Enabling materials design of ionic systems

Materials discovery and design critically relies on accurate enthalpies. The formation enthalpy – quantifying the thermodynamic stability of a compound – is a key quantity in ab initio materials databases such as AFLOW [1] to enable autonomous materials design. For ionic systems such as chalcogenides (e.g. oxides), pnictides (e.g. nitrides), and halides, standard semi-local DFT leads, however, to errors of several hundred meV/atom [2,3] for this quantity inhibiting materials design. To address this critical issue, we have developed the "coordination corrected enthalpies" (CCE) method yielding highly accurate room temperature formation enthalpies with mean absolute errors down to 27 meV/atom [3]. Recently, we have also introduced AFLOW-CCE [4]: an implementation of the method into the freely available AFLOW software for automated correction of DFT results. The tool returns the CCE corrections, or even the CCE formation enthalpies if pre-calculated LDA, PBE or SCAN values are provided. The autonomous implementation enables the enthalpy correction of an extensive library of materials as well as the accurate and quick generation of convex hull phase diagrams. The results can also be used for the computational design of e.g. nanoscale materials [5]. [1] S. Curtarolo et al., Comput. Mater. Sci. 58, 218 (2012). [2] V. Stevanović et al., Phys. Rev. B 85, 115104 (2012). [3] R. Friedrich et al., npj Comput. Mater. 5, 59 (2019). [4] R. Friedrich et al., Phys. Rev. Mater. 5, 043803 (2021). [5] R. Friedrich et al., in preparation (2021).