471505 High-Throughput Prediction of Finite Temperature Free Energies of Solids
Our broadly applicable method for evaluating temperature-dependent compound free energies of formation employs readily computable material-specific descriptors and utilizes existing datasets of more than 50,000 inorganic compounds to enable rapid computational prototyping at elevated temperatures. We build upon prior work that has demonstrated the use of total energy calculations to approximate the compound enthalpy of formation at 298 K with mean absolute error relative to experiment (MAE) = 0.054 eV/atom with fitted elemental-phase reference energies (FERE). Our prediction requires only the DFT total energy, the FERE correction, and two minimal-computational-cost material-specific predictors to compute compound free energies of formation with MAE < 0.1 eV/atom up to at least 1800 K. At 1000 K, the MAE between our prediction and experiment is 0.039 eV/atom for oxides, 0.057 eV/atom for nitrides, 0.055 eV/atom for selenides, 0.049 eV/atom for arsenides, 0.044 eV/atom for phosphides, and 0.037 eV/atom for sulfides. These results bridge the temperature gap between existing MGI inspired computational approaches, which have historically been limited to low temperature, and high temperature materials applications, providing the equivalent of tabulated thermochemical data for more than 50,000 inorganic materials.
See more of this Group/Topical: Materials Engineering and Sciences Division