Our primary goal was to compute various thermodynamic quantities related to the formation of the solid-liquid interface. This was achieved by following the thermodynamic cycle, shown in Figure , which relates the needed total free energies (F), free energy changes (∆F), and surface tensions (γ = ∆F/A). The primary quantities of interest were the areanormalized free energy of formation of the solid-liquid interface (∆F sl /A sl = γ sl ), the free energy of solvation of the metal surface (F solv ), and the work of adhesion (W ad ). Figure 1 demonstrates how the free energy of bulk solid metal F s and that of the bulk water F l can be used as the references for γ sl . Similarly, for F solv , the reference states are the metal surface in vacuum and the bulk water with the free energies of F sv and F l , respectively. W ad is obtained by referencing against the metal-vacuum and water-vacuum surfaces. Here, we give a general description of the methodology while the detailed working equations used in the present work are provided in the Supplementary material (SM), Section S1 and Equations S1-S9.