Chemical Physics

Personnel

Project Leader(s):
James Evans, Mark Gordon

Principal Investigators:
James Evans, Mark Gordon, Klaus Ruedenberg, Theresa Windus

Key Scientific Personnel:
Da-Jiang Liu, Michael Schmidt

Overview

The theoretical Chemical Physics program at Ames Laboratory supports integrated efforts in electronic structure theory and non-equilibrium statistical mechanical & multiscale modeling.  The primary focus is on the development and especially application of methods that enable the study of surface phenomena, heterogeneous catalysis, surface and bulk properties of solid clusters, solvent effects, and mechanisms in organometallic chemistry including solvents and relativistic effects.

Electronic structure theory efforts integrate development of fundamental theory by (expanding the capability for accurate treatment of large or complex systems of interest to DOE), with optimal strategies for computational implementation within GAMESS and NWChem. In particular, this includes development of embedding methods, effective fragment potential approaches, with special interest in liquid-solid interfaces, and a rigorous basis for semi-empirical tight-binding methods, all geared towards applications to various complex condensed phase systems.

The statistical mechanical & multiscale modeling studies often incorporate energetics from electronic structure analyses. A core focus is the modeling of chemisorption and heterogeneous catalysis on metal surfaces. We consider both reactions on extended surfaces (including multiscale studies of spatiotemporal behavior) and in nanoscale catalyst systems (including analysis of fluctuation effects). We also model transport and reaction processes at non-conducting surfaces and in mesoporous systems, and analyze fundamental behavior in general far-from-equilibrium reaction-diffusion systems.

 

This research is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences through the Ames Laboratory.  The Ames Laboratory is operated for the U.S. Department of Energy by Iowa State University under Contract No. DE-AC02-07CH11358.

Publications

2013
Boschen J S; Theis D; Ruedenberg K; Windus T L . 2013. Accurate ab initio potential energy curves and spectroscopic properties of the four lowest singlet states of C-2. Theoretical Chemistry Accounts. 133:1425. abstract
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West A C; Schmidt M W; Gordon M S; Ruedenberg K . 2013. A comprehensive analysis of molecule-intrinsic quasi-atomic, bonding, and correlating orbitals. I. Hartree-Fock wave functions. Journal of Chemical Physics. 139:234107. abstract
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Liu D J; Evans J W . 2013. Realistic multisite lattice-gas modeling and KMC simulation of catalytic surface reactions: Kinetics and multiscale spatial behavior for CO-oxidation on metal (100) surfaces. Progress in Surface Science. 88:393-521. abstract
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Miliordos E; Ruedenberg K; Xantheas S S . 2013. Unusual Inorganic Biradicals: A Theoretical Analysis. Angewandte Chemie-International Edition. 52:5736-5739. abstract
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Manna K; Everett W C; Schoendorff G; Ellern A; Windus T L; Sadow A D . 2013. Highly Enantioselective Zirconium-Catalyzed Cyclization of Aminoalkenes. Journal of the American Chemical Society. 135:7235-7250. abstract
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Wang J; Ackerman D M; Lin V S Y; Pruski M; Evans J W . 2013. Controlling reactivity of nanoporous catalyst materials by tuning reaction product-pore interior interactions: Statistical mechanical modeling. Journal of Chemical Physics. 138:134705. abstract
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Yan K; Schoendorff G; Upton B M; Ellern A; Windus T L; Sadow A D . 2013. Intermolecular beta-Hydrogen Abstraction in Ytterbium, Calcium, and Potassium Tris(dimethylsilyl)methyl Compounds. Organometallics. 32:1300-1316. abstract
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Russell S M; Kim Y; Liu D J; Evans J W; Thiel P A . 2013. Communication: Structure, formation, and equilibration of ensembles of Ag-S complexes on an Ag surface. Journal of Chemical Physics. 138:071101. abstract
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2012
Ivanic J; Schmidt M W; Luke B . 2012. High-level theoretical study of the NO dimer and tetramer: Has the tetramer been observed?. Journal of Chemical Physics. 137:214316. abstract
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Zeng T; Fedorov D G; Schmidt M W; Klobukowski M . 2012. Natural Spinors Reveal How the Spin-Orbit Coupling Affects the Jahn-Teller Distortions in the Hexafluorotungstate(V) Anion. Journal of Chemical Theory and Computation. 8:3061-3071. abstract
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