Towards an atomic-scale understanding of electrochemical interface structure and dynamics.

For the knowledged-based development of electrochemical processes, a better fundamental understanding of the interfaces between electrodes and electrolytes is necessary. This requires insight into the interface structure and dynamics on the atomic-scale, including that of the liquid electrolyte in the near-surface region, i.e., in the inner and outer part of the electrochemical double layer. This prespective describes current studies of simple and well-defined electrochemical interfaces by first-principles electronic structure calculations and in situ structure-sensitive methods. It is shown that these experimental and theoretical studies are now approaching a level, where they can operate on the same footing, making direct comparison of the obtained results feasible. Using selected examples, progress in clarifying the structure and dynamics of the double layer, of adsorbed species on electrode surfaces, and of initial steps in electrochemical phase formation processes is discussed.