Chemical Dynamics at Solid Surfaces

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John Tully of Yale University is supported by the Theoretical and Computational Chemistry Program for research that focuses on the atomic-level understanding of dynamical processes at solid surfaces. New theoretical and computational tools will be created and used to study specific chemical problems in three areas. First, dynamics at metal surfaces will be explored to enable prediction of the contribution of electron-hole pair transitions to adsorbate energy transfer. Methods for computing the relative intensities of vibrational modes and approximate propensity rules in scanning tunneling microscopy (STM) will be developed. Second, mixed quantum-classical dynamics will be developed with the goal of extending conventional molecular dynamics simulations to practical applications involving electronic transitions and/or quantum nuclear motion. Finally, ab initio methods for computing energies and lifetimes of adsorbate excited states at semiconductor and metal surfaces will be developed and tested, then extended to calculating energies and widths of adsorbate-ion resonance states and excited states. Understanding molecule and electron behavior on solid surfaces is important for gaining insights needed to drive innovations in technologically important areas such as semiconductor processing. Outcomes from this research are expected to impact a variety of important chemical applications, including the determination of molecular identity from observed topographical features in STM, and the understanding of multi-dimensional processes such as those involved in electrochemistry, condensed phase dynamics, and enzyme reactions.