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Chemical
Dynamics in the Gas Phase
H.
Theoretical Kinetics Studies
Albert Wagner
Research Objectives
The goal of this program is to apply
and extend kinetics
and dynamics theories to reactions of interest in combustion.
Typically, the potential energy surfaces used in these
applications are determined from ab initio electronic structure
calculations, usually by other members of the group. Generally
the calculated kinetics or dynamics is compared to experimental
results, often generated by other members of the group. In
recent years, we have become interested in data reduction
problems that do not neatly fall into a kinetics or dynamics
category. It is expected that in the future, this component
might increase as we become interested in soot chemistry.
Approach
Dynamics and kinetics problems can be
approach by statistical,
classical trajectory, or quantum dynamics means. We have
used all three according to the problem under consideration.
In recent years, much of our development and application work
has focused on statistical kinetics theories of the flexible
transition state theory (FTST) type that are incorporated into
the code VariFlex which we distribute in collaboration with
S. Klippenstein (SNL), D. Wardlaw (Queens), and S. Robertson
(Accelrys Inc.).
Highlights of Recent Work
(November 1998 – November 2001)
Kinetics Studies
Electrostatic Effects in the Stabilization of HO2*.
In
collaboration with J. Michael in our group, we investigated
the buffer gas dependence of the low pressure limit of the
recombination of H with O2.
H + O2 «
[HO2]* ®
HO + O
¯ M
HO2
Recent experiments described by Michael
in his research
summaries confirm the observations of others that when M is
H2O, the recombination rate constant to form HO2
is an order
of magnitude higher than when M is a rare gas or N2. The
stabilization ability of M is controlled by two factors: the number
of collisions between M and [HO2]* and the average energy
transfer that results from each collision. Traditional approaches
to calculate the collision number when applied to this reaction
require outrageous or unphysical values of the energy transfer
between buffer gas and complex to agree with experiment. We
have explored a new approach to determining the collision
number by equating it to the thermal rate constant to recombine
M and HO2 as if they both were thermalized reactants colliding
under the influence of long-range electrostatic forces. This is
not to say that M-HO2 form a collision complex that lasts long
enough to influence chemistry but rather that the closeness of
approach required by complex formation is a good measure
of the kind of collisions that de-activate chemically activated
molecules. This approach is easy to implement with even high
order long-range electrostatic potentials. The central
approximation is similar to the work of others (e.g., I. Smith
at Birmingham) in estimating the high pressure limit of A+BC
by measuring the deactivation of A+BC(n=1).
The approach
compares favorably with the closest available trajectory
calculations (done by Lendvey (Hungarian Academy of
Science) and Schatz (Northwestern U.) on the collision number
for the stabilization of the chemically activated triatomic molecule
CS2*). In collaboration with L. Harding in our group, we have
calculated the dipole and quadrupole moments of HO2 and
found them comparable to those of water. Along with other
tabulated electrostatic information, we have used the code
VariFlex to systematically study M+HO2 "recombination"
in
the high pressure limit. For M=H2O, this amounts to an
electrostatic long range potential energy surface with R-3,
R-4,
R-5, and R-6 terms. For M=Ar, only the R-6
induction term
is present. The resulting collision numbers vary by about a factor
of five between H2O and Ar with H2O being higher.
(Traditional
estimates would have these collision numbers quite similar.)
These collision numbers along with realistic average energy
transfer parameters reproduce the kinetics measurements.
This study suggests that electrostatics forces are an important
component to energy transfer between polyatomics and many
radicals. Further trajectory studies are needed to more carefully
test the approximations in this approach.
The Initiation Reaction of O2+H2CO.
The reaction between
H2CO and O2 has been studied by J. Michael in our
group.
An Ab initio theoretical survey by L. Harding indicates
that
the process, H2CO + O2 ®
HCO + HO2, is the only possible
reaction. An ab initio kinetics study on the reaction has been
carried out at the canonical FTST level of rate theory using four
different potential energy surfaces generated by both L. Harding
and T. Truong (U. Of Utah). These four surfaces are: (1) hybrid
non-local density functional theory (DFT) using Becke’s
half-and-half (BH) non-local exchange and the Lee-Yang-Parr
(LYP) correlation functionals, (2) DFT using Becke’s original
non-local exchange with LYP functionals, (3) a DFT using the
Truhlar corrected functional (MPW1K) and (4) Coupled Cluster
Singles and Doubles with Triples excitation correction (CCSD(T)).
Basis set effects were explored by using both cc-pVDZ and cc-p
VTZ basis sets. Hindered rotation potentials were also calculated
and incorporated classically into rate constant calculations. With
the potential energy surface from either methods (1) or (4), the
thermal rate constants calculated via VariFlex agree well with
the experimental measurements and agree reasonably well with
earlier indirect experimental measurements by Baldwin et al.
They display substantial curvature due to effects of hindered
rotations. The other two electronic structure methods do not
agree well with experiment because of a poor description of the
late transition state. This demonstrates a case where functional
choice in a relatively high level DFT calculation has important
kinetics implications.
The Reaction of H with NO2. The reaction
with H+NO2 ®
HO+NO has been measured by J. Michael in our group.
Theoretical calculations by others (Peeters et al., U. of Leuvan,
Belgium) indicate that the rate limiting step in this reaction is
complex formation (either HONO* or HNO2*). In collaboration
with L. Harding we have generated a multi-reference singles and
doubles configuration interaction potential energy surface for the
approach of H to NO2 in the NO2 plane that displays
both
attack of the N radical orbital and the O radical orbital. By use
of calibrated pairwise additive models, this planar potential has
been extrapolated into a non-planar potential in the two angles
(spherical and azimuthal) that locate H relative to the C2v
axis
of the NO2. This allows a FTST treatment of the transitional
degrees of freedom in this complex formation collision (those
degrees of freedom that evolve from free rotations in the product
to bends in the HNO2 or HONO complex). Subsequent
calculations with VariFlex show the FTST rate constant to be
in good agreement with the measurements of Michael and with
two previous lower temperture experimental studies.
OHCO and OHOC van der Waals Dissociation.
L. Harding,
S. Gray, and I have an ongoing collaboration with the M. Lester
group (U. of Pennsylvania). The goals of this collaboration are
to use the experimental vibrational levels and widths to calibrate
the accuracy of the electronic structure calculations in the entrance
channel region of the OH+CO reaction. As L. Harding has found,
the OHCO and OHOC van der Waals molecule equilibrium
positions are on reaction pathways that lead to the HOCO
transition state. Thus vibrational excitation of the weakly bound
van der Waals molecules could not only lead to direct dissociation
to OH+CO but also to formation of HOCO and its subsequent
decay to either OH+CO or to H+CO2. Collaborative studies
between our group and the Lester group will both guide and
interpret experiment. Renner Teller and spin-orbit coupling at
a four atom level are involved in the vibrational spectroscopy
and S. Gray (primarily) and myself are generating bound
vibrational levels on the Harding surface including consideration
of this coupling. (See research summaries of Harding and Gray
for more details.)
Method and Code Development
Development and Implementation of
Flexible Transition
State Theory. In collaboration with D. Wardlaw (Queens U.)
and S. Robertson (Accelrys Inc.), variable reaction coordinate
FTST formalism has been significantly simplified at the energy
and angular momentum resolved level. The inaugural treatment
of FTST by Wardlaw and Marcus in the mid 1980s determined
microcanonical and canonical rate constants by the minimization,
along the center-of-mass separation coordinate, of a 2(n+1)
nested set of phase space integrals over angular momenta and
their conjugate angles where n is the number of transitional
modes (modes that describe free rotation in the reactants but
bound vibrations in the products). For bimolecular collisions,
up to five transitional modes are possible resulting in tedious
evaluations of up to 12-dimensional integrals. Since that time,
especially over the last decade, our collaboration and others
[S. Klippenstein (SNL), S. Smith (U. of Queensland)] have
systematically discovered ways of formally doing many of the
phase space integrals analytically, thereby reducing the residual
number of integrals that must be done numerically and
dramatically improving the computational efficiency of FTST.
With our simplified formalism referred to above, the residual
number of integrals has now been reduced to the minimum
possible without specification of the interaction potential.
For the energy-resolved microcanonical and for the canonical
rate expressions, the dimension of the numerical phase space
integral has been reduced to n. For energy- and angular
momentum-resolved microcanonical rate expression, the
dimension has been reduced to n+1 in general. However, the
additional integration beyond n reduces to an elliptic integral
expressible as an analytic series and, under certain circumstances,
can be solved in closed form (i.e., can be done analytically).
In all cases, the residual integrals are only over spatial coordinates
and include the potential in the integrand. They have a physical
interpretation as a steric factor. A Laplace transform relationship
between canonical and mircocanonical rate coefficients is
exploited in the simplification of the formalism.
POTLIB, a Library of Potential Energy Surfaces. In
collaboration with D. Truhlar (U. of Minnesota), R. Duchovic
(Purdue U. Indiana U. at Fort Wayne), and T. Allison (NIST),
we have constructed a potential energy surface subroutine library
called POTLIB, the description of which has recently been
submitted for publication. Because of an a common interface,
any code that uses potential energy surfaces can check out any
subroutine from the library and, via a single interface routine,
compile, link, and execute with that subroutine. The library
contains five example interface routines for ABCRATE and
POLYRATE (Truhlar et al.), VENUS (Hase et al.), VARIFLEX
(Klippenstein et al.), and DYNASOLVE (Zhang et al.). About
100 potential energy surfaces are now enrolled in the library.
Parallel Implementation of Miller Cumulative Reaction
Probability Method. With M. Minkoff (ANL Math. and Comp.
Sci. Division), we are developing a parallelized code for the
direct calculation of the cumulative reaction probability (CRP)
in a time independent manner using formalism originally developed
by Miller et al. (Berkeley). This code is built upon the PETSc
library of parallel subroutines for common mathematical kernels.
Up to seven degree of freedom model problems have been
examined on up to 128 processors at the NERSC SP with
relatively good parallelization and a time to solution per
eigenvalue of under eight minutes for the largest problem. The
SPAM technique (see R. Shepard’s summary) may result in
an effective preconditioner for this problem and will be examined.
(See S. Gray’s research summary for a time-dependent approach
to the CRP.)
Thermodynamics Studies
Heat of Formation of OH.
As discussed in greater detail in
the Research Summaries of B. Ruscic, our group initiated a
multi-laboratory experimental/theoretical study of DHf 0°(OH).
This study has definitively concluded that the consensus value in
all standard thermochemical tabulations is incorrect by up to 0.5
kcal/mol (depending on the tabulation). The origin of the error is
that a spectroscopic, rather than ion-cycle, value was incorrectly
accepted as more reliable. My role in this study was to contribute
to the analysis of the original spectroscopy measurements. These
measurements involved a Birge-Sponer extrapolation over only
one missing vibrational level of the A2S+
of OH. Using a high
quality ab initio curve for the same state by L. Harding and
applying the same Birge-Sponer extrapolation method to all but
the highest theoretical vibration level, the extrapolated dissociation
energy falls well below the directly calculated one. Using the
computed C6 long-range constant and the experimental RKR
curve, a Pade approximate extrapolation of the dissociation energy
also indicates that the Birge-Sponer estimate was significantly low.
Underestimation of the dissociation energy of the A2S+
state of
OH leads to an overestimation of the DHf 0°(OH)
by a number
of tenths of a kcal/mol. The photoionization studies that underpin
the ion-cycle value of DHf 0°(OH)
are free of this extrapolation
error and give a lower value that is corroborated by extremely
high level electronic structure calculations on the ground state of
OH by the Pacific Northwest National Laboratory members of
our collaboration.
Cyclopentadienyl Entropy. In collaboration
with H. Wang
(U. of Delaware) and J. Kiefer (U. of Illinois at Chicago), we
have determined the entropy of the cyclopentadienyl radical
C5H5 including its Jahn-Teller coupling. The C5H5
molecule
is implicated in several routes to the formation of the first aromatic
rings in the sooting chemistry of aliphatic fuels. However, several
key reactions, in particular, C3H3 + C2H2
® c-C5H5, have
been studied only in the reverse direction, requiring an accurate
equilibrium constant and thus entropy to obtain the rate in the
direction needed. C5H5 is distorted from D5h
symmetry by the
Jahn-Teller effect. The result is a peudorotation of all the atoms
in the molecule about each atom’s D5h position. The 2A2
and
2B1 electronic states are each visited alternately five
times in a
complete pseudorotational period. The 2A2 electronic
state
provides an equilibrium C2v structure and the 2B1
electronic
state provides a transition state only a few wavenumbers higher
in energy than the equilibrium energy. We carried out
CASSCF/cc-PVDZ calculations of both potential surfaces
involved in C5H5 along all normal coordinates that
can be
affected by Jahn-Teller distortion. In contrast to recent
calculations by others (Barckholtz et al.), we find the C-H E’2
in-plane bend and stretch modes are negligibly Jahn Teller
coupled. However both the E’2 in-plane bend and stretch
skeletal modes are found to be involved, but the bend
contribution is very small and its contribution to the entropy
is negligible. The in-plane C-C stretch modes strongly dominate,
affording a maximum stabilization energy of 4.73 kcal/mol
(i.e., the difference between the conical intersection at D5h
geometry and the 2A2 equilibrium geometry). Harmonic
frequencies are calculated for the other modes in the D5h
configuration, and these are scaled in accordance with a
comparison of experimental frequencies with similar calculations
on cyclopentadiene. Energy levels for nuclear motion in the
Jahn-Teller modes are then determined using the calculated
surface, and these are combined with the scaled harmonic
frequencies to obtain complete thermodynamic functions for the
radical. The computed results allow us to compare the Jahn-Teller
thermochemistry with two other simpler but approximate models.
One model ignores the Jahn-Teller coupling altogether and
derives from the potential energy surfaces what the frequencies
would have been if the conical intersection were removed. The
second model uses the frequencies for the 2A2 equilibrium
geometry, even though the lowest frequencies is hindered-rotor
like as it corresponds to motion along the direction of the
pseudorotation. The Jahn-Teller entropy splits the difference
between these two models, being about 1 cal/mol-degree higher
than that for the model that ignores the Jahn-Teller and about 2
to 3 cal/mol-degree lower than that for the model that uses the
2A2 equilibrium frequencies.
Publications, Submissions, and Talks
(1998 – 2001)
Publications and Submissions
VARIFLEX, A Program for Flexible Transition
State Theory,
S. J. Klippenstein, A. F. Wagner, S. H. Robertson, R. C. Dunbar,
and D.M. Wardlaw, at http://chemistry.anl.gov/chem.- dyn/VariFlex/index.html,
(1999)
High-Performance Computational Chemistry:
Hartree-Fock
Electronic Structure Calculations on Massively Parallel
Processors, J. L. Tilson, M. Minkoff, A. F. Wagner, R. Shepard,
R. J. Harrison, R. A. Kendall, A. T. Wong, Int'l
J. High-Perf.
Comp. App. 13, 291 (1999)
Initiation in H2/O2:
Rate Constants for H2+O2 ®
H+HO2
at High Temperature, J. V. Michael, J. W. Sutherland,
L. B. Harding, and A. F. Wagner, 28th Symposium
(International) on Combustion 28,1471-1478 (2000)
Exploring the OH+CO Reaction Coordinate
Via Infrared
Spectroscopy of OH-CO Reactant Complexes, M. I. Lester,
B. V. Pond, D. T. Anderson, L. B. Harding, A. F. Wagner,
J. Chem. Phys. 113, 9889-9892 (2000)
Flexible Transition State Theory for
a Variable Reaction
Coordinate: Derivation of Canonical and Microcanonical
Forms, S. H. Robertson, A. F. Wagner, D. M. Wardlaw,
J. Chem. Phys. 113, 2648 (2000)
Ab inito Determination of Americium Ionization
Potentials,
J. L. Tilson, R. Shepard, C. Naleway, A. F.
Wagner,
W. C. Ermler, J. Chem. Phys. 112, 2292 (2000)
Evidence for a Lower Enthalpy of Formation
of Hydroxyl
Radical and a Lower Gas Phase Bond Dissociation Energy
of Water, B. Ruscic, D. Feller, D. A. Dixon, K. A. Peterson,
L. B. Harding, R. A. Asher, and A. F. Wagner, J. Phys.
Chem. A 105, 1-4 (2001)
The Subspace Projected Approximate Matrix
(SPAM)
Modification of the Davidson Method, R. Shepard,
A. F. Wagner, M. Minkoff, and J. L. Tilson, J. Comp.
Phys. 172, 472-514 (2001)
The Calculation of f-f Spectra of Lanthanide
and Actinide
Ions by the MCDF-CI Method, M. Seth, R. Shepard,
A. F. Wagner, K. G. Dyall, J. Phys. B. 34, 2383-2406 (2001)
Flexible Transition State Theory for
a Variable Reaction
Coordinate: Analytical Expressions and an Application,
S. H. Robertson, A. F. Wagner, D. M. Wardlaw, J.
Chem. Phys. (in press)
Flexible Transition State Theory for
a Variable Reaction
Coordinate: Derivation of Canonical and Microcanonical
Forms with Angular Momentum Conservation, S. H. Robertson,
D. M. Wardlaw, A. F. Wagner, J. Chem. Phys.
(in press)
Mapping the OH + CO ®
HOCO Reaction Pathway
Through Infrared Spectroscopy of the OH-CO Reactant
Complex, M. I. Lester, B. V. Pond, M. D. Marshall,
D. T. Anderson, L. B. Harding, and A. F. Wagner,
Faraday Disc. (in press)
Thermodynamic Functions for the Cyclopentadienyl
Radical:
The Effect of Jahn-Teller Distortion, J. H. Kiefer, R. S. Tranter,
H. Wang, A. F. Wagner, Int. J. Chem. Kin. (in press)
POTLIB 2000: A Potential Energy Surface
Library for
Chemical Systems, R. J. Duchovic, Y. L. Volobuev,
G. C. Lynch, T. C. Allison, D. G. Truhlar, A. F. Wagner,
B. C. Garrett, Comp. Phys. Comm. (in press)
An Ab Initio Study of the f-f Spectroscopy
of Americium+3,
J. Tilson, M. Seth, C. Naleway, M. Seth, R.
Shepard,
A. F. Wagner, W. Ermler, J. Chem. Phys. (in press)
An Ab Initio Study of the Ionization
Potential and f-f
Spectroscopy of Europium Atoms and Ions, C. Naleway,
M. Seth, R. Shepard, A. F. Wagner, J. Tilson, W. C. Ermler,
and S. R. Brozell, J. Chem. Phys. (in press)
On the Enthalpy of Formation of Hydroxy
Radical and
Gas-Phase Bond Dissociation Energy of Water and Hydroxyl,
B. Ruscic, A. F. Wagner, L. B. Harding, R. L. Asher, D. Feller,
D. A. Dixon, K. A. Peterson, Y. Song, X. Qian, C.-Y. Ng,
J. Liu and W. Chen, J. Phys. Chem. (in preparation)
Rate Constants, 1100 £
T £ 2000 K, for the Reaction,
H + NO2 ® OH + NO, Using Two
Shock Tube
Techniques: Comparison of Theory to Experiment, M.-C. Su,
S. S. Kumaran, K. P. Lim, A. F. Wagner, L. B.
Harding,
and J. V. Michael, J. Phys. Chem. A (in preparation)
Talks and Presentations
Rate Constant Calculations for Barrierless
Reactions. II.
CFnH3-n + H (n=0,...,3) Rate Constants, A. F. Wagner,
D. Wardlaw, S. Robertson, Talk, 15th International
Symposium on Gas Kinetics, Bilbao, Spain (1998)
The Role of Kinetics in High Performance
Computing,
A. F. Wagner, Invited Talk, Council of Chemical Sciences
Workshop on Research Frontiers in Molecular Simulation and
Computational Chemistry, Santa Fe, NM (1998)
Role of Anharmonic Motion in Rcombination/Dissociation
Kinetics, A. F. Wagner, Invited Seminar, Department of
Chemistry, Wayne State University, Detroit, MI (1998)
Anharmonic Effects in the Recombination
of Free Radicals,
A. F. Wagner, Invited Talk, Mesilla Conference on Statistical
Theories in Chemistry, Los Cruces, NM (1998)
Reaction Rates for Reactions with Low
Barriers: Steric Factors
and Statistical Theories, A. F. Wagner, Invited
Seminar,
Department of Chemistry, Illinois Institute of Technology,
Chicago, IL (1999)
The Effect of Hindered Rotations on Reaction
Kinetics,
A. F. Wagner, Invited Seminar, Department of Chemistry,
Iowa State University, Ames, IA (1999)
The Influence of Hindered Rotations on
Barrierless
Dissociation/Recombination Reactions, A. F.
Wagner,
D. Wardlaw, S. Robertson, and L. Harding, Invited Talk,
217th American Chemical Society Meeting, Anaheim,
CA (1999)
Theoretical Studies in Actinide Chemistry,
A. F. Wagner,
Invited Talk, 217th American Chemical Society Meeting,
Anaheim, CA (1999)
Experimental and Theoretical Study of the Kinetics of
H + NO2 ® OH + NO, A. F. Wagner,
M.-C. Su,
S. S. Kumaran, K. P. Lim, J. V. Michael, L. B. Harding,
and D. C. Fang, Poster, 28th International Symposium on
Combusion, Edinburgh, Scotland (2000)
Rate Constants for H + O2
+ M ® HO2 + M at Room
Temperature in Seven Bath Gases and at High Temperature
in N2, Ar, and O2, J. V. Michael, M.-C. Su, J. W.
Sutherland,
J. J. Carroll, and A. F. Wagner, Poster, 28th International
Symposium on Combusion, Edinburgh, Scotland (2000)
Rate Constants for H2CO +
O2 ® HCO + HO2 at
High
Temperature, A. F. Wagner, J. V. Michael, M.-C. Su,
J. W. Sutherland, D.-C. Fang, and L. B. Harding, Poster,
28th Symposium (International) on Combustion, Edinburgh,
Scotland (2000)
Rate Theory for Barrierless Reactions:
Advances in Flexible
Transition State Theory with Applications, A. F. Wagner,
D. Wardlaw, S. Robertson, Talk, 16th International Symposium
on Gas Kinetics, Cambridge, England (2000)
The Influence of Hindered Rotations in
Kinetics, A. F. Wagner,
21st DOE-BES Combustion Research Contractors Meeting,
Westfield Conference Center, Chantilly, VA (2000)
Hindered Rotational Effects in Radical-Radical
Reactions,
A. F. Wagner, Invited Talk, American Chemical Society
Central Regional Meeting, Cincinnati, OH (2000)
The Role of Hindered Rotations in Recombination
Reactions,
A. F. Wagner, D. Wardlaw, S. Robertson, Invited
Talk, 219th
American Chemical Society Meeting, San Francisco, CA (2000)
Collisional Deactivation of HO2*
by Rare Gases, Small
Diatomics, and Water: The Importance of Long Range
Interactions, A. F. Wagner, J. V. Michael, M.-C. Su,
J. W. Sutherland, and J. J. Carroll, The XVIII Conference on
the Dynamics of Molecular Collisions, Copper Mountain Resort
and Conference Center, Copper Mountain, CO (2001)
Rate Constants for H + O2
+ M ® HO2 + M in Seven Bath
Gases, J. V. Michael, M.-C. Su, J. W. Sutherland,
J. J. Carroll,
and A. F. Wagner, Fifth International Confernce on Chemical
Kinetics, National Institute of Standards and Technology,
Gaithersburg, MD (2001)
The Calculation of Reliable Reaction
Rates for Combustion
Simulations, A. F. Wagner, First MIT Conference on
Computational Fluid and Solid Mechanics, Boston, MA (2001)
The Interplay between Mathematics and
Chemistry in
Computational Chemistry, A. F. Wagner, Invited Seminar,
Applied Mathematics Department, Northern Illinois University,
DeKalb, IL (2001)
Thermodynamic Functions for the Cyclopentadienyl
Radical:
The Effect of Jahn-Teller Distortion, A. F. Wagner, J. H. Kiefer,
R. S. Trantor, and H. Wang, Western State Section Meeting
of the Combustion Institute, Oakland, CA (2001)
ALBERT F. WAGNER
Office Address:
Chemistry Division
Argonne National Laboratory
9700 S. Cass Avenue
Argonne, IL 60439
(630) 252-3380 Fax: (630) 252-9292
Email: wagner@ tcg.anl.gov
Education:
California Institute of Technology,
Ph.D. in Chemical
Physics, 1972
Boston College, B. S. in Chemistry, 1966
Professional Experience:
5/90 – Present - Senior Chemist
and Group Leader,
Chemistry Division, Argonne National Laboratory
3/79 – 5/90 - Chemist, Chemistry Division, Argonne
National Laboratory
2/74 – 3/79 - Associate Chemist, Chemistry Division,
Argonne National Laboratory
2/72 – 2/74 - Postdoctoral Appointee,
Chemistry Division,
Argonne National Laboratory
Areas of Research and Expertise:
Theories of reaction dynamics and chemical
kinetics, especially
related to combustion. Parallel computing in theoretical chemistry.
Electronic structure calculations for lanthanides and actinides.
Structural models for X-ray scattering off of particles.
Professional Organizations:
Americal Chemical Society
American Physical Society
Combustion Institute
Professional Activities:
Member of the High Energy Density Review
Panel for the
AFSOR (1990-1995)
Visiting Scientist, Institute for Molecular
Science, Okazaki,
Japan (January-April, 1997)
Co-Symposium Chair for the Chemistry
of Combustion
Symposium, 215th American Chemical Society
National Meeting
(1998)
Vice-Chair of the 2000 Gordon Research
on Molecular
Interactions (Chair, 2002 Conference)
Vice-Chair of the 2003 Dynamics of Molecular
Collisions
Symposium
ANL Committees:
Computer Science Advisory Board and
the Senior Advisory
Committee
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