  We present a study of the solvation properties of model aqueous electrode
interfaces. The exposed electrodes we study strongly bind water and have closed
packed crystalline surfaces, which template an ordered water adlayer adjacent
to the interface. We find that these ordered water structures facilitate
collective responses in the presence of solutes that are correlated over large
lengthscales and across long timescales. Specifically, we show that the liquid
water adjacent to the ordered adlayers forms a soft, liquid-vapor-like
interface with concomitant manifestations of hydrophobicity. Temporal defects
in the adlayer configurations create a dynamic heterogeneity in the degree to
which different regions of the interface attract hydrophobic species. The
structure and heterogeneous dynamics of the adlayer defects depend upon the
geometry of the underlying ordered metal surface. For both 100 and 111
surfaces, the dynamical heterogeneity relaxes on times longer than nanoseconds.
Along with analyzing time scales associated with these effects, we highlight
implications for electrolysis and the particular catalytic efficiency of
platinum.
