beam, such as the SLAC linac. In
scattering, switch crystal domains, or move
the CM frame of the backscattered gamma ray and a
charge in solids and plasmas;
counter-propagating laser beam, the field can rise to
• Energy channeling, the controlled transport and above ten million gigavolts per centimeter, at which
deposition of laser energy into media which are field the vacuum itself becomes unstable, decaying into
generally opaque to weak or unshaped optical an electron-positron plasma. Positrons from this
pulses. The mechanisms for energy channeling mechanism were recently observed at SLAC (D.L.
change dramatically when the intensity is very Burke, et al., PRL 79, 1626 (1997)). This was the first
high, and this leads us to the third grand vision: example of coherent sparking of the vacuum.
I.C. Matter in extreme conditions I.D. Reading List and References.

At the extreme limit of high intensity in a laser focus, This document was prepared at an intense two-day
the electric fields can exceed trillions of volts per workshop in Chantilly, VA. As such, it can only
centimeter; magnetic fields can approach gigagauss; provide qualitative and general information on the
pressures aproach a gigabar. Physics in this subject. There are, however, several important
environment is largely unexplored. focused conferences in this field where current work
Panel B 20
and future prospects are discussed in detail, and the II. Opportunities in Intense-Field AMO
reader may find additional details and documentation Physics
in their proceedings:
Under high-field conditions, systems are driven by
• Super-intense laser-atom physics (SILAP), most
external fields to evolve more rapidly than their
current meeting was in Russia in August, 1996.
natural dynamical time scale. In quantum mechanical
Proceedings edited by H.G. Muller and M.
language appropriate to atomic and molecular physics,
Federov.
we state this as follows: A dynamical system u(t)
• OSA Topical Meeting on Short Wavelengths and evolves according to a Hamiltonian
High Fields, most current meeting in Santa Fe in
(H + H’(t))u(t) = i hbar [d(u(t))]/dt
March, 1997, Proceedings edited by L.
DiMauro and M. Murnane, not yet published. Where H is the Hamiltonian of the system excluding
The previous meeting in this series is available: the field interaction, and H’ is the interaction
“High Field Interactions and Short Wavelength hamiltonian. When H’ evolves on a time scale faster
Generation, AUG 1994, St. Malo, France, than the natural dynamical timescale of u(t), and/or has
Paperback, ISBN 1-55752-361-4, Available a magnitude comparable to or greater than H, then we
from the Optical Society of America. are in the high field regime. Typically, traditional
approaches to dynamics in quantum systems such as
• International Conference on Multiphoton
perturbation theory do not reveal the physics of such
Physics (ICOMP), most recent meeting in
systems.
Munich in October, 1996, Proceedings edited by
P. Lambropoulos.
Instead, the field and the matter form together a new
• 10th ICFA Beam Dynamics Panel Workshop; system which generally has altogether new properties.
4th Generation Light Sources, Grenoble, France Some of these properties will be critical for advances
Jan 22-25, 1996, editor J.L. Laclare. The report in energy science and technology, and these areas form
is available on the web: http://www.esrf.fr/ the grand challenges of this field.
conferences/conclusions/webconc.htm
II. A. Frontiers of Time, Intensity, and Wavelength
• Proceedings of the Seventh Advanced
Accelerator Concepts Workshop, Lake Tahoe, In this section we will discuss the physical frontiers in
CA, Oct., 1996, W. Chattopadhyay, J. materials, concepts, and optics at high fields, short
McCullough and P. Dahl, Editors, AIP, wavelengths, and short pulsewidths. The generation of
conference Proceedings 398 (American Institute ultrahigh fields continues to go hand in hand with the
of Physics, New York, 1997). generation of ultrashort pulses. The current state-of-
the-art in solid state lasers operating at wavelengths
• OSA Topical Meeting on Ultrafast Processes,
near 1000-nm have yielded pulses as short as 5 fs and
ULTRAFAST PHENOMENA, MAY 1996, San
intensities 1022 W/cm2. Currently, the intensity is
Diego, CA, ISBN 1-55752-441-6, available
limited primarily by the saturation intensity and
from the Optical Society of America.
geometry of the gain medium. The pulse duration is
• University of California at Berkeley Fast Ignitor close to the limit of the uncertainty principle with a 5
Physics Workshop, March 1997. Unpublished fs pulse at 1000 nm consisting of approximately 3
proceedings might be available from Dick Lee at optical cycles. If future technology could scale the
Lawrence Livermore National Lab. current 1 cm diameter solid state lasers to 1 m, then
intensities of 1026 W/cm2 and concomitant field
strengths of 1014 V/cm should be achievable.
21 Panel B
If these technological extremes (e.g., scaling the size II.A.2. Frontiers and Physical Limits of Solid
of gain medium) are achieved, where will the next State Lasers
advances come from? Laboratory intensities even
II.A.2.1 Laser-Based Mechanisms
above the solid state laser intensity limit of 1026 W/
cm2 might be reached by future Free-Electron Laser Electromagnetic fields are proportional to the square
sources. Alternatively, the problem of scaling can be root of the intensity in the focus of a coherent source.
sidestepped altogether by the use of relativistic targets, They are thus limited by the laser power (W) and the
which see the optical fields upshifted by a factor of focal size, which, in turn, depends on the wavelength
gamma. Although many processes cannot be studied through diffraction limits.
this way, relativistic electron and ion beams have
already been used to study special regimes in The laser power is theoretically limited by the saturation
high-intensity physics. fluence and the pulse length, both being ultimately
determined by material constants (cross sections and
In the area of ultrashort pulse generation, if we push bandwidth). In practice, additional properties like
the limits of high harmonic generation for example to spectral absorption, thermal conductivity, temperature-
the 1000th harmonic of a solid state laser to 10- and intensity-dependent index of refraction play a
Angstroms (~ 1 keV) and assumed we could phase crucial role, limiting the number of suitable high-
match this process then we would predict pulses of intensity laser materials to a handful of host materials,
order 10 as (attoseconds). We have always inferred glasses and crystals. They typically contain a small
that the timescale for electron orbits was on this order, concentration of ions with mostly vibrationally
but we may soon have the capability to directly broadened transitions in the near-infrared as active
measure it and predict new phenomena! components (solid state high power lasers).
High intensity ultrashort pulses are necessary to Extensive and systematic screening of possible new
generate coherent sources of x-rays. Recent work by materials over the last 5 to 10 years has yielded limited
two groups have demonstrated coherent high harmonic success in pushing the theoretical physical limits of
generation within the water transparency window of intensity and field strength. We note that at least the
critical importance for imaging biological processes. bandwidth of the best known materials (like
Among the many uses for this unique source of light Ti:sapphire) is already within a substantial fraction of
would be the following: x-ray holography for medical the photon energy, which is the ultimate physical limit,
imaging applications; table-top sources could and can only be substantially improved by going to
complement synchrotrons as the sources of light much shorter emission wavelengths.
necessary for x-ray lithography to push the limits
below 0.1-micron line rules. Even shorter wavelength The physical limits of laser field strength and intensity
coherent radiation is proposed using high energy free- were increased by more than four orders of magnitude
electron lasers. One such proposal would use the through introduction of chirped pulse amplification
SLAC linac to generate 1-Angstrom level or ~ 10 keV (CPA). We assume that this technique and the
photons. Beyond this, ultrashort pulses of gamma properties of presently known materials will
rays can be produced by backscattering intense lasers essentially determine the maximum achievable
from relativistic electron beams. Photon energies up intensities and field strengths for solid state high
to 29 GeV have been demonstrated using this intensity lasers over the next 5 to 10 years.
technique, opening the prospect of ultrafast nuclear or
high energy science! Under this assumption, the maximum power out of 1
cm beam diameter of a solid state laser is between
Panel B 22
100TW and 1 PW, the intensity (at wavelengths conversion of some longer wavelength driving field or
around 1um and nearly diffraction limited) is of the the direct production of coherent light via free
order of 1022 W/cm2, the electric field strength is of electrons either confined to a plasma or fourth
the order of 1012 V/cm (1000 a.u.). A beam diameter generation accelerator based device.
(limited by materials processing) of the order of one
meter would increase the focused intensity by another II.A.3.1 Direct Frequency Conversion of Long
four orders of magnitude (1026 W/cm2), and the field Wavelength Lasers
strength by two. However, we do not believe that this
The following assumptions are used to estimate the
is a realistic assumption. Furthermore, even to reach
ultimate limits of creating ultra-high fields at short
the maximum values for 1 cm beam diameter requires
wavelengths by direct frequency conversion of ultra-
enormous technological advances in laser etchnology
high intensity lasers. Direct frequency conversion
(B- integral, stretching factors etc.). Hence, even for
schemes are High Harmonic Generation, the VUV-
the visionary purposes of the present study we
emission of relativistic free electrons under the
anticipate the following frontiers:
influence of an ultrahigh laser field, and Compton
backscattering from high energy electrons.
Laser power: 10 petawatts (1016 watts)
pulse duration: 5 fs
II.A.3.1.1 HHG
wavelength: 0.8 to 1 µm
Intensity: 1023 W/cm2 The study of the interaction of atoms/molecules with
Electric field strength: 1013 V/cm (2000 a.u.) intense laser fields has resulted in the understanding of
Magnetic field strength: 106 Tesla the dynamics associated with the production of high
ponderomotive energy: ~ 10 GeV (Relativistic harmonic radiation in gas jets. The refinement of
scaling) experiment and theory have led the way for
understanding not only the single atom response to the
II.A.2.2 Other Mechanisms to Create Ultra- laser field but also the macroscopic propagation
High Fields associated with the harmonic source. Current sources
can produce coherent radiation out to 2 nm and a
The upper limits of the electromagnetic field strength
brightness exceeding third generation accelerator
as well as the lower limit for pulse durations will be
based light sources. The intensity produced by
encountered in relativistic heavy ion collisions. At the
harmonic generation have thus far has been limited
LHC at CERN, Pb82+ ions at energies of ~3000 GeV/
more by macroscopic target considerations then the
nucleon will collide head-on and generate electric field
fundamental bounds placed by the single atom-laser
strengths exceeding 1023 V/cm for pulse durations of
interaction.
only 10-28 s.
If the technical constraints of the target can be

II.A.3. VUV- and XUV- Sources for High
overcome by some means of a quasi-phased matched
Intensities and High Fields
extended source of atoms,ions and clusters then it is
The physical limitations of present technology invokes possible to estimate obtainable intensities. Assume a
the need for developments beyond our conventional near visible drive laser of 1 PW peak power producing
approach for generating coherent high fields and ultra- harmonic photons with a 1 keV limit and 10-6 power
short pulses at short wavelengths. The issue is an old conversion efficiency. Using multilayer mirrors
problem associated with materials, e.g. absorption, as producing a spot size of 10-3 of the fundamental beam
one pushes the wavelength beyond the VUV region. yields an intensity of 1022 W/cm2, well in excess of an
The options are either the use of nonlinear up- atomic unit of field. Furthermore, temporal
23 Panel B
compression of the harmonic process could produce an II.A.3.2 VUV- and XUV-Sources and Amplifiers
additional factor of ten in the peak power, although the
An intriguing new vista of TW, short wavelength
fundamental limit will be one optical cycle of the field
sources have been discussed in the context free
or 20 as.
electron lasers. The basic principle relies upon the
efficient exchange between the photon field and
II.A.3.1.2 Free Electrons in Intense Laser Fields
relativistic electrons accelerated in the magnetic field
Free electrons in intense laser fields undergo periodic of a wiggler. In this regard, two approaches are under
ponderomotive oscillations. At intensities above 1018 investigation each with their own merit but based on a
W/cm2 for visible-frequency lasers, this motion similar principle of high gain amplification. The
become relativistic. This has obvious importance for SASE (self amplified spontaneous emission) scheme is
light-source generation, and has been explored in the based on the exponential amplification of radiation
context of interactions with relativistic laser beams and which builds up out of the noise in the first few
with electrons in plasmas. sections of the wiggler. Thus, the technical limit of this
emission will be based on electron beam energy and
The oscillating fields in lasers make them interesting quality, e.g. emittance.
candidates for high periodicity insertion devices in
accelerators, and one could imagine such devices Both SLAC and the TESLA project at DESY have
producing tailored vacuum-ultraviolet or x-ray proposed operation at 1 nm with an intensity of 1020
radiation sources, possibly with high coherence. W/cm2. In the beginning of calendar year 1997,
important proof-of-principle demonstrations of the
In this context, we note several recent reseach projects SASE mechanism have been conducted at three major
in this area. (This is NOT a comprehensive list!) laboratories (Brookhaven, Los Alamos, UCLA) at
infrared wavelengths. These results provide an
Transverse Thompson scattering of photons from an important benchmark for testing the theoretical models
ultrafast laser scattering from a linear accelerator which are being used to scale to shorter wavelengths.
electron bunch at the ALS has produced ultrafast Current analysis have been promising.
pulses of hard x-rays.
A second approach (BNL and Jefferson Labs) is based
A SLAC proposal would turn part of the linac into a on harmonic up-conversion of a laser-seeded FEL. The
FEL producing 1-10 angstrom x-rays. advantages of this scheme over SASE are in the
coherent properities, peak power and pulse duration
SLAC has also produced 29 GeV gamma rays by (as short as 3 fs) of the output light. However, the
Compton backscattering of an intense laser from the SASE scheme is able to produce light at shorter
46 GeV electron beam. Compton backscattering wavelengths (below 10 nm).
produces extremely intense, ultra-short radiation with
associated high field strengths, which will be of main Based on recent current designs in the area of VUV-
interest to the high energy physics community. While free electron lasers and X-ray lasers we estimate the
it is outside the scope of AMO applications, it following limits of intensity and field strength at
represents one of the interdisciplinary links within the wavelengths between 1 µm and 1nm:
DOE program.
@ 200nm (TJNAF FEL) design intensity 1017 W/
A wakefield acceleration experiment at Michigan has cm2
produced MeV electrons in sub-picosecond bunches, @ 100nm (BNL FEL) design intensity 1020 W/
which could produce ultrafast x-rays via bremstrahlung. cm2
Panel B 24
@ 10nm (TTF FEL) design intensity 1017 W/ c. The focal spot size increases proportional to the
cm2 wavelength, thus decreasing the maximum
@ 1nm (TESLA FEL, SLAC FEL) design intensity. Hence, for comparable volumes of the
intensity 1020 W/cm2 active medium the maximum intensity is
@ 1nm hypothetical x-ray laser (10 mJ / 1 ps) expected to decrease at least with the fourth
intensity 1024 W/cm2 power of the wavelength.
(Note that these are “back of the envelope” upper II.B. Harnessing Quantum Dynamics
limits which don’t take into account possible sub-
In this section, we would like to project a vision of
optimal focusing characteristics in these sources.)
harnessing quantum dynamics as an important
enabling capability for the future. Here we have in
Conclusion: Current technology allows the assumption
mind not simply new probes of matter (be they optical
that the wavelength region between 1 µm and 1nm will
or otherwise), but more generally, the ability to
be covered by various high-intensity (1020 W/cm2),
manipulate complex quantum systems to do our
high-field (1011 V/cm) light sources, available to AMO
bidding with a degree of dexterity that is only
physics.
glimpsed by current capabilities. Because the systems
of interest are bound on energy scales given by
II.A.4. Infrared Sources of High Intensities and
electron volts over distance scales of Angstroms, the
High Field Strengths
time scales implicit for these investigations are in the
While today’s most intense solid state lasers operate in femto-second domain and beyond, and the intensities
the near infrared around 1 µm, no materials or involved are greater than 100 terawatts per square
concepts are presently known to create coherent light centimeter. Hence, a necessary component of our
at longer wavelengths (10 to 100 µm) with comparable vision is the need for the advancement of technical
intensities and field strengths. This is in remarkable tools to a frontier well beyond current capabilities.
contrast to the short wavelength region (1µm to 1 nm),
where both frequency conversion methods and As pulsewidths have decreased and peak power and
independent light sources exist at intensities around wavelength control has increased in the recent decade,
1020 W/cm2 and field strengths around 1011 V/cm. it has become possible to conceive of a new regime of
light-matter interaction in which the light is no longer
From a physical point of view one expects lower treated as a passive observer. We are approaching an
intensities and field strengths for the following era in which we can “sculpt” dynamical systems to a
reasons: large number of purposes, improving techniques for
chemistry, fast microelectronics, optical
a. The amount of energy stored in a given volume
communication, and even energy deposition in high
of an active laser medium of density rho
density plasmas. Some tantalizing recent work
decreases inversely with the wavelength of the
pointing to this new area is the coherent control of
radiation.
Bragg scatterers at synchrotrons, which could provide
b. The maximum bandwidth (ultimately limited by
a way to make high-brightness sub-picosecond x-ray
the transition energy) also decreases
sources (Larsson, Z. Chang, E. Judd, P.J. Schuck, R.W.
inversely with the wavelength, thus lengthening
Falcone, P.A. Heimann, H.A. Padmore, H.C. Kapteyn,
the pulses and decreasing the maximum power.
P.H. Bucksbaum, M.M. Murnane, R.W. Lee , A.
Machacek, J.S. Wark, X. Liu, B. Shan, Optics Letters
22 1012-1014 (1997)); production of wakefield
plasmas for compact particle accelerators and ultrafast
25 Panel B
sources of gamma rays and relativistic electrons (R. II.B.3. Pulse shaping and adaptive control
Wagner, S.Y. Chen, A. Maksimchuck, and D.
II.B.3.1. What and Why
Umstadter, PRL 78, 3125 (1997)); production of
unique forms of radiation, such as “half-cycle pulses” Behavior of quantum systems is determined by the
(D. You, R.R. Jones, P.H. Bucksbaum, and D.R. time-dependent Hamiltonian and initial conditions.
Dykaar, Opt. Lett. 18, 290 (1993)); and tailoring of Therefore, modifications of this behavior are made
coherent xuv radiation from high harmonics (I.P. possible by the application of external fields that
Christov, M.M. Murnane and H.C. Kapteyn, PRL 78, change the Hamiltonian and/or the initial state of the
1251 (1997)). system. Developments in optical technology have
now made it possible to envision detailed
Each of these has important applications to basic manipulation of quantum systems using carefully
science and to energy research; each also presents shaped electromagnetic pulses. This capability will
special opportunities for contact to other areas of allow the development of technologies at an entirely
science and technology. new sub-atomic scale, and at the same time allow the
utilization of uniquely quantum mechanical properties
II.B.2. Detailed Manipulation of Quantum for practical application. There are classical analogies
Systems to certain types of manipulation. For example, fields
might push an electron in a certain direction within an
The tools are now at hand that one can begin to realize
atom, deposit energy in a specific chemical bond, or
the long-sought goal of reaching inside of a quantum
induce directed electron currents in solids. However,
system and manipulating it with the same ease that one
there is also an inherent complexity in these systems
can manipulate a macroscopic system. Of course, the
due to their quantum nature. While this complexity
term “quantum systems” encompasses an enormous
can make simple classical manipulation more difficult
range of topics, and there is no one set of tools and
or impossible, it also provides additional degrees of
methods that will allow manipulation of all of them.
freedom for non-classical control. For example, states
At present there are some particular systems that are
of multi-electron atoms and molecules are naturally
promising for achieving this detailed level of control.
correlated and entangled. These uniquely quantum
features are exactly what is needed for applications in
Among these are the control of the center-of-mass
quantum computing, secure encryption, and other
degree of freedom of atoms and ions in traps; the
areas not yet envisioned that rely on the ability of
control of the vibrational degree of freedom in a
quantum systems to explore simultaneously many
molecule, and the internal electronic degree of
parallel paths.
freedom in an atom.
II.B.3.2. What do we need?

The most important applications that will be available
if this capability is realized are no doubt yet to be To realize arbitrary manipulation, tools are needed to
conceived, but some are obvious: the control of shape or mold the quantum wavefunction. These tools
chemical reactions, the production of materials with are electromagnetic fields and the interaction
unique optical and electrical properties, and the Hamiltonian. Wavefunction “sculpting” has two basic
development of better understanding of quantum requirements. First, the amplitude of the
dynamics. There are less obvious possibilities of electromagnetic field must have temporal variations
some promise including massively parallel computing, over periods comparable to the characteristic
and secure communications. dynamical time-scales of the system. Second, the field
amplitude must be sufficient to cause a significant
change of the quantum mechanical state. Therefore,
Panel B 26
the development of sources that can provide intense, currently used in classical control problems must be
coherent, broad-band radiation is a prerequisite to adapted to specific multi-dimensional quantum
quantum manipulation. Furthermore, optimal control problems. These algorithms will rapidly interpret the
cannot be achieved without the ability to arbitrarily quantum state feedback and produce an error signal
alter the time- dependent structure of the fields that for input into the field shaping device.
are used to sculpt the quantum state. In a very real
sense, the prospects for quantum manipulation are tied II.B.3.4. (Im)Possible Dreams
directly to our ability to alter coherent
In the following subsections, we outline potential
electromagnetic fields at will. In turn, exquisite field
applications of quantum manipulation to problems of
manipulation requires currently unrealized control of
fundamental scientific, and possibly practical, concern.
the properties of optical materials.
We do not imply that this is an exhaustive list.
Because the realization of these dreams is inexorably
II.B.3.3. Problems to be solved
linked to future technological developments, we
Incremental progress is currently being made in cannot provide specific example systems or
manipulating dynamics in atomic, molecular, and experimental details.
condensed matter systems. However, the ultimate
control described above cannot be realized until II.B.3.4.1. Controlling Coherent Collisions
solutions to extremely challenging problems have
At first glance, the random nature of collison processes
been found. First, new laser and electro- optic
seems at odds with the concept of a coherent collision.
materials must be developed to facilitate the
However, there does not seem to be any fundamental
production and control of the requisite fields. The new
physical restriction which would prevent the use of
frontiers for increasing the coherent bandwidth,
coherent radiation to affect collision dynamics. For
frequency, and intensity of laser sources is discussed
example, tailored light pulses could be used to
in Section III A above.
enhance or inhibit particular photo-assisted reactions
at specific times. Alternatively, coherent fields could
Second, in most systems of interest, the complexity of
be used to produce an initial atomic or molecular state
the Hamiltonian and number of degrees of freedom in
which is transparent to collisions at specific energies
the system prohibits the a priori determination of the
and/or the relative orientation of colliding particles.
most appropriate time-dependent field. Therefore,
Conversely, the atomic or molecular wavefunction
active feedback techniques must be developed to
could be manipulated so that it reacts at specific
adjust the field characteristics until the final quantum
times, and only in certain reaction coordinates. Lastly,
state converges to the desired configuration.
dynamics established in the internal degrees of
Implementation of adaptive feedback requires that
freedom of an atom or molecule, A, might be
several obstacles be overcome. First, methods for
transferred to a collision partner, B. In this case the
detailed control of the time-dependent fields must be
collision dynamics would facilitate excitation of
developed. This is no small task considering that in
internal direct application of radiation fields.
some situations sub-femtosecond temporal structure
will be required. Second, experimental methods for
II.B.3.4.2. Quantum Encoding
determining the time-dependent quantum state of the
system must be discovered and implemented. Such Secure communication is an important and ongoing
techniques will require high spatial and temporal problem. The properties of quantum systems make
resolution in each dimensional coordinate and will them potential useful for encryption applications. For
necessarily rely on the generation of tailored light example, information (phase and amplitude) can be
pulses. Third, the efficient algorithms that are encoded into the wavefunction of a complicated
27 Panel B
quantum system with many entangled degrees of Coherent control in the strong field limit may solve
freedom. After a very short time, phase evolution two fundamental problems in bond selective
makes the code unrecognizable. A time-dependent chemistry: dephasing, and low yield. This is because
field applied to the system at any time after the strong fields can dominate the energy scale in the
creation of the coded state acts as a “key” which problem as they reshape the molecular system. For
produces an echo of the initial state. The key can have recent work in this area, see G.N. Gibson, M. Li, C.,
limited access and be universal so that it is capable of Guo, and J. Niera, Phys. Rev. Lett. 79, 2022-2025
retrieving any code stored in that system. (1997), and E. Constant, H. Stapelfeldt, and P.B.
Corkum, Phys. Rev. Lett. 76, 4140-4143 (1996).
II.B.3.4.3. Single Atom/Molecule Electronics
II.B.4. High Intensity Optical Channeling.
Tailored light pulses produce a coherent quantum state
in an atom/molecule/nanostructure. This quantum When high intensity light propagates through a
state acts as a transistor, switch, or logic gate. Digital transparent medium, its presence alters the optical
data or analog signals are input to the device using an properties of the medium. The resulting self phase-
additional electromagnetic pulse. A third pulse modulation and self-focusing have already found
interogates the quantum state of the device providing many applications in short pulse laser technology,
the readout. The complexity of device function is micromachining and optical propagation. Other
determined by the complexity of the initial similar phenomena are electromagneticaly induced
configuration field as well as the I/O pulses. In fact, transparency and “photon bullets,” which are stable
single function quantum logic gates have already been conducting plasma channels. The latter have been
produced using trapped ions suggested for remote lightning protection.
II.B.3.4.4. Bond-Selective Chemistry Through As the power scales up, the nonlinearity changes in
Coherent Excitation some important ways. Above a critical whole-beam
power threshold, the principal nonlinear self-focusing
There has been recent progress towards this long-
mechanism becomes relativistic self-focusing. The
discussed goal of physical photochemistry. Multiple
consequences of this are pretty startling: An intense
interfering pathways toward specific ionization or
laser beam focused into a plasma in this regime forms
dissociation products has been demonstrated (L. Zhu,
a cavitation channel, a region of low or even zero
et al., Science 270, 77 (1995)). Ultrafast coherent
electron density, in which the laser can penetrate for
wavepacket control in molecules has also been
long distances. The channel formed in this way can
observed (B. Kohler, et al., PRL 74, 3360 (1995)).
be tailored by shaping the intense optical pulse to
Since most interesting photochemistry involves
optimise a number of physical properties, such as the
systems in contact with rapidly dephasing media such
density, width, length, or field gradients.
as solvents, a great premium is placed on ultrafast,
coherent, and strong fields that can perform their
One important application of this technology is
quantum-mechanical tasks in only a few tens of
transmission of the bulk of the laser energy deep into
femtoseconds, before dephasing of the system.
a plasma, where it can be deposited at a plasma
Furthermore, since the Hamiltonian for these systems
density gradient. Such schemes may be critical for
can be quite complicated, and only known
efficient energy conversion using laser-compressed
approximately, adaptive control strategies will be quite
fusion targets (ref: Fast Ignitor workshop).
important.
As important as this is for future energy development,

it is only a small part of the potential applications of
Panel B 28
high intensity laser-channeling. This expulsion of transition of the atomic structure of matter from its
electrons coupled to relativistic self-focusing then different states (eg. from solid to liquid to gaseous
produces a large (GeV/m) longitudinal wake field phase can be observed with unprecedented temporal
which can accelerate bunches of electrons to multi- resolution. Matter can also be heated isochorically
MeV energies over millimeter distances. Such beams (without change in density) to extreme temperatures
have already been shown to have some unique (kilovolts). These studies are important for the
properties, such as short bunch length and narrow understanding of radiation damage, material ablation
divergence. for thin-film deposition, fusion, pulsed power,
propulsion, waste disposal and plasma processing.
Applications to the needs of traditional particle The x-ray emission from the laser-heated solid-
acceleration are obvious: the tremendous increase of density plasma also makes a bright, ultrafast and
the field gradient in these plasmas can lead to great coherent table-top x-ray source that can be used to
scaling advantages for small accelerators. There may study transient phenomena on an ultrashort timescale.
be some unique opportunities here as well to take Such a source can also be used to study nonlinear
advantage of the novel conditions in the plasmas. For optics with inner-shell transtions. It is relevant to x-
example, the bremmstrahlung radiation produced ray lithography and indirect drive ICF. In the latter
when these ultrashort electron bunches hit a solid case, the source can be used as an imager to freeze
target may provide the best short pulse technology for hydrodynamic motion and provide a test bed for the
ultrafast gamma radiation. study of material properties at a wavelength relevant to
hohlraums.
II.C. Matter in Extreme Conditions
II.C.2. Extreme Fields
Advanced laser and particle sources providing short-
pulse and high-intensity photon, electron, and ion When the work done on an electron by the field over
beams are expected to become primary enablers of the distance of the laser wavelength equals the
AMOP science and technology in both the near and electron rest mass (1018 W/cm2 ), we enter a new
distant future. Each source has spatial, temporal and regime of nonlinear optics. In this case, a plasma
spectral characteristics that are unique and medium can be modified by the laser field in such a
complimentary. They will allow controlled deposition way that it can be used to guide the laser light at high
of energy into various systems, producing states intensity over a much greater distance than it would in
previously inaccessible in earth bound laboratories. vacuum. The light pipe that results when the
They will permit studies of the atomic physics of electrons and ions are driven from the axis of the
matter under extreme and unusual conditions, which channel can be used to guide another laser pulse. This
include: extreme pressure (Gbar) extreme fields (E >> is the basis for the proposed fast-ignitor fusion
1 keV/Angstrom, B > 1 gigagauss) concept. Gigagauss magnetic fields and electron-
positron plasmas may be created. Interesting ionic
II.C.1. Extreme Pressure states may be created and relativistic effects dominate
the interaction physics. The largest electrostatic fields
Everything from Fermi-degenerate gases,
ever produced in the laboratory are generated in
nonequilibrium plasmas and highly perturbed atomic
wakefield plasma waves, which can accelerate useful
systems can be studied in these interactions. Extreme
numbers of electrons to gigavolt energies in a distance
pressures are found in astrophysical objects, pulsed
of just a centimeter. This is a new regime of
power machines, weapons, advanced x-ray sources,
parameter space that may result in new properties of
and ICF fusion pellets. They may also enable new
matter and is relevent to advanced accelerators,
routes to IC fusion such as the fast ignitor. The
electron sources and fusion energy concepts. One of
29 Panel B
the exciting possibilities opened by high-intensity intense fields, atoms may undergo recombination
laser and ultra short relativistic electron and ion with electrons or other particles that are pulled out of
beams is the creation in the laboratory of extremely the vacuum.
high electric and magnetic fields at the critical
Compton limit of 1016 V/cm. In these extreme fields,
the relation between energy and the vacuum are
modified in a dramatic way. One expected
consequence is the breakdown of the vacuum. In
addition, the large energies deposited over a
macroscopic volume would be sufficient to generate
collective and coherent effects. This will result in the
formation of an e+e- plasma. Just as one needs a
theory of non-linear optics to understand strong
electromagnetic interactions, a theory of non-linear
QED will be needed to understand these collective
effects.One concept for achieving these fields
coherently backscatters an intense femtosecond laser
from relativistic electron beams to generate fields on
the order of 1029 W/cm2. Coherent effects in the
backscattering would then enhance the field by
ne2.Also, laser-based sources can be built for the
generation of energetic electrons (laser accelerators),
ions or neutrons. The pulse duration of these electron
bunches can potentially be subfemtosecond, which is
sufficiently short to lead to novel effects. For instance,
coherence effects can enhance the intensities when the
electrons in the beam are acting collectively (scaling
as N2 instead of N). The duration can also become
shorter than several interesting characteristic
timescales, such as Auger lifetimes.
II.C.3. Connections to Other Fields at DOE

High field AMO physics experiments are related to the
nuclear physics studies of interactions between
relativistic heavy ions at RHIC. In contrast to the
interactions at RHIC, which involve quarks and
gluons, the AMO experiments described here involve
photons and leptons. Studies of the interaction and
creation of particles in these experiments may be a
subset of those observed at RHIC. Because there are
fewer types of interactions interpreting these
experiments maybe be less complex. In addition, the
intense fields found in pulsars may be recreated by
high power laser lasers (or other sources). In these
Panel B 30
Panel C: Surface Interactions With Photons,
Electrons, Ions, Atoms, and Molecules
Chair:
J. Wayne Rabalais (University of Houston)
Panelists:
Raul A. Baragiola (University of Virginia)
Barbara H. Cooper (Cornell University)
F. Barry Dunning (Rice University)
Charles S. Fadley (Lawrence Berkeley National Laboratory)
J. William Gadzuk (National Institute of Standards and Technology)
Wilson Ho (Cornell University)
Dennis C. Jacobs (University of Notre Dame)
Theodore E. Madey (Rutgers University)
Steven J. Sibener (University of Chicago)
Nicholas Winograd (Penn State University)
Executive Summary comparable battery of techniques for control of the

state of a surface and improved theories, particularly
NEEDS: The present understanding of the interactions for thermal processes at the gas/surface interface. The
and behavior of particles (ions, atoms, molecules, relatively recent advances in the production of large
clusters, electrons) and photons with surfaces at the clusters of atoms and molecules represents an area that
basic atomistic level is far from complete. A large is naturally intermediate between AMOP and surface
number of outstanding questions remain that pertain science. Each area has much to learn from the
to, for example, the detailed dynamics of particle- expertise of the other. For example, for almost every
surface interactions, localized energy deposition at particle-surface interaction, there exists a comparable
surfaces, nonequilibrium phenomena, and the analog in gasphase collisions.
properties of atoms and molecules on a surface.
Central to improving the present understanding is BENEFITS: This synergistic relationship between
control of the energetic, spatial, and temporal degrees AMO and surface scientists will enable new advances
of freedom of the particles involved in the interactions, in:
coupled with manipulation of atoms and molecules at • experiments that involve selection, control, non-
the surfaces. Improved understanding of surface thermal chemical manipulation, and complete
phenomena is fundamental to the development and analysis at the atomic and molecular level.
synthesis of materials with specific physical and • theory that couples the discrete excitations of
chemical properties. This underpins future atoms and molecules with the continuum
technological advances in areas such as energy excitations in solids.
production and conservation, microelectronics, and the • the use of molecules and clusters for achieving
environmental and life sciences. Many of these an atomic level understanding of the
applications are based on phenomena that occur at mechanisms responsible for chemical catalysis
surfaces and interfaces, e.g. solid/vacuum, solid/gas, and gas-surface energy transfer.
liquid/vapor, and solid/liquid, as a result of stimulation • novel schemes for materials growth and
by particles or photons. Studying such phenomena has nanostructure fabrications.
historically been difficult and challenging. Although
much progress has been made to date, the microscopic The synergy will facilitate progress in the important
understanding of many interfacial phenomena remains areas of: (1) dynamics of excited states at surfaces, (2)
below that currently existing for homogeneous phases, non-equilibrium phenomena induced by particles and
i.e. gas-phase atomic and molecular physics and solid photons at surfaces, (3) control and manipulation of
state physics. particle- and photon-surface interactions at the atomic
and molecular level, and (4) advanced techniques for
OPPORTUNITIES: A unique opportunity currently probing particle- and photon-surface interactions.
exists to advance this challenging area of basic
science. This involves the integration of the expertise
and technology from atomic, molecular, and optical
physics (AMOP) with that of surface science. AMOP
scientists have developed an in-depth understanding of
the properties and behavior of gas phase atoms and
molecules, highly sophisticated experimental
techniques to produce and analyze particle beams in
well controlled states, and advanced theoretical
methods. Surface scientists have developed a
Panel C 32
Outline VI. Summary List of Basic Unsolved Problems

Involving the Interactions of Low Energy
I. Fundamental Understanding of Particle- and
Particles (Electrons, Ions, Atoms, Molecules,
Photon-Interactions with Surfaces
Clusters) and Electrons with Surfaces
II. Non-Equilibrium Phenomena
A. Low Density Excitations
VII. Summary List of Applications of Particle and
A1. Non-Equilibrium Conditions in Film
Photon Interactions at Surfaces
Growth and Modification
A2. Theoretical Approach
VIII. Conclusion Statement
A3. Technological Importance
B. High Density Excitations
B1. Dynamics of Electron Transfer I. Fundamental Understanding of
B2. Dynamics of Highly Concentrated Particle and Photon Interactions with
Excitations Surfaces
B3. Mechanism of Energy Flow in Considerable progress has been made over the past
Collisions several years in describing the properties of clean and
B4. Particle-Surface Interactions as Probes adsorbate-covered surfaces. Less is understood about
of Surface Dynamic Properties the dynamical processes that occur when particles
B5. Laser Induced Non-Linear (electrons, ions, atoms, molecules, and clusters) and
Phenomena photons impinge on a surface, especially when excited
states are involved. A detailed knowledge of the
III. Control and Manipulation at the Atomic and formation and relaxation of excited states is of
Molecular Level principal importance in understanding nonequilibrium
A. Energetic Control and State Selection processes and in exploiting these processes in novel
B. Spatial Control applications.
C. Temporal Control
Excited electronic states are formed near the surface as
IV. Other Advanced Techniques for Probing a result of the absorption and scattering of photons and
Particle- and Photon-Surface Interactions electrons and by the impacts of ions, atoms, molecules,
A. Beams of Ions, Atoms, Molecules, and clusters. Energy is also deposited directly into
Clusters, Electrons, and Photons nuclear motion by momentum transfer to surface
B. Advanced Combinations of Supersonic atoms. These impact-induced excitations range from,
Beams, Atomic Traps, and Atom Optics for example a change in the charge state of a low-
C. Femtosecond (fs) Surface Spectroscopy energy scattered projectile or an electron-hole pair
D. Spatial- and Temporal-Imaging of Surface creation by the absorption of a photon, to high density
Atomic Structures excitations such as track formation and material
E. Coincidence Techniques ablation resulting from heavy or highly charged ion
F. Surface Studies in High Pressure impact. State-of-the-art experiments utilizing surfaces
Environments that are well-characterized, i.e. atomically clean,
G. Higher-Efficiency and Higher-Speed aligned structures, and highly controlled beams of
Detectors particles that are mass-, energy-, charge-, and state-
selected, collimated, and pulsed (in some cases), in
V. Key Research Areas in this Report that are conjunction with techniques for complete delineation
Under-Represented in the United States of the interactions in terms of elemental-, spatial-,
33 Panel C
temporal-, and final state-resolution, are needed in nuclear collisions, excitation of electronic transitions,
order to reach a new level of fundamental creation of a local non-equilibrium, high-energy-
understanding. content region (mini-collision cascade), and generation
of vacancy and interstitial pairs. (2) The
Beam-surface experiments that probe the fate of a thermalization regime (0.1 - 10 ps) involving
scattered projectile or that follow the nascent dissipation of excess energy through phonons, rapid
excitations in the surface are required to provide a quenching of the cascade region, and material
comprehensive understanding of the relevant energy recrystalization. (3) The diffusion and recombination
and charge exchange mechanisms and the relaxation of regime (1 ns - 10 µs) involving thermal diffusion and
excited states. For example, final electronic state annihilation of point defects by diffusion to
distributions of scattered atoms or molecules, coupled recombination sinks. Meeting this theoretical
with theoretical models of nonadiabatic electronic challenge requires well coordinated expertise from
interactions, reveal the charge transfer mechanisms many areas in AMOP as well as from chemical and
and information about the lifetimes of excited states condensed matter physics. Theoretical modeling and
near surfaces. Desorption of atoms or molecules simulation of the time evolution of an excited atomic
following electron impact indicates the coupling of or molecular system coupled to a surface (with all its
nuclear motion to electronic excitations. Ultra-low unique attributes), possibly in an intense AC field
and thermal collisions of neutral atoms and molecules (laser) or DC field (scanning tunneling microscope
with interfaces are also of high interest, with such (STM), tunnel junction, field ion or emission tip),
gentle interactions dominating phonon exchange, requires creative new approaches transcending brute
sticking, and chemical reactivity. Fragmentation force diagonalization of large matrices or numerical
patterns following cluster impacts reflect energy solution of large but finite systems of ordinary
redistribution pathways and the time scales over which differential equations which incorporate standard force
energy redistribution occurs. Electron emission laws or manageable potential energy surfaces.
subsequent to impact identifies the specific excited
states produced in the projectile and/or substrate. Because of the importance of electron charge
Moreover, time-resolved spectroscopies involving redistribution and transfer, quasi-localised resonance
ultrafast lasers or third generation photon sources will state formation, and field-induced electron dynamics,
allow one to directly follow how electronic excitations the coupled, multi-dimensional quantum equations of
couple to other degrees of freedom and how localized motion must be able to treat the electronic and nuclear
excitations decay in space and time. Experimental dynamics on an equal footing. An additional challenge
advances, focused on increasing control of the incident arises because the solid and laser fields each present a
species and improving temporal and spatial resolution continuum of excited states that must be considered
for probing the final states, will provide new windows and exploited within theoretical models. Low and
for understanding dynamical pathways. ultralow energy interactions present another exciting
challenge due to the unusually large deBroglie
New theoretical developments are essential to wavelengths and sharp resonances which characterize
accurately treat the inherent many-body nature of such interactions. Surface charge density distributions
particle-surface interactions, including electronically and collective surface phonon modes must receive
excited states at surfaces and relaxation pathways. accurate treatment if such calculations are to
One of the challenges is the treatment of phenomena realistically model atomic scale behavior. It is
that evolve over a time scale of some ten orders of envisioned that innovative combinations of
magnitude. A simplistic delineation is as follows: (1) appropriately statistically averaged classical (Newton,
The collision regime (< 100 fs) involving direct Langevin equations, etc.), semiclassical (WKB,
Panel C 34
Gaussian wavepacket dynamics, etc.), and quantum surfaces which govern such processes. Consider, for
(coupled channels, wavepacket propagation on grids, illustrative purposes, the energy regime that is directly
soluble model Hamiltonians, etc.) particle-field models applicable to film growth and modification on surfaces
will be required, together with intuition for involving appreciable entrance channel barriers. In
differentiating the relevant from the irrelevant aspects this instance, a reasonable lower limit is a kinetic
of the interacting system. This work should provide a energy of the order of bond energies, ca 1 eV. The
tractable, useful, and informative theory on energy released upon bond formation is dissipated as
fundamental processes at surfaces that can serve to phonon-like excitations and lattice distortions which
guide, interpret, and predict experimental results. perturb the local environment in a manner similar to
Close experimental-theoretical coupling must be the excess kinetic energy supplied by the incident
maintained, each helping to guide the other in this beam. At this lower limit, chemical bonding
“self-correcting” drive to achieve a fundamental interactions become significant, the binary-collision
understanding of the interactions involved. This, in approximation becomes questionable, and inelastic
turn, will lead to unprecedented control and interactions between the incident particle and substrate
exploitation of these interactions in important can alter the incident trajectories. A reasonable higher
applications such as nanoscale surface modification, limit, in the case of ions, is a kinetic energy of the
low temperature growth of novel materials, and order of a few keV. In this range the sputtering yield
creation of metastable phases. becomes equivalent to, or higher than, the beam flux,
classical ion-trajectory simulations using a binary-
II. Non-Equilibrium Phenomena collision approximation provide a satisfactory
description of many of the collision phenomena, and
Energetic particle and photon beams provide a means
the impinging ions remain in the near-surface layers.
of producing conditions in the surface region that are
The thresholds for penetration, displacement,
far from thermodynamic equilibrium. Understanding
sputtering, and reaction occur in this energy range. In
the fundamental particle- and photon-surface
the case of neutral atoms, supersonic beams can easily
interactions will improve our ability to exploit them.
span the range from sub-thermal energies up to several
The new degrees of freedom resulting from the use of
eV. This allows one to selectively and systematically
controlled beams allow non-equilibrium excitation of
examine chemical reaction channels which become
solids, which can be used to deposit films, synthesize
accessible at ever increasing energies. Some of these
new metastable materials and phases and understand
channels may lead to new or more highly optimized
radiation effects. This section is roughly divided into
growth conditions than are typically accessible in
two subsections, i.e. low density and high density
CVD environments. Moreover, supersonic beam
excitations.
experiments permit intentionally selected growth
precursors to impact the target sample, greatly
A. Low Density Excitations
simplifying the analysis of growth mechanisms.
By low density excitations we refer to those created in The ability to select the energy, type, and arrival rate
the near surface region by, for example, the impacts of of particles, incident polar and azimuthal angles,
relatively low energy atoms, molecules, and ions. substrate temperature, background gases, and
stoichiometry allows control of the penetration and
A1. Non-Equilibrium Conditions in Film defect energy thresholds, film growth mechanisms,
Growth and Modification isotopic composition, low temperature epitaxial
growth, chemical reaction mechanisms, collision-
Particles of a wide range of incident kinetic energies
induced surface chemistry, energy flow in collisions of
can selectively influence film growth chemistry
molecular species, and coupling of gas and solid phase
depending on the nature of the potential energy
35 Panel C
excitations. While conventional film growth and clean/adsorbate covered surfaces. Such
techniques rely on high temperature to activate interactions, typically mediated by phonons, are
chemical reactions and diffusion processes, growth of crucial to an improved understanding of surface
novel high quality materials at low temperatures can phonon spectroscopy, i.e. bonding at surfaces, sticking,
be achieved by coupling the internal and translational and energy accommodation in general.
energy of the incident particles with the surface energy
modes. Low temperature growth is becoming A2. Theoretical Approach
increasingly important in a number of technological
A full understanding of the interactions involved will
applications where it is desirable to prevent
require the more sophisticated atomistic simulations that
interdiffusion at interfaces and to stabilize nanoscale
are currently emerging. A central problem that needs to
structures. The fundamental mechanisms
be resolved is the importance of the coupling between
distinguishing energetic beam deposition from thermal
electrons in the solid and the moving atoms in the
techniques result from localized deposition of energy
collision cascade initiated by the energetic interactions.
by the incident particles. The energy stored in the
Molecular dynamics simulations of radiation effects
incident particles can be used to overcome reaction
have incorporated this special case of electron-phonon
barriers and induce nonthermal chemistry.
coupling in a parametric form, and show that
Electronically excited states of impinging atoms is an
solidification and phase transformations in the energetic
example that is open for exploration. Nonequilibrium
atomic cascades are affected by the uncertainty in this
surface atom configurations can change nucleation and
coupling. Recent attempts have focused on ab-initio
growth modes, which include processes such as
descriptions of energy levels and energy transfer in
adatom and vacancy production and enhanced
energetic cascades, but this type of theory is still in its
interlayer mobility. The challenge is to learn to
infancy. Improvements are needed in calculating the
balance the beneficial effects of ion irradiation, such as
fate of reactive molecular precursors with reactive
local relaxation, creation of mobile vacancy/interstitial
interfaces. Sophisticated electronic structure
pairs, and enhanced diffusion, with the undesirable
calculations analogous to those developed for quantum
effects, such as permanent defect formation, lattice
chemistry and precision atomic physics applications
damage, sputtering, atomic mixing, etc. It is necessary
would have high impact in this area of endeavor.
to understand the role of particle energy, mass, and
charge in penetration of surfaces, displacement of
A3. Technological Importance
atoms, stimulation of chemical reactions, production
of metastable structures and high density materials, Many techniques employ energetic particles in the
and enhancement of epitaxy. growth process. These include sputter and plasma
Other non-thermal processes in surface modification deposition, pulsed laser deposition, and ion-assisted
by energetic beams include electron- and photon- and direct ion beam deposition. These techniques
stimulated desorption and reactions. These processes often involve a wide range of incident species and
involve electronic excitations that lead to bond- energies. Experiments with highly controlled incident
breaking. The manifold of possible electronic beams (ions, neutral molecules, clusters, photons) and
excitations allowed in gaseous molecules may be very real-time in situ diagnostics are critically needed to
different in the condensed phase. Many challenges gain a better understanding of the role of energy in
remain in understanding energy transfer, charge modifying growth modes and materials properties.
transfer, and the dynamics of excited-state evolution. This new understanding will enable us to control
An improved understanding of energy flow in thermal important film properties such as structure,
energy collisions is also needed if we are to predict stoichiometry, internal strain, surface and interface
energy transfer between impinging neutral particles roughness, and adhesion. Energetic beams have been
Panel C 36
shown to have beneficial effects in the growth of a solid, stimulating multiple electron transfers that
magnetic multilayer materials and wide band gap result in the transient formation of “hollow atoms”.
semiconductors (SiC, Group III nitrides, and Electrons evolve in unusually high n orbits which
diamond). This approach shows great promise for would resemble Rydberg states except that they are
controlled growth of novel materials and metastable polarized by the huge fields and they merge into
phases. In order to achieve spatially resolved extended electron states of the solid.
deposition and surface modification, it is desirable to
develop new techniques relying on atomic optics and B2. Dynamics of Highly Concentrated
ion beam focusing. Of course, energetic electron and Excitations
photon beams will continue to be of critical
Ionization spikes (dense plasma) in non-metals, their
importance for lithography in microelectronics
evolution in some cases to a dense exciton gas, and
applications as dimensions are reduced to the sub 100
their role in particle ejection, and non-thermal
nm range.
transformations in the solid (cratering, bond-breaking
and reforming, phase transitions, etc.) cannot be
B. High Density Excitations explained by existing theories. These phenomena, that
An exciting new development in the field of can be started by fast ionizing particles or slow highly
interactions of particles and photons with surfaces is to charged ions, are important radiation effects in living
produce extended regions in solids that are excited far tissue and semiconductor devices. A frontier in this
from equilibrium conditions through the impacts of area is the development of models for the complex,
energetic heavy ions and slow highly charged ions, multiple-particle excited region and the time-varying,
clusters or large molecules. The highly unusual inhomogeneous electric fields. This can be
conditions which result cannot be described with accomplished by a new generation of molecular
existing models of particle-solid interactions. dynamics simulations which can include the
Questions of interest include the following: appropriate local electric fields and many body
interactions between ions, excited atoms and
B1. Dynamics of Electron Transfer molecules.
Interactions between ions and surfaces present new

B3. Mechanism of Energy Flow in Collisions
challenges which arise from the many-body target and
its low geometric symmetry. Well-defined The flow of energy in collisions of clusters and large
experiments involving ion neutralization and charge biomolecules with surfaces is a complicated, albeit
exchange at surfaces are needed to probe thresholds very important problem. Current atomistic and
for excitation and ionization, to examine energy level continuum mechanics approaches are found,
shifts and broadening, and their dependence on particularly for large, fast projectiles, to be insufficient
particle velocity, surface electronic structure, and to explain the coupling and evolution of vibrational
crystal structure and to investigate the effects of and electronic excitations in the cluster and at the
external fields and hybridization of electronic states surface. These interactions result in extreme
near surfaces. The use of highly charged ions (HCI) phenomena that include the formation of very hot
provides a test bed for models that go beyond the plasmas in the solid, accompanied by photon and
independent particle description. HCI can range from particle emission. This can lead to shock waves
He2+ to U92+ . At the upper end of this charge scale, propagating through the material, cratering, and
they are a source of a wide variety of new physics. ejection of material. The projectile cluster can
The electric field produced by a HCI and its image can disintegrate in the collision or, at low velocities, be
induce enormous distortions of the surface potential of reflected in an unusual excited state, which includes
37 Panel C
shape distortions, internal shocks, and vibrations. The III. Control and Manipulation at the
relaxation of the cluster can result in fragmentation and Atomic and Molecular Level
thermionic electron emission and evaporation. The
latter permits study of highly localized thermal The previous two sections have focused on
phenomena. A goal here is to obtain complete experimental and theoretical approaches to address
characterization in terms of the underlying unanswered questions regarding fundamental particle-
mechanisms, including molecular and surface quantum and photon-surface interactions, and the non-
state-specific excitations, reactive processes, molecular equilibrium excitations that they entail. We have
fragmentation, and dissociative deposition. stated that an increased understanding of these
Controlling the many reaction channels is also of interactions will enhance our ability to exploit them.
interest, as are interactions with complex surfaces Here we elaborate on techniques and approaches that
(frozen gases, organics, polymers, clusters). will ultimately lead to our ability to understand,
control, and manipulate these interactions at the
atomic and molecular level.
B4. Particle-Surface Interactions as Probes of
Surface Dynamic Properties
Understanding of the physical and chemical properties
Plasmons, collective excitations of valence electrons, of materials and of the means for achieving energetic-,
provide an example of electron correlation effects that spatial-, and temporal-control and manipulation of
can occur at surfaces or in the bulk of solids and small atoms and molecules are the fundamental
particles. A long standing fundamental problem in underpinnings upon which nanotechnology is based.
solid-state physics has been how plasmons form and Atoms and molecules impinging on a surface can now
evolve in time and space, including their decay into be prepared in specific translational, electronic (exited
quasiparticle excitations. It may soon be possible to ions and neutrals), spin, and internal states (vibrational
study this important problem as a result of the and rotational), providing well-defined reagents. Once
development of new ultrafast laser techniques that adsorbed, selective and nonthermal chemical processes
provide a time resolution smaller than, or of the order can occur, driving a diverse body of research. The
of, the response time of the valence electrons (10-16 - scanning tunneling microscope (STM) has become a
10-14 s). Surface plasmon excitations by photons and powerful tool with the ability to probe and manipulate
high energy particles can be monitored optically for single atoms and molecules. Using femtosecond (fs)
real-time characterization of surfaces during materials lasers, it is possible to access electronically excited
processing and synthesis. intermediates and tailor intramolecular response
dynamics. Both the tunneling electrons from the STM
B5. Laser Induced Non-Linear Phenomena and photons from fs lasers can induce forces
Non-linear phenomena in the coupling of high power associated with select electronic excited states and can
lasers with solids can lead to ejection of material from be used to “push” constituent atoms along desired
the surface. These phenomena induce a wide range of reaction pathways, including motion on the surface,
physical and chemical processes, depending on the the breaking and forming of individual bonds, and the
excitation density, that have analogies and differences desorption of products. From measurement of the
to those caused by ions. The unusual states of matter final translational and internal state distributions of the
that are produced can be studied using AMOP desorbed molecules, further insights into the
techniques, such as picosecond (ps) lasers, sub-ns mechanisms driving atomic and molecular motion can
particle detectors, and coincidence techniques. High be obtained. Since charge transfer underlies many of
power lasers can be used for materials synthesis, the mechanisms involved in atomic and molecular
micromachining, desorption, and other surface manipulation and reaction, it is important to study
modification processes. electron interactions with atoms, molecules, and
Panel C 38
clusters at surfaces. The energy levels and spatial B. Spatial Control

distribution of excited states of atoms and molecules
Recent advances in scanning probe technology make it
are directly involved in these interactions. Little is
possible to study single atoms and molecules,
known about these states and theoretical investigations
providing an unprecedented opportunity to understand
are critically needed for guiding the interpretation of
and control materials. It is now possible not only to
experimental results and in making predictions of how
image with atomic resolution, but to obtain
individual bonds are made and broken. For electron
spectroscopic information and to induce chemical
and photon interactions with surfaces, the goal is to
reactions with single bond precision. By examining
understand the mechanisms of excitation, ionization,
individual atoms and molecules, it is possible to isolate
electron capture, desorption, sputtering, reactions,
environmental effects and obtain their intrinsic
damage, ablation, and charging of insulators.
properties. Results from such studies are particularly
attractive to theoretical investigations. Since tunneling
A. Energetic Control and State Selection
electrons are confined to atomic dimensions,
Materials modifications can be controlled by manipulation of single atoms and molecules is
impacting the surface with atoms and molecules possible, providing the opportunity of building
prepared in specific energetic states. High materials from basic atomic units. Atoms and
translational energies can be used to overcome molecules can be arranged into specific configurations,
reaction barriers. Molecules in one vibrational state leading to nano-materials with novel properties. The
may be more effective than another in breaking or ability to control and manipulate individual atoms and
forming a chemical bond. Electronically excited molecules and to induce chemical reactions with
atoms and molecules can also promote chemical atomic resolution is the basis for single electron
reactions, as is evident in plasma assisted deposition devices with ultra-small dimensions which can operate
and etching. By preparing atoms and molecules in at room temperature.
well defined excited states, it is possible to unravel the
mechanisms and dynamics of many complicated Another exciting and AMOP-based opportunity
reactions in catalysis, atmospheric chemistry, and involves stimulation of new research activities in gas-
plasma reactors. State selection of atoms and surface atom optics, incident beam control, and pattern
molecules offers another dimension in the control of formation. The use of either physical,
materials and the opportunity to tap into the extensive electromagnetic, or optical fields can lead to well-
tools which have been developed by the AMOP focused beam spots of selected reagents on surfaces.
community. In addition to obtaining a basic Standing wave-interference patterns, already in use for
understanding of fundamental interactions between such purposes, are but one application that will come
atoms and molecules with surfaces, state selection is from this new field of endeavor. This may well lead to
expected to result in reactions which cannot be the controlled fabrication of nanoscale structures
accessed by atoms and molecules with a thermal having equivalent impact to the more traditional
distribution. For example, new adsorption sites can be technologies of lithography, STM-based manipulation,
occupied and reactions can occur on entirely different and self-assembly.
parts of the potential energy surface. Species on the
surface resulting from such reaction pathways can be C. Temporal Control
probed by the STM. By creating an interference
Surface chemistry can be induced by tunneling
pattern on the surface with photon and atom beams,
electrons from STM, photogenerated electrons from a
nanoscale structures can be formed on the surface
fs laser, and particles (ions, atoms, molecules,
which are composed of materials with novel structures
clusters). Several different mechanisms are known to
and compositions.
be important in these interactions. For example, a
39 Panel C
mechanism which involves inelastic negative ion deposit more energy or material in a small spot, thus
resonance scattering is often responsible for the stimulating changes in the local effective temperature
induced reactions. Using fs lasers, the goal is to probe or concentration of reacting/exciting species. Such
the time scales for bond breaking and formation on the beams can also be rastered over the surface (either by
surface. Since the photons are confined to a pulse of moving the beam or by moving the sample) so as to
10 - 100 fs duration, the induced chemistry can be yield laterally-resolved images of the surface. Such
significantly different than that induced by cw and ns imaging is becoming increasingly more important for
laser and particle pulses. Excitation with fs laser complex, technologically or environmentally relevant
pulses also allows the study of energy transfer and surfaces that are often highly heterogeneous in the
coupling of the electronic degree of freedom to the lateral dimensions. Rastering can also be used to write
nuclear motion. It is very useful to consider fs induced nanometer-scale patterns on surfaces in a variety of
chemistry of the same molecules in the gas phase and materials, thus presenting exciting possibilities for the
in solutions, which provides a general understanding characterization and production of next-generation
of chemical dynamics. In excitation with fs laser semiconductor circuits and magnetic storage devices.
pulses, important information comes from using an By combining imaging while sputtering, it is possible
excitation time scale that is shorter than, or to carry out 3D tomography of solids of arbitrary
comparable to, the time scales involved in energy composition at an unprecedented resolution.
relaxation and transfer. By stretching the laser pulse to Commercially available ion beam sources permit
a ps timescale, the excitation rate becomes smaller focusing of Ga+ ions at 15-50 keV down to a spot size
than the relaxation rate, resulting in different reaction approaching 5 nm. With further development using
pathways. The combination of fs lasers with STMs AMOP techniques, it should be possible to improve on
provides an opportunity to probe, manipulate, and this resolution and/or create beams of state and energy
control matter on the fs temporal and angstrom spatial selected ions at lower energies. The sizes of such
scales. Nonlinear optical excitation is expected at a beams are thus smaller than the collision cascade
tunnel junction, resulting in the measurement of induced in the solid by the projectile itself, opening up
atomically resolved optical properties. the possibility of studying the physics of the cascade
process in more detail than has been possible
previously. With associated theoretical interpretation,
IV. Other Advanced Techniques for such studies would have a very positive impact on the
Probing Particle- and Photon-Surface technique of secondary ion mass spectrometry that is
Interactions an ubiquitous tool in materials science and,
particularly, in the electronics industry. These focused
In addition to those mentioned in earlier sections of probes, when combined with mass spectrometry, offer
this report, several unique new techniques have been new possibilities for high-spatial-resolution chemical
developed over the past decade, many of which are imaging with applications in geology, environmental
still evolving, that offer unique opportunities for science, and biology.
probing particle-and photon-surface interactions.
Many of these new techniques have strong overlap Photon beams from third-generation light sources can
with existing AMOP interests and expertise. be focused down to 10-20 nm, permitting
simultaneous spectroscopy and microscopy (via
A. Beams of Ions, Atoms, Molecules, Clusters, sample scanning). Such “spectromicroscopy” can be
Electrons, and Photons fruitfully applied to atomic and molecular species
deposited on surfaces, e.g. from ion or atom beams.
The use of highly focused beams to study surfaces is
Using both focused ion beams and focused photon
of interest for several reasons. A focused beam can
Panel C 40
beams together would permit studies of the rates of C. Femtosecond (fs) Surface Spectroscopy
diffusion of species as well as changes in chemical
The development of ultrashort laser pulses that are
state with lateral displacement away from the position
now typically 60 fs in duration, but with values as
of the primary collision. Core-and valence-level
short as 5-10 fs having been obtained, has opened up
photoelectron spectroscopy, Auger electron
new possibilities for studying electron, photon, and
spectroscopy, and soft x-ray absorption spectroscopy
energy transfer dynamics at surfaces. In these
can be carried out with unprecedented resolution and
experiments, single- and multi-photon absorption can
experimental control, including the variation of light
lead to time-resolved electron excitation, e.g. into
polarization and measurement of outgoing electron
image states near surfaces that are one-dimensional
spin.
analogues of Rydberg states in atoms. Electron
emission from these excited states can be studied by
Optical pumping or magnetic state selection via
using pump-probe techniques. Thus, the energies and
hexapole magnets can produce beams of aligned atoms
lifetimes of electronic states near surfaces can be
and ions. Studies of spin dependences and their
probed as well as the influence of photochemically-
surface interactions will be invaluable for probing of
induced surface reactions. Alternatively, the energy
magnetic surfaces and interfaces, giant
from a single laser pulse can be deposited over a short
magnetoresistive structures, colossal magnetoresistive
time into secondary electron creation, with these
compounds, and high-temperature superconductors.
electrons then driving surface chemical bond changes
that can be followed in time, e.g., via time-of-flight
B. Advanced Combinations of Supersonic
mass spectrometry.
Beams, Atomic Traps, and Atom Optics
Supersonic beams have revolutionized our D. Spatial- and Temporal-Imaging of Surface
understanding of precision spectroscopy and reaction Atomic Structures
dynamics. Atomic traps have had a similar impact in
New probes of surfaces based on ion and photon
many fields, spanning the range from atomic fountains
beams also offer the possibility of studying the internal
for clocks to Bose-Einstein condensation. Atom optics
atomic structures of surfaces on time scales relevant to
are now being applied for precision measurements,
surface chemical processes. For example, in the
interferometry, and pattern generation including
recently developed technique of scattering and
holography. It is clear that outstanding scientific and
recoiling imaging spectroscopy (SARIS), the atomic
technological advances will result from the combined
structure is determined via two-dimensional ion
use of these incisive techniques. New techniques
scattering patterns from a crystal in a time-of-flight
involving high-brightness neutral beams, spatially-
system. The pattern acquisition time is in the few-
guided and tightly-focused neutral beams, and
second range and individual images of the scattered
mesoscopic pattern deposition will follow from such
and recoiled particles can be resolved on a 10 ns scale.
studies. Already extant exploratory studies involving
For many surface reactions at near-UHV conditions,
ultra-cold and spatially controlled neutral beams
this is rapid with respect to surface atomic diffusion
injected into optical fibers may lead to new classes of
and reaction. These ion scattering images exhibit
atomic gyroscopes. Atoms exiting such fiber-optics
extreme sensitivity to surface structure, providing a
based devices may find application as atomic
real-space, element-specific surface crystallography.
“fountain pens” for lithography and mesoscale
This technique also offers new opportunities in the
chemistry.
detection of surface hydrogen, the study of non-planar
scattering events, the analysis of disorder at surfaces,
determination of surface diffusion and kinetics, and the
41 Panel C
study of ion-surface charge transfer characteristics. provide new insights into the details of dynamic
New applications of this ion scattering technique to surface processes.
liquid surfaces, which are currently emerging, offer
the possibility of monitoring dynamics on fluid F. Surface Studies in High Pressure
surfaces. With high-brightness photon beams from Environments
third-generation synchrotron radiation, it is currently
possible to measure high-resolution chemical-state- Most surface studies have been carried out in ultrahigh
resolved core-level photoelectron spectra on time vacuum environments, with possible pretreatment of
scales in the second range and to measure two- the surface at slightly higher pressures so as to carry
dimensional photoelectron scattering and diffraction out chemical reactions. The ability to carry out
patterns from the crystal lattice in minutes. Similar measurements at higher effective pressures of up to
information can be obtained on a smaller scale by even 10-3 torr would permit duplicating the conditions
Auger mapping with finely focused electron beams. found in semiconductor device and magnetic disc
Such ion and photon probes can follow the fabrication and provide data of more technological
development of different chemical states in time, thus relevance. Optical probes are most readily adapted to
directly deriving kinetic information. The scattering high pressure environments since photons can travel
images and diffraction patterns also permit through dense gases under appropriate conditions. An
determination of local atomic structures for the example is probing second-harmonic generation with
various chemical states present. Such measurements lasers, fluorescence, and Raman techniques. Particle
could be applied, for example, to surface reactions beams present a greater challenge since they are
carried out with state-selected ion or atom beams. attenuated in dense gases. The use of particle beams
could be achieved by using ionic or atomic beams of
suitable flux and/or surrounding the sample with a
E. Coincidence Techniques
differentially-pumped cell whose apertures
Coincidence measurement techniques are widely used accommodate the entrance of the excitation source and
in AMO physics. Application of similar techniques to the exit of the detected products. With suitable
surface studies offers several advantages. The use of designs, it might be possible to work at pressures in
pulsed ion, atom, or photon probe beams coupled with the 5-10 torr range, thus more nearly approaching the
coincidence measurements of outgoing ions or conditions of atmospheric and environmental reactions
electrons, or among the various products of the on surfaces.
excitation, could significantly enhance our knowledge
of energy flow and time evolution in surface G. Higher-Efficiency and Higher-Speed
processes, including the electronic states and atomic Detectors
configurations involved in desorption, decomposition,
and electron emission. One challenge in such Developments in particle and photon detectors now
measurements is that surfaces are copious sources of allow single particle detection under a wide range of
secondary electrons, ions, and atoms, making the conditions. However, this is not yet possible in some
detection of true coincidences more difficult. Other important cases, such as very large molecules and
problems are the difficulty in efficiently collecting clusters (>106 Daltons) in mass spectrometry, atoms
ions or electrons from surfaces and the ability of and molecules sputtered from surfaces, and low energy
surfaces to reneutralize and recapture species. atoms and molecules important in new processing
Electron-electron and electron-ion coincidence applications. The development of higher-speed and
measurements are currently being studied by a few higher-efficiency detectors for atoms and ions requires
research groups. Expansion of such efforts would an understanding of how the kinetic energy of atomic
motion is transferred to electronic excitations in solids
Panel C 42
at low impact velocities, resulting in electron emission. • The STM was developed in Europe and novel
Even with more intense beams of both photons and applications of scanning probes are continually
ions, many experiments are detection-rate limited. For being demonstrated, especially in Germany and
example, the rate of acquisition of photoelectron Switzerland.
spectra is currently limited by the capabilities of • Both Japan and Germany have substantially
multichannel detectors. For ions or atoms, detection is larger commitments to femtosecond laser work
complicated further by the low and strongly energy in chemistry, biology, and materials science.
dependent efficiency of the detectors. The standard
particle detectors employed in particle/surface VI. Summary List of Basic Unsolved
interaction experiments are the channeltron multiplier Problems Involving the Interactions
and the microchannel plate array. These have near of Low Energy Particles (Electrons,
unity efficiency for detection of electrons and Ions, Atoms, Molecules, Clusters)
energetic ions at 10 keV, but the efficiency for ions or and Photons with Surfaces
atoms monotonically falls to zero as the velocity of the
ions decreases. Developments in detector technology 1. Theoretical treatment of excited states at
would enormously expand the capabilities of many interfaces.
beam scattering techniques, permitting more sensitive 2. Atomically resolved structure determination of
and/or higher-resolution studies in many surface surfaces and adsorbed species.
characterization and surface analysis studies. Possible 3. Quantum-state-specific control and atomically-
approaches for enhancing particle detection involve and chemically-resolved spectroscopic
laser ionization of the neutral beam and/or characterization and manipulation of surfaces.
development of new surface coatings with higher 4. Time- and spatial-resolved spectroscopic
electron emission coefficients. Fundamental research monitoring of dynamic bond breaking and
on detector development, including how the kinetic formation processes at surfaces.
energy of atomic/molecular motion is most efficiently 5. Dynamics of energy and charge transfer at
transferred to electronic excitations in solid surfaces at surfaces, i.e. the flow of energy and charge and
low impact velocities, would thus be very beneficial. the motions of atoms in particle-surface
interactions.
V. Key Research Areas in This Report
That are Under-Represented in the VII. Summary List of Applications of
United States Particle and Photon Interactions at
Surfaces
• Basic studies of the interactions of low energy
(0.1eV - 0.5 keV), well-defined neutral and ion 1. Nonequilibrium growth, nanoscale fabrication,
beams with surfaces is vastly under-represented and processing of materials.
in this country. Germany, Japan, France, and The 2. New techniques involving high intensity,
Netherlands are presently leading the ion beam spatially guided neutral and ion beams for
field. The area is replete with important mesoscopic pattern deposition.
applications. 3. Mechanisms of surface chemical reactions and
• Basic studies of the effects of low energy (1 eV - catalysis.
1 keV) electron beams with surfaces are under- 4. Environmental problems, including sensing and
represented in this country. This area also has processing of biological molecules.
important applications. 5. Futuristic materials based on atomic and
molecular manipulations.
43 Panel C
VIII. Conclusion Statement

This report has identified some important research
needs, opportunities, and applications that can be
achieved through the interaction of two groups of
scientists, i.e. atomic, molecular, and optical physicists
and surface scientists. The synergistic expertise and
techniques from both groups provide an unparalleled
opportunity to make significant advances in our basic
understanding and application of the interactions of
energetic particles (electrons, ions, atoms, molecules,
and clusters) and photons with surfaces.
Panel C 44
Panel D: Theory of Structure and Dynamics
Chair:
Chris Greene (University of Colorado)
Panelists:
Alexander Delgarno (Harvard Smithsonian Center for Astrophysics)
Charlotte Fischer (Vanderbilt University)
Kate Kirby (Harvard College Observatory)
Kenneth Kulander (Lawrence Livermore National Laboratory)
Uzi Landman (Georgia Institute of Technology)
James McGuire (Institut fur Kernphysik)
Vincent McKoy (California Institute of Technology)
Anthony Starace (University of Nebraska)
Malcolm Stocks (Oak Ridge National Laboratory)
David Yarkony (Johns Hopkins University)
Executive Summary the development of femtosecond lasers has brought

coherent control to the brink of reality, so has the
In AMO physics, the terms “structure and dynamics” enhanced ability to manipulate atoms on surfaces
encompass diverse topical areas that intellectually brought the potential of engineered nanostructures to
challenge and relate closely to the mission of the the forefront of this field. The techniques of atom
Department of Energy (DOE). In these working interferometry and lithography will certainly play key
papers, we summarize our findings. Our deliberations roles in the design of nanostructures.
have identified key themes in the theory community
that overlap and further the research goals of Basic “AMO physics in extreme conditions” includes
Energy Sciences at DOE, broadly-construed. This unusual environments where basic scientific questions
panel has assessed new areas ripe for future remain inadequately understood. Atomic and
development within the next 5-10 years. Because our molecular collisions at ultracold temperatures, for
charge has been specifically aimed at identifying new instance, probe the pure quantum limits. Ultra-intense
research directions, we stress at the outset that many laser fields produce dramatic new physical effects and
exciting theoretical (and experimental) areas will not processes, while ultra-short light pulses are important
be explicitly discussed. Other theoretical areas with for the “Control” goals discussed above. New
great potential and relevance to the DOE mission are generation synchrotron light sources probe atomic and
not covered in this report. We have no room, for molecular structure at ultra-high resolution (and in
example, to detail the varied and deep connections of some cases at ultra-high energies), which magnifies
AMO science to the disciplines of astrophysics, the limitations of conventional independent-particle
atmospheric science, space science, environmental models and points to the need for improved theoretical
science, nuclear physics, particle and fundamental capabilities.
physics and the physics of reactive flows and shock
waves. “Novel states of matter and light” have energized
much of the scientific community in a fast-paced
The areas of greatest excitement and potential for near- exploration of striking new directions, largely driven
term development in structure and dynamics are by recent experimental progress. Several groups can
grouped into five categories: Control; AMO physics now create BEC in their laboratories on a daily basis,
in extreme conditions; Novel states of matter and light; but at the same time many basic theoretical issues
Extending the frontiers; Opportunities and horizons in require a far deeper understanding. Quantum optics
high-performance computing. We begin with a short theory and experiment, especially in the area of laser
summary of each of these categories. The rest of our cooling of atoms, continue to show rapid, exciting
report elaborates on each in somewhat greater detail. progress.
A continuing theme in all of these areas is a natural
progression of knowledge and understanding from “Extending the frontiers” groups together several
simple prototype atomic species to more complex areas that touch on or encompass current work in the
species like molecules, clusters, and surfaces. BES AMO Physics program. New directions and
current bottlenecks deserving of priority effort are
“Control” is an important theme for the future. It mentioned, including the direct description of real-
embodies a clear long-range goal for AMO science. time dynamics for problems like intense laser-atom
The field of coherent control, for instance, involves the interactions, where the interaction is strong and
manipulation of atomic and molecular processes by the localized in time, and must be treated
design of femtosecond light pulses that cause the nonperturbatively. Another area ripe for extension is
system to respond in a prespecified manner. Just as the theoretical study of relativistic correlation effects,
Panel D 46
both in heavy atoms and in simple molecules theory does differ from experiment in “equipment
containing heavy atoms. These tie in with the DOE needs.” Access to large-scale computational hardware
mission, as discussed below. Short-time dynamical is needed by theorists in order to undertake certain
studies using periodic orbit theory and scaled-variable types of cutting-edge calculations.
spectroscopy can be applied to a range of new
problems. Finally, the interpretation of energetic CONTROL
plasmas requires a deeper understanding and the
Coherent control
development of methods to explore a large number of
processes involving collisions of electrons, ions, The dynamics of quantum systems can be modified by
atoms, and molecules. coherent light pulses, and energy can be moved around
in a predetermined way on an atomic scale. Advances
“Opportunities and horizons in high-performance in short pulse laser technology have made it likely that
computing” includes areas where progress in AMO the long-sought goal of quantum control of molecular
science hinges on the utilization of large-memory, collision dynamics will finally be achieved. In
scalable multicomputers. The high performance of principle, manipulation of a time-dependent pulse will
these powerful modern computers can dramatically permit the subsequent evolution of the system to be
enhance our ability to achieve robust descriptions of controlled. Amplified few-fs Ti:sapphire pulses have
fundamental processes and complex systems across a focused intensities larger than 1014 W/cm2, which is
wide spectrum of AMO science. Development of strong enough to drive molecular transitions
scalable and paradigm-changing algorithms required efficiently. Selective dissociation, control of reactions,
for efficient use of these new computing architectures, and preparation of desired molecular states or
coupled with ready access to large parallel computers, structures can be achieved by these methods.
can lead to major breakthroughs in computationally Accomplishing these goals requires intimate
intensive applications and can enhance the impact of interaction between experiment and theory.
theory on experiment. Knowledge of the molecular potential energy surfaces,
dipole coupling strengths as functions of molecular
Elaboration on the Five Themes Described geometry and the ability to determine the variations of
Briefly Above the time evolution of the coherent wave packet caused
by changes in the phases of the pulse will allow
Before we discuss the scientific directions and
optimization of the product yields. Precise
connections identified by our panel, we believe it is
determination of these required parameters exceeds
important to recognize one of the constraints we faced
existing theoretical capabilities for all but the simplest
in our undertaking. The separation of “Theory” into
diatomic systems.
one panel at this workshop, split off from the other
topical areas represented in this report, is unfortunate
For more complicated systems, nevertheless, theory
because the most productive advances in science—
can provide approximate starting points for
especially in AMO science—result from fruitful
experiments designed to provide feedback to more
synergism between experiment and theory.
accurately calibrate the system response, leading
Consequently, most of the forefront areas mentioned in
iteratively to the desired results. One anticipated
this section overlap closely with the areas discussed by
experimental problem is that the UV or VUV
the other panels. In cases where the other panels
wavelengths required to induce an electronic transition
propose an area ripe for further development in the
in most molecular systems are much shorter than those
coming decade, it should be understood that extensive
produced by the Ti:sapphire amplifier. Harmonic
theoretical contributions can be very valuable for
conversion or frequency mixing techniques can
guiding and interpreting experiments. However,
47 Panel D
generate coherent light pulses, as short as (or even functions of the number of atoms). These originate
shorter than) the incident pulse, with almost any from cluster shape deformations similar to the Jahn-
central frequency. Coherent control provides the Teller distortions familiar in molecular (and nuclear)
capability to probe and understand, at the most physics. Such clusters possess collective excitation
fundamental level, the making and breaking of spectra (giant photoabsorption resonances), and they
chemical bonds in addition to enabling the production fission upon multiple ionization.
of novel product states of the quantum system. This
can mean the generation of new chemical compounds, The adaptation of AMO physics methodologies and
the establishment of more efficient routes to desired their application to clusters and nanocrystals, in
reaction products or even the construction of particular conjunction with computer-based (time-dependent)
structures of the product molecules. This technology first-principles molecular dynamics simulations, could
has applications beyond the modification of molecular contribute significantly to elucidation of the above-
collision dynamics, such as the generation of Rydberg mentioned phenomena. Work in this area also bears on
wave packets in atoms and the control of current flow problems pertaining to: supershells and semiclassical
in semiconductors. descriptions (using periodic-orbit theory) of electronic
spectra for larger clusters; multiple charging (shape
Nanoscale Materials: Clusters, Nanocrystals, resonances), basis-set selection and correlation effects;
and Dots single-particle and collective (plasma) excitations;
atom (or ion)-cluster and intercluster collision
Investigations of the microscopic physical origins
dynamics, product branching ratios, and collisional
underlying size-evolutionary patterns of materials
energy redistribution; cluster and nanocrystal growth
properties are among the main themes in modern
mechanisms; cluster thermodynamics (structural and
condensed matter physics and materials science.
phase transformations); magnetic properties; dipole
These studies are enabled by the emergence of novel
(and higher multipole) excess electron binding to
experimental probes and by the development of new
molecular clusters [e.g. (H2O)n , n>2] and solvation
theoretical and algorithmic approaches. Coupled with
energetics and dynamics; and size-dependent
the availability of high-powered computational tools,
reactivity. These studies could lead to formulation of
they allow deep insights into the structure of matter
atomic-scale principles to guide the controlled design
bridging the atomic, molecular, and condensed-matter
and preparation of nano-scale materials with
regimes. In addition to their basic scientific
prescribed size, shape, property, and functionality.
significance, the above issues form the scientific base
for technological developments, particularly in the
Another class of novel 0D nanoscale structures, with
area of device miniaturization.
close analogies to atomic systems, consists of confined
(2D) electron gases in the form of dots. These are
Atomic material aggregates with nanometer-scale
often referred to as “super-atoms”. Both basic science
dimensions exhibit certain properties analogous to
and technology will be advanced by development of
those found in other “zero-dimensional” (0D) systems,
an understanding of the electronic level structure, of
namely atoms and nuclei. Most prominent among
the excitation spectra (both single-particle and
these is the electronic shell structure of small
collective resonances), and of the charging properties
(metallic) clusters. At shell closures this leads to
in such systems. The improvement of theories beyond
enhanced stability and self-selection of clusters having
the mean-field approximation is essential, both under
“magic numbers” of atoms. Moreover, other
field-free conditions and under the influence of an
properties such as ionization potentials, electron
applied magnetic or optical field.
affinities, and single-atom detachment energies of
open-shell clusters exhibit odd-even alternations (as
Panel D 48
Atom Interferometry and Lithography are far larger than atomic dimensions and in which
collision times are longer than atomic radiative decay
Atom optics has shown promise in recent years, both
times. Atomic collision cross sections are dependent
for the fundamental interest it has generated and for its
on long-range atom-atom interaction potentials. At the
technological promise. Atom interferometry has
lowest energies, hyperfine interaction effects must be
progressed beyond the demonstration of basic two-
included. Acquisition of a deeper understanding of
and multi-slit interference patterns used as textbook
these cold collisions is crucial to the control and
illustrations of quantum mechanics. It can now be
application of BEC phenomena, to improvements in
used as a tool to measure atomic properties including
the precision and stability of atomic clocks, and to
the phases of quantum amplitudes in addition to their
enhancements in the sensitivity of experiments to
magnitudes. The future applications of these
detect small effects and to make precision
interferometric techniques are hard to envision fully at
measurements.
this time, but they will certainly probe the quantum
mechanical ideas of entanglement, coherence, and
Ultra Intense Fields
decoherence. Experimental work in this area would
benefit from theoretical studies, particularly when At laser intensities greater than about 1012 W/cm2,
noise and dissipation play an important role in the nonlinear laser-atom effects (e.g., above threshold
interference structures. ionization, high harmonic generation, etc.) become
increasingly prominent; above about 1019 W/cm2, the
As technologies continue to improve for handling electric field in the laser light—rather than the nuclear
phase-coherent atomic beams of small dimension, so Coulomb field—controls electronic motion and the
will the ability to lay down atoms on surfaces in induced electron velocity becomes relativistic; above
prescribed arrangements. The continued development about 1029 W/cm2, the laser field is strong enough to
of these novel lithographic techniques is likely to have “spark the vacuum,” i.e., to create electron-positron
far-reaching application to microchip production and pairs. The theoretical description of such phenomena
nanoscale fabrication. requires a non-perturbative treatment of the laser-atom
interaction and, often, a time-dependent solution of the
AMO PHYSICS IN EXTREME quantum equations for the laser-induced electronic
CONDITIONS motion. Prominent among possible applications is the
use of high harmonic generation to produce coherent
The theoretical description of AMO phenomena under sources of VUV and X-ray radiation.
extreme conditions generally requires the development
of appropriate (and often new) theoretical approaches. Ultra Short Pulses
Advances in experimental technologies have permitted
The development of laser pulses as short as 5 fs is now
measurements covering a broad range of such
possible, and shorter pulse durations are on the
phenomena, thus providing the opportunity for theory
immediate horizon. Pulses this short permit excitations
and experiment to progress together. Many of these
of localized electronic or vibronic wavepackets in
opportunities have significant applications to energy-
atoms and molecules. The theoretical description of
related technologies. The following are some of the
the electronic dynamics requires a time-dependent
leading opportunities:
approach. Furthermore, additional coherent, short
laser pulses permit one to control the evolution of the
Ultra Cold Collisions
system. Analysis of the wavepacket motion in atoms
At sub-milliKelvin temperatures, atom-atom collisions or molecules has important applications. In Rydberg
enter a new regime in which de Broglie wavelengths atoms, theory can explore the connections between
49 Panel D
classical and quantum behaviors. In molecules, a goal methods, but analyses using detailed quantum
for theory and experiment is to develop robust calculations are largely incomplete. This is true not
methods for controlling the evolution of the only for many-electron systems but also for simple
probability density along particular desired Born- systems at low velocities. A difficult challenge for
Oppenheimer pathways. quantum theory is to develop methods that go beyond
the independent particle model for reactions involving
Ultra High Resolution and Detection Sensitivity multiple electron transitions. Often these many-
electron transitions are dominated by the dynamics of
Lasers and third generation synchrotron light sources
electron correlation, which is a key to understanding
are permitting atomic and molecular spectra to be
mechanisms for energy transfer in complex atomic
observed with unprecedented resolution and
systems. The general question is how to understand
sensitivity. Energy resolutions of 1 meV and better are
complex systems (including large molecules or
becoming available in the 100 eV photon energy
nanostructures) in terms of simpler atomic systems.
range; while this does not translate into a “resolution”
figure as impressive as can be achieved with state-of-
Ultra Fast Collisions
the-art CW laser systems, it is a major step forward in
the high energy regime. Cross sections as small as An example of a highly localized conversion of energy
hundredths of a barn are being observed. In molecules, occurs in interactions of relativistic ions with atoms in
vibrational and even rotational energy levels can now which electron-positron pairs are produced.
be resolved even in some synchrotron experiments. In Calculations have not yet been able to give a reliable
atoms and in atomic negative ions, such high energy interpretation of the spectra observed, in which it is
resolution and sensitivity requires theory to transcend believed that disruption of the negative energy sea has
the independent-electron model to incorporate many- occurred.
body correlation effects, as well as the effects of
normally feeble interactions (e.g., polarization effects, Ultra High Photon Energies
spin-orbit and other relativistic effects). In molecules,
Another window of opportunity is being opened by
theory at an elementary level has not been widely
new third and fourth generation synchrotron radiation
applied, even for relatively small systems.
facilities. These facilities are just beginning to
Photodetachment of negative ions leads to spectra
produce data useful in both the gaseous and condensed
dominated by correlated two-electron resonances, with
phases of matter. For example, Raman emission by x-
spectral patterns very different from the one-electron
ray scattering is being used to determine composition
Rydberg series omnipresent in neutrals. Knowledge
of materials used in new semi-conducting devices.
about such resonance features is essential for a number
Interpretation of these experiments requires a theorist
of energy technologies, such as in the design of gas
to consider both atomic and condensed-matter issues.
lasers, arcs, fluorescent lamps, and high-power
The development of a microscopic understanding of
discharge switches, because resonances affect the
the effects of high energy photons that penetrate matter
conductivity of a low-temperature discharge and
requires us to unravel multiple ionization and
plasma environment.
excitation events produced by x-rays, both in
photoionization and in Compton scattering. Cross
New experimental techniques hold promise also in
sections and reaction rates for these processes are
collision physics as they allow more detailed analysis
dominated by the concerted motions of non-
of chemical kinematics and reaction dynamics. One
independent electrons, and photons probe the electron
such technique is cold target recoil ion momentum
correlation dynamics cleanly. Sorting out such
spectroscopy (COLTRIMS). Analyses of data
processes could help us to understand how to modify
obtained with this method have used classical
Panel D 50
or control site-specific reactions in more complex whose total energy is several electron volts per atom
chemical and biological systems. higher than the ground state. In other words, the
condensate, despite being ultracold (50nK)
NOVEL STATES OF MATTER AND translationally, stores a surprisingly high density of
LIGHT internal energy since about 106 atoms are confined to a
volume of order 10-18 m3. Another type of proposed
Bose-Einstein Condensation (BEC) and atom
condensate consists of helium atoms in metastable
lasers
electronic states; if experiments succeed in forming
Interest in AMO science intensified in 1995 following such a condensate, the amount of energy stored per
the first experimental observation of BEC for a dilute atom would be increased by nearly an additional order
gas of spin-polarized alkali-metal atoms. The ensuing of magnitude. Should future research demonstrate
excitement has had few parallels in the physical ways to achieve the controlled release of this energy,
sciences. Experimental laboratories worldwide e.g. through an “output transducer,” this could be an
quickly initiated their own attempts to reproduce the important source of coherent atoms. Such a phase-
first experiments, and at last count six independent coherent beam of atoms was demonstrated earlier this
groups had achieved BEC. While the initial year at MIT, and has been called an “atom laser.” The
observation was primarily an experimental atom laser beam is qualitatively different from an
achievement, theoretical studies have since played a ordinary incoherent atomic beam, and is likely to
key role in the continued growth and excitement of the spawn spectacular capabilities for lithography and
field. BEC theory is now a high profile activity atom interferometry in the coming decade.
represented in some of the best physics departments, ·
and is carried out by both condensed matter and AMO Quantum Optics
theorists. This subject has already spawned extensive
Entanglement: Quantum optics brings fundamental
interdisciplinary interactions that extend our
quantum mechanical theory to bear on thought
understanding of the many-body problem from the
experiments that have recently been realized
perspectives of both fields. Fundamental questions
experimentally with the advent of high-precision
arise relating to: the mechanisms of spontaneous
cavities and state-specific control of atomic states
symmetry breaking and the formation of coherence;
through stable, tunable lasers. Micromaser cavities
phenomena such as superfluid flow and persistent
with exceptionally high Q-factors provide photon
currents; specific heat and critical temperatures; first
traps, analogous to particle traps, which are used to
and second sound waves and excitations; the kinetic
localize injected photon fields. These fields are
and dynamic evolution of the condensate.
typically tunable over a wide range of frequencies near
resonance between two atomic levels of interest, e.g.,
This panel believes that theoretical efforts to
alkali Rydberg levels. The passage of one or more
understand BEC will help to unravel a number of
atoms through such a cavity leads to an entanglement
issues that need to be better understood such as: the
of the atom with the cavity, which can then be probed
energy spectrum of this many-body condensate; its
by a second atom, which in turn becomes entangled
formation and decay mechanisms; its coherence
with the first atom. Alternatively, two cavities can be
properties; the variety of novel forms in which it can
entangled with one another via the passage of a single
be created. A key question concerning its possible
atom, which might transfer a photon from one cavity
relevance to DOE interests arises from the simple
to the other. All of these coherent processes are
energetics of BEC. What is usually termed the “ground
manifestly quantum mechanical in nature, as is
state” of the condensate is not actually the true ground
revealed dramatically when the states are correlated
state of this many-body system; it is a metastable state
51 Panel D
with macroscopic detectors. Note that the use of have interesting and anomalous statistical properties.
explicitly nonclassical light fields (i.e. squeezed states) Experiments on lattices of light that confine atoms in a
for high-precision frequency metrology is presently three-dimensional array of optical potential wells are
funded in the DOE Atomic Physics Program. important for precision measurements.
Related fertile areas include:
Antimatter and exotic species
Dissipation theory: A central theme in quantum optics
Experimentalists and theorists have recently studied
has been the development of powerful theoretical
the spectroscopy of antiprotonic helium. Efforts
methods that can efficiently handle irreversibility in
continue toward creating antihydrogen at low energies
nonrelativistic quantum mechanics. These include
for tests of fundamental physics. A dedicated
quantum Monte Carlo and quantum trajectory methods
antiproton storage ring is being built at CERN, which
in which the continuous evolution of the Schroedinger
will enable the collection of antiprotons in a Penning
equation is disrupted by quantum jumps of the state.
trap. As these experimental capabilities leap forward,
The concepts are general and diversely applicable in
the branch of atomic physics concerned with the
quantum mechanics. In many-state simulations they
structure and collisions of exotic particles at low
are far more efficient than the more standard “master
energies has many opportunities and challenges, in
equation” techniques.
which theoretical contributions are essential.
Enormous amounts of energy could be stored in the
Quantum computing: When the usual binary logic of
form of antimatter, if its creation and manipulation
computation is modified by quantum mechanically
advances tremendously beyond present-day
entangling two states, this leads to exponential gains in
capabilities, though this appears too remote to serve as
computation speed for certain important problems. The
a goal for the immediate future.
experimental difficulties arising from decoherence for
realizing a quantum computer are formidable, but the
potential gains are extremely high. Proposals for EXTENDING THE FRONTIERS
quantum error correction, transfer and cloning of Time-Dependent Real-Time Dynamics
quantum states, quantum communication, and
The dynamics of quantum systems can often be
quantum cryptography are all interesting by-products
described directly in the time domain. This approach
of this research. It has been shown that arbitrary
provides accurate product-state distributions over a range
quantum states can be engineered, and using recently-
of total energies from a single calculation. When coupled
developed tomographic methods, experiments can
with modern visualization tools, it can provide key
characterize these states completely.
insights into the underlying mechanisms. For many
processes this is the only practical formulation, especially
Laser cooling and atom optics: The interaction of
in cases for which the number of open channels is very
atoms with the electromagnetic field allows trapping
high (e.g. when three-body continua are present) or
and cooling and to create optical elements such as
where the Hamiltonian for the system is explicitly time-
beam splitters and mirrors for matter-wave
dependent (e.g. when an intense laser pulse is applied).
interferometers. There have been tremendous
For even the simplest systems this approach can require
experimental advances in laser cooling techniques
very substantial computational resources. Utilization of
over recent years with the lowest temperatures given
large multi-processor computers has allowed the
by dark state cooling in which the coldest atoms
investigation of many phenomena for simple systems
become decoupled from the field through a destructive
that are central to the missions of the DOE. Many of the
internal interference of the absorption amplitude.
currently-used methods solve the time-dependent
Atoms cooled in this way undergo Levy flights and
Schroedinger equation iteratively—a scheme that is
Panel D 52
ideally suited to parallel architectures. The complexity of binding of an electron to heavy atoms with closed
problems that can be addressed in the future is contingent subshells; the escape of two or more electrons
upon the development of efficient algorithms that following absorption of a single photon; collective
maximize the division of labor among numerous fast excitations of two-electron resonance states.
processors. Problems that have been successfully Numerous successes of this line of research can be
investigated include molecular dissociation by electron, identified. Theoretical capabilities have advanced
ion, or photon impact; inelastic and reactive atomic and tremendously, especially in the last few years. While
molecular scattering processes; atomic excitation and this field maintains a continuing interest in further
ionization by intense, pulsed laser fields. improving theoretical methods for even the simplest
atoms with only two or three valence electrons, we
An outstanding problem in this area is the study of focus here on new advances that are increasingly
multielectron systems subject to a time-dependent desirable. This is truly a frontier, a theoretical subfield
interaction: either a collision or a pulsed electromagnetic that remains, comparatively speaking, in its infancy:
field. Even for two electron systems, there are many the description of electron correlation effects in bound
problems that have not yet been solved. The and continous spectra where relativistic effects are
independent-particle approximation often fails important. This includes mainly the atoms heavier
dramatically in a time-dependent problem, and is thus than, say, Kr (Z=36), as well as diatomic and triatomic
inadequate. Resources and numerical methods are molecules containing one or more of these heavy
presently being developed that should eventually permit atoms.
an accurate numerical solution of the full-dimensional
two-electron problem for a number of non-trivial In the atomic realm, the most commonly-used
regimes. Among these is the surprisingly strong approaches start with the Dirac-Coulomb Hamiltonian,
simultaneous double ionization of helium by a short and a multiconfiguration Dirac-Fock wave function
pulse optical laser field: interpretation of these expansion which, in the case of fixed basis set
experiments continues to resist theoretical efforts. The methods can be obtained through configuration
calculations challenge our ability to solve the time- interaction (CI) calculations. Further effects can be
dependent Schroedinger equation, of course, but perhaps added perturbatively. Despite the ability to treat
of equal importance, they challenge our visualization aspects of the low-lying bound state spectrum for far
skills needed to identify the dynamical mechanisms that more complex open-shell atoms and negative ions than
operate. A desired outcome is that, based on the insight was conceivable ten years ago, roadblocks loom. To
gleaned from a solution of the dynamics for two- be sure, the spectra of these species are extremely
electrons in a laser field, a general improved technique complicated, especially in the lanthanides (currently
will be developed that can handle similar nonperturbative important for the lighting industry) and in the actinide
problems for multielectron systems. and transuranic elements (of continuing relevance to
the DOE environmental cleanup mission). For
Relativity and correlations in structure and example, in Lr (Z=103), theoretical investigations
dynamics have concentrated on the determination of the ground
state properties, but even the ionization energy is not
Two active research areas that have been traditionally
known accurately. The number of configurations that
addressed within current AMO theory projects in this
arise, even in the most constrained CI expansions,
program include electron correlations and relativistic
grows explosively in these systems with one or more
effects. The study of correlations aims broadly at the
open subshells. In fact, it is worth asking whether
derivation of theoretical tools capable of describing
calculations based on this methodology truly have a
numerous atomic phenomena that are beyond the
realistic hope of being able to calculate accurate
scope of the independent-particle approximation: the
53 Panel D
energy levels, photoabsorption and photoionization Quantum Mechanical Approximations Derived

oscillator strengths, dielectronic recombination, and from Semiclassical Methods
hyperfine and weak-interaction couplings, at a level of
A minor revolution has occurred during the past
precision that is spectroscopically useful. Multichannel
decade in the theoretical description of quantum
level perturbations are so rampant that it may make
systems with two or more strongly-coupled degrees of
sense to pursue the more limited initial goal of
freedom. The most exciting possibilities arise in
describing short-time spectra, i.e. the spectroscopy at a
systems whose classical Newtonian analogues are
comparatively coarse-grained energy resolution.
chaotic. Classical chaos arises when classical
trajectories are exponentially sensitive to initial
Many of these same bottlenecks arise in the theoretical
conditions. The quantum dynamics for such systems
description of a diatomic or triatomic molecule, of
is sometimes referred to as “quantum chaos.”
course. Additional complexities arise because of the
much greater difficulty of performing an electronic
Our panel has for the most part avoided a discussion of
calculation in a multicenter geometry, and with the
theoretical possibilities based on the merits of any
intimidating complexity of the nuclear dynamics on
particular “technique.” The semiclassical “quantum
nonadiabatically-coupled potential surfaces. In
chaos” methods devised by Gutzwiller, Berry, and
triatomics, conical intersections lead to all the
their followers seem to us worth singling out, however,
difficulties, e.g., of Jahn-Teller effects that modify the
because their new capabilities complement more
molecular symmetry one would expect based on fixed-
conventional schemes used by AMO theorists. In
nuclei calculations. Atom-diatom scattering
particular, new types of spectroscopies (such as scaled-
calculations can sometimes describe these effects with
variable spectroscopy) give deep insight into the origin
modest computational effort, and in a conceptually-
of short-time features in the “time domain” of the
appealing manner, by using geometric phases
observables such as photoabsorption cross sections.
appropriately. Moreover, while the construction of
Of course, short-time features translate via Fourier
bound-electronic potential surfaces and a description
analysis into global, coarse-energy features; this is
of the nuclear dynamics is a tremendous challenge,
often of greatest qualitative interest when an
one would like the theory to advance and develop the
experimentalist seeks an interpretation of a hopelessly
capability to treat electronic continua that arise in
dense spectrum of innumerable lines. Quantum chaos
photoionization, photodetachment, and electron
techniques interpret the main global features in terms
scattering processes. In the molecular realm, much
of a modest number of periodic classical orbits. The
remains to be understood even for molecules
new capabilities of such theories are deserving of
containing the first-row transition metal atoms, where
special scrutiny from this scientific community. Their
relativity can still be handled perturbatively.
full domain of applicability remains to be identified. It
is encouraging that for a class of problems involving
The research in this area requires extensive conceptual
Rydberg state dynamics in external fields, they have
and computational development. We believe that it is
provided unparalleled insights into the origin of the
poised to make tremendous strides in the coming
short-time spectrum.
decade, by coupling the deeper understanding we have
achieved in how to treat these types of bound and
For decades, applied mathematics has been exploring
continuum problems with the rapid improvements in
problems relating to the asymptotic distribution of
computational hardware and algorithms.
eigenvalues, a classical area in mathematics that has
been reinvigorated by periodic orbit theory. More
generally, theoretical atomic physics would also
Panel D 54
benefit from stronger interaction with the larger the presence of neutral and ionic molecules and
applied mathematics community. That community negative ions. Dust may be formed and will exercise a
contains expertise in areas of key relevance to atomic major influence on the characteristics of the plasmas.
physics, including differential equations, numerical The molecular composition is drastically modified by
methods, and asymptotic analysis. the production of metastable species and by the
vibrational excitation of the molecular species.
Low-Temperature Plasma-Related Research Important processes are dissociative recombination,
dissociative attachment, associative detachment,
The problems presented in understanding the physics
collisional dissociation, and chemical reactions
of high and low temperature plasmas lie at the
involving excited species. Few data are available and
forefront of atomic, molecular and optical physics.
for many of the processes no adequate theory has been
The behavior of plasmas is determined by a complex
formulated. The processes of dissociative
of interactions of a wide array of atomic, molecular
recombination (DR) of molecular ions with electrons
and optical processes involving electrons, ions, atoms
and charge transfer reactions of ions with molecules,
and molecules. The full characterization of many of
in particular, pose formidable theoretical challenges.
the processes that determine the nature of plasmas wait
For even some of the simplest diatomics (HeH+) and
upon advances in theoretical concepts and
triatomics (H3+), theory and experiment disagree about
developments in computational methods. Thermal
the near-threshold DR cross sections by more than an
fusion plasmas, inertial confinement plasmas and
order of magnitude.
plasmas designed to simulate weapons effects are hot,
with temperatures approaching one million to ten
Present models of plasmas contain only a limited
million degrees. Similar hot plasmas occur naturally
description of the processes and are based on
in the solar corona, in supernova remnants and in gas
unreliable data. With anticipated advances in collision
surrounding cosmic X-ray sources. The behavior of
theory for complex systems and access to enhanced
high temperature plasmas is determined by ionization,
computing capabilities, it will be possible to identify
recombination and excitation processes. The
the critical processes, to calculate their efficiencies and
efficiencies of many of the processes can be calculated
to construct models that can be used to guide the
by the application of methods that have been already
design of low temperature plasmas for specific
developed and tested. For others, and particularly for
applications.
systems of high nuclear charges, further development
is needed that takes fully into account relativistic
Ion-Atom and Ion-Molecule Collisions
effects. Using the data, computer-based models that
simulate the behavior of the plasmas can be New data are becoming available for many different
constructed. The plasma properties can then be kinds of reactions. As the possibilities of observing
explored over a wide range of conditions of density, transitions and reactions in many-electron systems
temperature and radiation environments and diagnostic grow, so do the difficulties of finding which studies
probes can be designed. will provide the best insight into the nature of
dynamical processes in complex systems. In these
Lower temperature plasmas are created for cases theory can often provide guidance in selecting
manufacturing purposes in the lighting and plasma reaction details most crucial to understanding
processing industries. They occur naturally in the mechanisms for dynamics in complex systems. A
ionospheres of the planets, in lightning discharges in challenge in the field of collisions is to unravel
the terrestrial atmosphere and in the interstellar reaction mechanisms among many-electron atoms,
medium. The behavior of cooler plasmas with molecules, clusters, and surfaces, including instances
temperatures below about 5000 K is complicated by in which perturbation techniques fail. In this field
55 Panel D
experiments carried out at ion storage rings have use of such tools pervades the entire AMO community.
provided critical data at unprecedented resolution for a Many AMO codes (RMATRIX, MCHF, GRASP, and
number of electron-ion recombination and collision Cowan’s suite of programs) have been developed and
processes. This is an area in which the United States used by theory groups, but little attention has been
has fallen significantly behind development in Europe. given to making them user-friendly and readily
Smaller, less expensive, “table-top” storage rings, accessible to experimentalists. Other communities
which should be available soon, provide an important such as the chemistry community have begun to make
opportunity for U.S. science to explore many of these this transition. Here, quantum chemistry codes such as
topics. GAUSSIAN, GAMES, QCHEM and others have been
become the every day tools of organic and inorganic
OPPORTUNITIES AND HORIZONS IN chemistry. Few similarly-accessible tools exist for the
HIGH-PERFORMANCE COMPUTING interpretation of experimental results for a wide range
of problems that involve dynamics, such as electron
Progress in this century in atomic, molecular and collisions, photoionization, and molecular and ionic
optical theory has placed the field in an enviable collisions. With the advent of new DOE national
position to make accurate predictions about experimental facilities such as the Advanced Light
fundamental processes. However, for the complex Source and the Advanced Photon Source, the need for
systems and processes of increasing relevance to this such tools and for closing the gap between theory and
field, the impact of theory on experiment can be experiment is more urgent than ever.
increased dramatically through use of the most
powerful modern computers and computing
techniques. The significant increase in performance
provided by such computers will enable AMO theory
to address fundamental processes in more complex
systems. Furthermore, as many branches of AMO
theory make the transition to parallel computing,
within a decade the applications developed for today’s
massively parallel computers will be running on
widely-available laboratory-scale multiprocessors.
The accurate theoretical description of collisions

among electrons, ions, atoms, molecules, clusters and
surfaces cannot be achieved without this scale of
computation. Such advances will allow us to predict
the rates of the many important collision processes and
to construct simulations of the low-temperature
plasmas used widely in processing materials. They will
also permit studies of bound and continuum states of
heavy elements and of new phenomena occurring in
complex systems in intense fields. A further impact of
high-performance computing is the opportunity to
make the computational tools of modern theory more
accessible to the experimental community by moving
beyond the “grand challenge” stage to the point where
Panel D 56
Panel E: Nano- and Mesoscopic Structures
Chair:
Paul Alivisatos (Lawrence Berkeley National Laboratory)
Panelists:
Daniel Chemla (Lawrence Berkeley National Laboratory)
Vicki Colvin (Rice University)
Robert Compton (University of Tennessee)
Therese Cotton (Iowa State University)
James Heath (University of California, Los Angeles)
Mark Knickelbein (Argonne National Laboratory)
Charles Lieber (Harvard University)
Paul McEuen (University of California, Berkeley)
Horst Schmidt-Boecking (Universitat Frankfurt)
Stanley Williams (Hewlett-Packard Laboratories)
Solids of nanometer scale exhibit strongly size chemical behavior of the particles. Thus, nano-scale
dependent chemical and physical properties which building blocks lend major new experimentally
represent limiting behaviors for different types of controllable variables for fabricating desired materials.
matter (atomic to bulk). The variations with size are In the last decade, it has been possible to fabricate
enormous, and this represents a new opportunity to nanostructured materials at a level where they now
optimize material properties by varying their size and compare in quality to the high performance solids and
shape rather than by changing their chemical thin films used in the electronics industry. A partial
composition. The developments in nanoscale science list includes highly monodisperse colloidal metal and
are of a sufficiently fundamental nature that we can semiconductor nanocrystals, STM-assembled
anticipate the development of this field will “quantum corrals,” molecular beam epitaxy grown
significantly impact several other disciplines of basic self-assembled quantum dots, laser ablation and cluster
science and will also help address key energy related beam expansions, electric discharge growth of carbon
technologies. tubes and clusters, thermal flow reactors, rapid
pyrolysis, as well of course as e-beam and x-ray
Advantages and Challenges of Nanometer Scale lithography. Atom manipulation, and matter
Science and Technology diffraction from light waves, are important new tools
emerging from atomic and optical physics which may
The ability to shape and control matter on the
lead to new ways of fabricating nanostructures.
nanometer scale offers a tremendous number of
established and potential advantages, but to fully
Despite the wide range of fabrication methods, a high
exploit this area there are a number of critical issues
degree of structural perfection is often observed in
that must be addressed over the long term. In this
nanostructures, and this can be attributed to several
section of the report, we discuss both the major
factors: In a bulk single crystal, it is impossible to
advantages that nano-scale based systems offer to new
remove all defects. In a nanostructure, the high
and/or improved technologies, as well as the major
surface area provides a route for the annealing and
questions that surround the development of any such
removal of defective sites on short time scales. Related
new technologies.
to this is the fact that the melting temperature of solids
is substantially reduced in finite size, which allows not
The primary advantage of any nanostructured material
only for the fast diffusion of defects, but also for
lies in the extensive tunability of its properties. For
growth schemes at surprisingly low temperatures.
example, the physical and chemical characteristics of
Thermodynamically, the probability of defect
materials have traditionally been determined by the
formation dictates the fraction of atoms likely to be in
chemical stoichiometry and structure of the material.
defect sites; when the total number of atoms in the
However, by controlling the size and shape of a nano-
system is small, this number approaches zero. These
scale solid, many of the physical and chemical
arguments suggest that the manufacture of
properties of the system can be tuned over a large
nanostructures can be done very cheaply, with simple
range. For example, the fundamental characteristics of
processing. This makes nanostructures extremely
a material, such as its melting temperature, color,
attractive candidates for a host of technologies.
saturation magnetization and coercivity, charging
energy, chemical reactivity, etc., are all a function of
As the quality and variety of nanostructures has
size and shape. For instance, the color of
improved over the last decade, many new
semiconductor quantum dots can be varied
technological applications have been envisioned. This,
continuously from the near infrared to the ultraviolet.
in turn, has raised several questions related to the
Such color changes correlate to electron and hole
integration and performance of nanostructures in
energy levels, which in turn affect the catalytic and
Panel E 58
various technologies. First, can sufficient quantities of An isolated nanometer scale object such as a
high uniformity nanostructures be made to enable nanocrystal or a nanotube can be viewed as an
technological applications? All current fabrication artificial atom, possessing a well-defined charge state
schemes operate on a typical laboratory scale (ranging and energy level structure. Unlike real atoms,
from 1 monolayer to 1 gram). Second, one of the however, the size, shape, properties, and local
advantages of nanostructures is that they are environment can be controlled and adjusted. As a
characterized by a very high surface area. However, result, nanostructures are ideal model systems for
this also makes interface characterization and control exploring the physics of small quantum systems.
imperative. Opportunities for the development of new
spectroscopic and imaging tools exist here. There is as The electronic structure of the delocalized electrons in
yet no tool available to determine the bond lengths, a nanostructure can be continuously tuned by adjusting
angles and reconstructions of nanoparticles, as exists the size of the object. This shifts the absorption and
for plane single crystal surfaces. Third, many emission spectrum from the bulk material and results
envisioned applications require nanostructures to be in discrete lines. Further, the charge state of the
placed into chemically and/or structurally complex nanostructure can be tuned using a voltage applied to
environments – i.e. around other nanostructures, an external electrode, continuously adjusting the
connected to electrical devices, in chemical sensing ionization energy of the artificial atom. Finally, the
environments, etc. The assembly of nanostructures shape can also be adjusted. For example, 3D spherical
into specific architectures is a challenge that is just nanocrystals, 2D disc shaped quantum dots, and 1D
now beginning to be addressed. Fourth, the chemical rod-like molecules are currently under study to
and thermodynamic stability requirements for investigate the energy level structure of systems of
nanostructures will vary from application to different dimensionality. This tunability makes
application. This issue remains largely unexplored. possible the systematic investigation of the relative
importance of Coulomb interactions and quantum
Nanostructures are extremely promising new confinement effects in small quantum systems. It also
materials, with significance for both basic and applied makes possible the creation of artificial quantum
science. Although the field of nanostructures is young, systems with properties that are specially chosen for a
it is already possible to identify key areas in which specific scientific application. This ability to control
nanostructure science must evolve for the field to the electronic structure is of considerable interest from
reach its full potential. At present time, none of the the point of view of interaction of light with matter
questions discussed here appear insurmountable. and quantum optics. The non-linear optical properties
and the question of electronic coherence in dot excited
Impact of Nanoscience on Fundamental states are particularly related to developments in
Problems atomic and optical physics. For example, dots are
possible candidates as qu-bits in quantum
Nanostructure studies are most often described in
computation.
terms of their potential technological impact, to the
point where it is a field often referred to as
The artificial atoms can also be assembled into
nanotechnology. Yet the ability to control matter on
artificial molecules and solids, and the properties of
the nm length scale can be expected to have important
this solid can be controlled. In particular, the level
consequences for fundamental studies in disciplines
structure of the individual nanostructures, their
ranging from condensed matter theory, to solid state
charging energy, their Coulombic and tunnel coupling,
chemistry, to materials science.
and their coordination can all be tuned. This is
tremendously important for understanding the
59 Panel E
behavior of interacting electrons in reduced the strength or structural metastability. In bulk

dimensions, which is probably the central task facing systems, these properties can be influenced by
condensed matter physics. From high temperature defects. The ability to create perfect materials makes
superconductors to Luttinger liquids, the non-Fermi measurements of the intrinsic, i.e. defect free,
liquid ground states that are believed to occur in 2D properties possible. The mechanical properties of
and 1D interacting electron gases remain poorly ultrasmall structures are also of fundamental interest,
understood, both due to a lack of tunable experimental e.g. size quantization of phonon modes and quantum
systems and their intrinsic theoretical difficulty. The “mechanical” oscillators. A new field of
optical, electrical, and magnetic properties of such nanomechanics is emerging that explores the physics
structures will be of great interest. and technology of mechanical structures at this scale.
Nanoscale materials provide many opportunities for The Role of Theory

improved understanding of basic chemical processes.
Theory plays a central role in the description of the
The study of chemical reactions occurring on and
structure and dynamics of nanostructures as well as to
within nanoscopic objects such as clusters, dots and
predict the growth of such materials, and can help to
nanotubes provide a unique opportunity for examining
guide experiment. In turn, nanostructures provide an
the effects of reduced dimensionality. One example
important proving ground for new theoretical
with environmental implications involves the study of
developments. The ability to describe complex
chemical reactions of atmospheric pollutants within
systems is of particular theoretical interest, and the
water nanodroplets and on the surface of ice
evolution with size of nanostructure properties
nanocrystals. A second example concerns our
provides a heirarchy of complexity.
understanding of solid state chemistry. Solid state
synthesis is generally thermodynamic, largely because
The theoretical description of isolated nanostructures
mechanistic thinking is difficult to implement in
is just beginning. Vastly different computational
inhomogeneous solids with defects present.
methods such as ab initio quantum chemical
Nanostructures provide the opportunity to prepare pre-
calculations, density functional theory coupled with
assembled, multi-component single grains, in which
molecular dynamics, and simple tight binding
the kinetics and mechanisms of solid state processes
approximations all yield electronic ground and excited
can be independently measured and controlled. The
state energy levels for neutral and charged isolated
studies of metal cluster nanosurfaces provide an
nanostructures. In some cases the applications of
opportunity to examine intrinsic (electronic of
semi-empirical methods combined with experimental
geometric) size effects on surface reactions of catalytic
benchmarks can be used to generate useful predictions
importance such as Fischer-Tropsch synthesis and
of a wide range of related structures such as
hydrodesulfurization. The newly developed ability to
functionalized nanoparticles. The issue of predicting
put stable molecules as well as molecular coreactants
equlibrium structures, including geometry
in finite cluster solvents, and in liquid helium
optimization and surface reconstruction including the
nanodroplets opens the possibility performing
presence of ligands or other interface atoms is
spectroscopic and reactivity studies at temperatures
particularly important. A number of theoretical
below 1K.
methods can be applied to the mechanisms and
kinetics of nanostructure growth. The calculation of
Nanometer scale materials such as semiconductor
vibrational and electronic density of states as well as
nanocrystals and carbon nanotubes can be created with
polarizability and multipole moments can be compared
no defects. This allows for fundamental materials
with experiment. Of particular importance is the
science studies of the properties of pure materials, e.g.
prediction of magnetic properties of nanostructures.
Panel E 60
The effects of geometry changes and external stress on benefit of the ease of processing of molecules.
these properties is of interest. Composites of inorganic nanoparticles with organic
polymers are of particular interest in this category, and
The physical and chemical mechanisms whereby every type of device mentioned above has been
nanostructures, for example quantum dots, are coupled demonstrated in composites
to the environment and to each other are of great
interest. Properties such as electron transfer rates A bit is a physical entity, and there is an energy cost
between quantum dots, artificial solid band structures associated with information storage and manipulation.
and collective excitations in coupled dots need to be In the past 25 years the energy efficiency and
addressed. There are many questions regarding the consequently the speed of computation per input
interactions of dots coupled to the environment. power have increased by a factor of ten thousand.
Empirical potentials for dot-dot and molecule-dot Silicon integrated circuit technology should be able to
interactions together with the long range forces deliver another factor of one hundred increase before it
responsible for the assembly of dot arrays are reaches technological limits. However fundamental
importance. Of equal importance is the chemical physical limits indicate that computers can improve
reactions occurring at dot surfaces. another factor of ten billion in energy efficiency. To
approach the thermodynamic limit it will be necessary
Relationship to Energy Technologies to construct computers from nanostructures and
several possible models for subsystems already exist.
Almost every basic energy related technology may be
Computing will benefit tremendously from the
impacted by developments in nanoscale science.
combination of decreased energy consumption,
These include: chemical technology, energy storage
increased speed, and enormous storage increases (x
and manipulation, information storage and
1010) that will be enabled by nanostructures.
manipulation, and structural and mechanical materials.
Magnetism is fundamentally different in nanosize

Catalysis inherently relies on nanoscale components
grains, which act as single domains. If the shape and
and can be expected to benefit greatly from the ability
arrangement of magnetic nanostructures can be
to rationally control the size and shape of components
controlled, this will have uses in magnetic storage and
with precision and to spatially organize the
sensors.
components. Nanostructures are also exquisitely
sensitive to changes in their chemical and physical
Nanoscale building blocks tend to spontaneously
environment, making them strong candidates for
exclude defects. As a consequence, the structural and
sensor elements; for this to be realized issues of
mechanical properties of the individual components
selectivity and amplification these must be addressed.
and of their assemblies are quite distinct from those of
Nanostructures also provide a model system for
extended solids. The striking example of this is carbon
studying reactions on aerosols, which in turn are
nanotubes which appear to be the strongest fiber ever
important for understanding atmospheric chemistry
discovered. Nanostructure composites with well
and pollution remediation.
defined architectures will have unusual and desirable
mechanical properties.
Photovoltaics, light-emitting diodes, batteries, fuel
cells and capacitors are some of the energy storage
Relationship of AMO Physics to Nanoscience
and manipulation technologies that may benefit from
the high surface to volume ratios provided by Atomic, molecular and optical physics has contributed
nanostructures. Nanostructures have the desirable greatly to the development of the emerging field of
physical properties of solid systems with the added nanoscience. Nanostructures and clusters, in fact,
61 Panel E
represent a “bridge” between the isolated atom or Nanostructures provide templates for the first detailed
molecule to the condensed matter state. Following the studies of multiply charged negative ions.
development of nozzle-jet expansions for the
production of gas phase clusters, many AMO scientists Many developments in optical physics may impact
have contributed to our understanding of such diverse nanoscience. As one example, the “holy grail” of laser
phenomena as solvation, the hydrated electron, chemistry is to coherently control the products of
chemistry of nanosurfaces, etc. More recently, the reactions by the application of shaped optical pulse
assembly of nanostructure materials at the sequences. This is a very active research area. It is
macroscopic level has produced a heightened level of possible that advances in this field could contribute to
interest in the AMO community. Many of the the “assembly” of nanostructured materials, or to the
traditional techniques inherent in AMO physics are manipulation of electronic coherence in quantum dot
being directly applied to the study of nanostructures, molecules and solids. The interaction of intense
e.g. mass spectroscopy, electron spectroscopies, optical fields with nanostructures is of interest.
photon spectroscopy, etc. In fact, the discovery of C60 Multiphoton ionization, and the measurement of
came about through the combination of a number of nonlinear susceptibilities as a function of the size are
these techniques: (1) laser ablation of graphite into a currently actively investigated. The ability to control
nozzle jet expansion, (2) laser multiphoton ionization size may provide more insight into the differences
of C60 followed by (3) time-of-flight mass between atoms and molecules in their non-linear
spectroscopy. In addition to these standard responses.
techniques, there are a number of new advances in
AMOP techniques which might be important to the It is possible to reduce the size of electrically
development of nanostructure science: controlled macroscopic objects to sufficiently small
dimensions that the nanostructure can be manipulated
Many possibilities exist for transferring experimental by the application of an external electrical field, e.g. a
techniques from atomic physics to nanoscience. very high field applied between two neighboring
Recent developments of laser cooling of atoms might quantum dots can directly influence the reactions of
be applied to the partial cooling of nanostructures. these quantum dots with their neighbors or scattered
The ability to cool these clusters would lead to a better projectiles. In such strong fields, collisions of atoms
interpretation of their spectroscopy. It is also or molecules with the nanostructures might allow
conceivable that such cooling could lead to new electron transfer from the quantum dot to the colliding
molecular states of matter. atom or tunnel directly to vacuum states. Such
enhanced electron emission processes might find
The study of the ionic properties of nanostructures applications in, for example, electron-induced
represents an exciting new field for AMO physics. catalysis, air pollution abatement, etc. By varying the
Many of the ionization processes operative in size, geometry, and external field one may also obtain
nanostructures do not occur on the atomic or direct information regarding the energy levels of
molecular level. For example, the ionization of nanostructures.
clusters such as C60 occurs through surface plasmon
excitations. The production of new “super atoms” Traditional electron, ion, atom, etc. beams can be used
such as metal endohedral fullerenes will afford studies to excite or even fragment these nanostructures to
of energy levels of interest to solid-state determine their structural and dynamical properties.
heterostructures. The attachment of electrons to In addition, new atomic beam microscopies (e.g. cold
nanostructures represents a new field of physics in supersonic He beams or atom laser beams) could be
which techniques of AMOP are essential. used to study the topography and phonon structure of
Panel E 62
the surface. Using seeded supersonic cluster beams, or

possibly laser cooling, very cold nanostructures may
be created.
Cold atomic beams can create interference patterns of

atoms with order 100 nanometer resolution. In this
case, the AMOP techniques for producing such cold
beams are directly applicable to lithography.
Furthermore, using UV or even low energy x-rays
from synchrotron light sources, 3-dimensional
nanostructures or layers can be produced.
63 Panel E

Atomic, Molecular, Optical Physics Workshop: Final Report

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Atomic, Molecular, Optical Physics Workshop: Final Report

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Atomic, Molecular, and

of the workshop held

Preface ...................................................................................................................................................................... iii

Panel D: Theory of Structure and Dynamics ........................................................................................................... 45

Panel E: Nano- and Mesoscopic Structures ............................................................................................................. 57

Panel A: Interactions of Atoms and Molecules with Photons - Low Field

Panel B: Interactions of Atoms and Molecules with Photons - High Field

Panel D: Theory of Structure and Dynamics

Panel E: Nano- and Mesocopic Structures

Lloyd Armstrong, Jr., Chair

Panel A: Interaction of Atoms and Molecules

2. Advanced Spectroscopies with New Light Sources

3. Quantum Dynamics of Interacting Systems

Summary include studies of the basic physics of photon-

1. ATOMIC AND MOLECULAR Within the past decade a revolution in atomic

spectroscopy and that have been taken up by Opportunities include:

The energetic, spectroscopic and dynamical

• Extending these techniques to clusters. In high resolution frequency domain spectroscopy,

3B. Visualization of Quantum States and Scientific opportunities include:

• Developing methods that reveal correlations important. In addition, a quantitative

Advancing our understanding of the quantum

a. Comprehensive sets of dynamical parameters of

b. The interaction of highly charged atomic ions

I.B. Harnessing Quantum Dynamics

I.C. Matter in extreme conditions I.D. Reading List and References.

If the technical constraints of the target can be

II.B.3.2. What do we need?

As important as this is for future energy development,

II.C.3. Connections to Other Fields at DOE

Executive Summary comparable battery of techniques for control of the

Outline VI. Summary List of Basic Unsolved Problems

Interactions between ions and surfaces present new

clusters at surfaces. The energy levels and spatial B. Spatial Control

VIII. Conclusion Statement

Executive Summary the development of femtosecond lasers has brought

energy levels, photoabsorption and photoionization Quantum Mechanical Approximations Derived

The accurate theoretical description of collisions

behavior of interacting electrons in reduced the strength or structural metastability. In bulk

Nanoscale materials provide many opportunities for The Role of Theory

Magnetism is fundamentally different in nanosize

the surface. Using seeded supersonic cluster beams, or

Cold atomic beams can create interference patterns of

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