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Method for long time scale simulations of solids: Application to crystal growth and dopant clustering

Description: An important challenge in theoretical chemistry is the time scale problem. Atomic motion can be simulated directly by integrating Newton's equations over a time scale of nanoseconds, but most interesting chemical reactions take place on a time scale of seconds. We have developed a methodology to bridge this time scale gap using harmonic transition state theory suitable for solid systems. Possible reactive events and their rates are found with a saddle point finding method called the dimer method. When enough events are found, a kinetic Monte Carlo algorithm is used to choose which event occurs so that the system's position can be advanced in time. This technique has two major advantages over traditional kinetic Monte Carlo -- atoms do not have to map onto lattice sites for classification and kinetic events can be arbitrarily complicated. We have studied the homoepitaxial growth of aluminum and copper using an EAM potential at 80K with experimentally relevant deposition rates of monolayers per minute using a multiple time scale approach. Atomic deposition events are simulated directly with classical dynamics for several picoseconds until the incident energy has dissipated, and the long time between deposition events is simulated with the adaptive kinetic Monte Carlo method. Our simulations indicate that the Al( 100) surface grows much smoother then Cu( 100) at temperature between 0 and 80K due in part to long range multi atom processes which enable aluminum atoms to easily descend from atop islands. The high rate of such processes is due to their low activation energy, which is supported by density functional theory calculations, and the trend that processes involving more atoms tend to have larger prefactors and be favored by entropy. The scheme is efficient enough to model the evolution of systems with ab-initio forces as well, for which I will show an ...
Date: January 1, 2002
Creator: Henkelman, G. A. (Graeme A.); Uberuaga, B. P. (Blas Pedro) & Jónsson, Hannes,
Partner: UNT Libraries Government Documents Department

Metal Oxides in the Environment

Description: Oxides are ubiquitous in much of environmental chemistry. Silica and related glasses are potential vehicles by which radioactive elements may be sequestered and stored. The migration of toxic waste in ground water is largely influenced by interactions at the liquid-solid interface, with several metal oxides making up the bulk of soil. In addition, metal oxides with Bronsted acid or Lewis base functionality are potential replacements for many traditional liquid catalysis that are hazardous to work with and difficult to dispose. In this proposal, we targeted two such areas of oxide chemistry. The long-term behavior of silicate materials slated for use in the entombment of high-level waste (HLW), and the use of solid acid metal oxides as replacements for toxic sulfuric and hydrofluoric acid used in industry (referred to as Green Chemistry). Thus, this project encompassed technology that can be used to both remediate and prevent pollution. These oxide systems were studied using density functional theory (DFT). The comparatively large size and complexity of the systems that will bweree studied made use of high-accuracy electronic structure studies intractable on conventional computers. The 512 node parallel processor housed in the Molecular Science Computing Facility (MSCF) provided the required capability.
Date: August 30, 2002
Creator: Jonsson, Hannes; Corrales, L. Rene; Gabriel, Peggy; Haw, James F.; Henkelman, Graeme A.; Neurock, Matthew et al.
Partner: UNT Libraries Government Documents Department