Article,
Some recent trends in computer simulations of aqueous double layers
Electrochimica Acta, 49 (1): 23--27 (December 2003)
Abstract
Recent molecular simulations of the electric double layer between
an aqueous and a metallic phase are reviewed. Several trends in the
field can be identified: (i) the increasing use of ab initio simulation
methods, most notably the Car-Parrinello method, allows to combine
a statistical mechanical description of the double layer with a description
of elementary chemical processes on the electronic structure level;
(ii) the application of free-energy methods in one and (recently)
two dimensions to describe chemical reactivity within and beyond
the framework of the Marcus theory of electron transfer; and (iii)
at high concentrations, direct simulations of two-phase systems with
an aqueous solution and a charged or uncharged solid phase or surface
can model the entire double layer region.
