Tall Bridge Following surface characterization, RNEMD simulations were carried out for at least 1 ns with an applied thermal flux, J z = 2.5 × 10 -6 kcal mol -1 Å-2 fs -1 for periodic systems and J r = 1.8 × 10 -6 kcal mol -1 Å-2 fs -1 for non-periodic systems. A thermal flux was applied to all systems for at least 1 ns. The flux values were chosen so the heat rate through the metal/solvent interface was nearly identical in the planar and spherical geometries. Relatively small flux values also ensure that the systems remain in a state close to ambient conditions, limiting thermally-induced density changes in the solvent phase which could interfere with measurements of the interfacial conductance. We studied the thermal profile after flux application times of up to 1 ns, and the results can be seen in Figure in the SI. Under steady state conditions, temperature discontinuities formed at the boundaries between the gold and the solvent, and a thermal gradient developed in the solvent.