The DFT-MD simulations were performed within the canonical NVT ensemble at 298 K using the Langevin thermostat with a friction coefficient of 5 ps -1 . The Langevin thermostat is recommended for uniform kinetic energy distribution over all degrees of freedom. However, the friction coefficient may impact the velocity auto-correlation functions and thereby the density of states distributions and entropy values computed from them. We selected the friction coefficient to provide both good temperature control and minimal change of the DoS. Each system was first thermalized at least for 5 ps, whereas the lengths of the subsequent statistical sampling runs were 40 ps for the interfaces (sl), 20 ps for the bulk water (l), 11 ps for the water film (lv), and 5 ps for reference metal systems (s and sv). Based on the previous studies, these sampling times are long enough for converged 2PT entropies within ±1 J K -1 mol -1 . Our thorough convergence study (Supplementary Material Section S6) also shows that the internal energies, entropies, and free energies are well-converged and have uncertainties of ± 2 meV/Å 2 , ± 0.01 meV K -1 , and ± 2 meV/Å 2 , respectively. The employed setup gives a liquid-vacuum surface tension of 71.5 dyn cm -1 in excellent agreement with experiments (72.8 dyn cm -1 ) thus providing a robust benchmark for the chosen approach and used parameters.