STUDIES OF THE INTERDEPENDENCE OF ELECTRONIC AND ATOMIC DYNAMICS AND STRUCTURE AT THE ELECTRODE-ELECTROLYTE INTERFACE

In many phenomena at the electrode-electrolyte interface, electronic a nd atomic structure and dynamics are strongly interdependent in ways t hat challenge traditional theory and simulation techniques. We illustr ate with some examples of our efforts to meet such challenges. In the case of the metal-aqueous electrolyte interface, we describe a recent direct dynamics model of the copper-water interface. For oxide-water i nterfaces, we review two methods: a self-consistent tight binding meth od applied to rutile surfaces and a polarizable, dissociable model of the water-ferric hydroxide interface. For modeling Faradaic reactions we describe recent progress on models of electron transfer reactions w hich shows that the rates are even more dependent on details of the el ectronic and atomic structure of the interface than traditional models might suggest. Copyright (C) 1996 Elsevier Science Ltd