Computational
Chemical Dynamics of Complex Systems
Funding
and resources:
"Computational Chemical
Dynamics of Complex Systems" is a Computational Grand Challenge project
of
The William R. Wiley Environmental Molecular Sciences Laboratory
(EMSL), a U.S.
Department of Energy national scientific user facility located at
Pacific Northwest
National Laboratory (PNNL) in Richland,
Washington. Resources are
provided by EMSL's Molecular Science Computing Facility (MSCF).
http://mscf.emsl.pnl.gov/research/intro_cgca.shtml
The project is a
collaborative
effort involving scientists in the Department of Chemistry at the University of Minnesota and scientists at
PNNL.
Participants:
| University of Minnesota
|
Donald
G. Truhlar, Principal Investigator |
|
|
Aleksandr
Marenich, Project Manager for UMN |
|
Elizabeth
A.
Amin |
|
Kelly
E.
Anderson |
|
|
Alessandro
Cembran |
|
|
Christopher J. Cramer
|
|
Jiali
Gao
|
|
|
Hannah Leverentz
|
|
|
Gillian
C.
Lynch (collaborator, University
of Houston)
|
|
|
Manjeera Mantina
|
|
|
Steven L. Mielke
|
|
|
Ewa Papajak
|
|
|
J.
Ilja Siepmann
|
|
Ke Yang |
|
|
Jingjing
Zheng |
|
|
|
| PNNL |
Marat
Valiev, Project Manager for PNNL |
|
|
Peng-Dong Fan |
|
|
Bruce C. Garrett |
|
|
Karol Kowalski |
|
|
Sriram Krishnamoorthy |
|
|
|
Project summary:
New research
capabilities in
computational chemical dynamics are expected to play a significant role
in
enabling environmental scientists worldwide to address environmental
challenges
facing DOE and the nation. The goal of this project is to apply
powerful new
simulation techniques to tackle computationally challenging problems in
chemical dynamics, with special emphasis on electrochemistry,
heterogeneous
catalysis, nanoparticles, solid-state dynamics, and photochemistry.
These
calculations are being carried out with new high-throughput integrated
software
that we are developing.
Recent advances in
computer power
and algorithms have made possible accurate calculations of many
chemical
properties for both equilibria and kinetics. Nonetheless, applications
to
complex chemical systems, such as reactive processes in the condensed
phase,
remain problematic due to the lack of a seamless integration of
computational
methods that allow modern quantum electronic structure calculations to
be
combined with state-of-the-art methods for chemical thermodynamics and
reactive
dynamics. These problems are often exacerbated by unvalidated methods
and
limited software reliability. Our consortium is developing an
integrated
software suite that combines electronic structure packages with
dynamics codes
and efficient sampling algorithms for a variety of condensed-phase
modeling
problems including thermochemical kinetics and rate constants,
photochemistry
and spectroscopy, chemical and phase equilibria, electrochemistry, and
heterogeneous
catalysis. These fundamental areas of research are important for solar
energy,
fuel- cell technology, environmental remediation, weather modeling,
pollution
modeling, and atmospheric chemistry.
Photochemical creation
of excited
states offers a means to control chemical transformations because
different
wavelengths of light can be used to create different vibronic states,
thereby
directing chemical reactions along different pathways. It is crucial to
understand how energy deposited into the system is used; this is
particularly
complicated in condensed phase systems where there are many ways to
dissipate
excess energy. Similar opportunities and challenges present themselves
in the
areas of electrochemistry and catalysis. We are therefore carrying out
prototype
large-scale applications on environmental problems as well as other
applications to complex chemical dynamics processes, focusing on three
high-impact areas. In the computational electrochemistry area, are
especially
concerned with processes that enhance the design of fuel cell
technology and
with the calculation of in situ reduction potentials. For
heterogeneous,
nanoparticle, and solid-state dynamics, we are developing an array of
methods
for multi-time-scale simulation of nucleation of crystals in solution,
reactions of radicals at solution-phase interfaces and in ice, zeolite
catalysis, structure and dynamics of gallazane precursors to gallium
nitride
nanocrystals, the regulatory role of metal ions in the reactivity of
inorganic
phosphates, nanoparticles structure and dynamics, and ice dynamics. In
the
computational photochemistry area, we are constructing potential energy
surfaces for a number of photochemical reactions and employing them for
dynamics calculations based on the new decay of mixing with coherent
switches
algorithm. We are also considering solvatochromic shifts on conical
intersections that govern selected photochemical processes.
List of publications
supported in part by this Computational Grand Challenge grant,
2007-2008:
- “Thermochemical
kinetics of hydrogen-atom transfers between
methyl, methane, ethynyl, ethyne, and hydrogen,” J. Zheng, Y. Zhao, and
D. G.
Truhlar, Journal of Physical Chemistry A 111, 4632-4642 (2007).
- “Attractive noncovalent interactions in grubbs second-generation Ru
catalysts
for olefin metathesis,” Y. Zhao and D. G. Truhlar, Organic Letters 9,
1967-1970
(2007).
- “Size-selective supramolecular chemistry in a hydrocarbon nanoring,” Y.
Zhao
and D. G. Truhlar, Journal of the American Chemical Society 129,
8440-8442
(2007).
- “Density functionals with broad applicability in chemistry,” Y. Zhao
and D. G.
Truhlar, Accounts of Chemical Research 41, 157-167 (2008).
- “Density functional theory in transition-metal chemistry: relative
energies of
low-lying ltates of iron compounds and the effect of spatial symmetry
breaking,” A. Sorkin, M. A. Iron, and D. G. Truhlar, Journal of
Chemical Theory
and Computation 4, 307-315 (2008).
- “A prototype for graphene material simulation: structures and
interaction
potentials of coronene dimers,” Y. Zhao and D. G. Truhlar, Journal of
Physical
Chemistry C 112, 4061-4067 (2008).
- “How well can new-generation density functionals describe the
energetics of
bond dissociation reactions producing radicals?” Y. Zhao and D. G.
Truhlar,
Journal of Physical Chemistry A 112, 1095-1099 (2008).
- “Benchmark data for interactions in zeolite model complexes and their
use for
assessment and validation of electronic structure methods,” Y. Zhao and
D. G.
Truhlar, Journal of Physical Chemistry C 112, 6860-6868 (2008).
- “Computational characterization and design of buckyball tweezers:
density
functional study of concave-convex pi...pi interactions,” Y. Zhao and
D. G.
Truhlar, Physical Chemistry Chemical Physics 10, 2813-2818 (2008).
- “Perspective on foundations of solvation modeling: the electrostatic
contribution to the free energy of solvation,” A. V. Marenich, C. J.
Cramer,
and D. G. Truhlar, Journal of Chemical Theory and Computation 4,
877-887
(2008).
- “Construction of a generalized gradient approximation by restoring the
density-gradient expansion and enforcing a tight lieb-oxford bound,” Y.
Zhao
and D. G. Truhlar, Journal of Chemical Physics 128, 184109/1-8 (2008).
- “Large-scale parallel calculations with
combined coupled cluster and molecular mechanics formalism: excitation
energies
of zinc-porphyrin in aqueous solution,” P.
D. Fan, M. Valiev, and K. Kowalski, Chemical Physics Letters 458, 205 (2008).
- “Exploring the limit of accuracy of the global hybrid density functional for main-group thermochemistry, kinetics, and noncovalent interactions,”
Y. Zhao and D. G. Truhlar, Journal of Chemical Theory and Computation 4, 1849-1868 (2008).
- “Benchmark energetic data in a model system for Grubbs II metathesis
catalysis
and their use for assessment and validation of electronic structure
methods,”
Y. Zhao and D. G. Truhlar, Journal of Chemical Theory and Computation (2009); article ASAP, DOI: 10.1021/ct800386d.
- “On the function of pentameric phospholamban: ion
channel or storage
form?” L. Becucci, A. Cembran, C. B. Karim, D. D. Thomas, R.
Guidelli, J.
Gao, and G. Veglia, Journal of Americal Chemical Society, submitted
October,
2008.
- “Universal solvation model based on solute electron density
and a continuum model of the solvent defined by the bulk dielectric
constant
and atomic surface tensions,” A. V. Marenich, C. J. Cramer, and D.
G.
Truhlar, Journal of Physical Chemistry B (2009); article ASAP, DOI: 10.1021/jp810292n.
- “Thermochemical kinetics for multireference systems: addition reactions of ozone,” Y. Zhao, O. Tishchenko,
J. R. Gour, W. Li., J. J. Lutz, P. Piecuch, and D. G. Truhlar, Journal of Physical Chemistry A (2009); article ASAP, DOI: 10.1021/jp811054n.
|
Research highlights:
Computationally Intensive Research Project (2009-2011):
grant proposal (submitted April 30, 2009)
2008 Summary
2008 Technical Report
2008 PowerPoint Slides
2007 Summary
2007 Technical Report
2007 PowerPoint Slides
Additional information:
Additional research documents for internal use (password-protected)
Request for a Grand Challenge account (password-protected)
Links:
Donald G. Truhlar's
Home Page
Integrated Tools Home Page
Computational Chemistry at the
University of
Minnesota
Chemical Sciences Division,
PNNL
Department of Chemistry at the
University of
Minnesota
This document last modified Tuesday, 05-May-2009 16:08:21 CDT