Chemical Dynamics at Solid Surfaces

Yale University, New Haven CT

Investigators

Abstract

Professor John Tully, of Yale University, is supported by the Theoretical and Computational Chemistry program to study chemical dynamics at solid surfaces. The objective of this research is to advance the atomistic understanding of dynamical processes at solid surfaces. New theories are developed and methodologies are implemented computationally. The focus is on the simulation of those photochemical processes at surfaces that are mediated by electronic excitations. There is an emphasis on understanding how vibrational tunneling and zero point motion affect such processes. Methods for accelerating the simulation of rare events associated with non-equilbrium chemical reactions are developed. These calculations rely on the use of density functional theory and conventional quantum chemistry methods. Atomistic motions and reactions can evolve smoothly but may also involve discontinuous processes that are associated with electronic transitions and absorption or emission of light. Such processes may not be modeled with classical potentials and require an understanding of both electronic and vibrational processes as well as the ability to describe interactions between electrons, vibrational degrees of freedom, and light. Such interactions are strongly relevant to catalytic activity, materials processing, biophysics and photochemistry. Understanding of such interactions is also relevant to the problem of nondestructive evaluation of materials such as ancient artifacts. A program aimed at including undergraduates in such endeavors is included in this research initiative.