Besides the fundamental understanding of interfacial structure and thermodynamics, the results of this work can be used for validating, benchmarking, and parameterizing other simulation methods. For instance, the contact angles and water structures we have obtained using DFT-MD differ significantly from those by Gim et al. who employed QM/MM-MD. The interfacial water entropies computed in our work for Pt differ from those obtained by Jung et al. , who used ReaxFF-MD. In particular, the interfacial water entropies by Jung are about 30 % smaller than ours. We speculate that the differences are due to both the short sampling time (1.5 ps) in the PT2 simulations and the deficiencies of the ReaxFF force field parameterized for Pt-O rather than Pt-H 2 O systems. These comparisons underscore the importance of QM/MM and ReaxFF validation and parameterization against DFT-MD quality data. We also anticipate that the results herein provide a rigorous test for current and future machine learning interatomic potentials.