Jung, Jong HyunSrinivasan, PrashanthForslund, AxelGrabowski, Blazej2023-09-132023-09-1320232057-39601860223044http://nbn-resolving.de/urn:nbn:de:bsz:93-opus-ds-134991http://elib.uni-stuttgart.de/handle/11682/13499http://dx.doi.org/10.18419/opus-13480Accurate prediction of thermodynamic properties requires an extremely accurate representation of the free-energy surface. Requirements are twofold - first, the inclusion of the relevant finite-temperature mechanisms, and second, a dense volume–temperature grid on which the calculations are performed. A systematic workflow for such calculations requires computational efficiency and reliability, and has not been available within an ab initio framework so far. Here, we elucidate such a framework involving direct upsampling, thermodynamic integration and machine-learning potentials, allowing us to incorporate, in particular, the full effect of anharmonic vibrations. The improved methodology has a five-times speed-up compared to state-of-the-art methods. We calculate equilibrium thermodynamic properties up to the melting point for bcc Nb, magnetic fcc Ni, fcc Al, and hcp Mg, and find remarkable agreement with experimental data. A strong impact of anharmonicity is observed specifically for Nb. The introduced procedure paves the way for the development of ab initio thermodynamic databases.eninfo:eu-repo/semantics/openAccesshttp://creativecommons.org/licenses/by/4.0/530article