Machine-learning octet $AB$-type binary compounds across chemical space with domain knowledge of the interatomic bond

Abstract

The prediction of the structural stability of octet $AB$-type binary compounds is a classical materials informatics problem. The challenge is to capture the relative stability of 4-fold coordinated atoms in zincblende ($β$-ZnS) structure and 6-fold coordinated atoms in rocksalt (NaCl) structure, modulated by charge transfer and atomic-size differences. Previous structure maps and machine-learning approaches used atomic features such as valence-electron count, ionization potential and atomic radii, using either physical intuition or symbolic regression. Here, we demonstrate that explicitly incorporating the domain knowledge of the interatomic bonds can significantly and systematically improve the prediction of $β$-ZnS/NaCl stability. We encode this bonding information through a coarse-grained representation of the local electronic structure obtained by a recursive solution of a tight-binding bond model. The underlying pairwise Hamiltonians are taken from downfolded eigenstates of density-functional theory calculations for diatomic molecules and thereby include domain knowledge of the bond between specific $A-B$ pairs. The benefit of this description is demonstrated with an ensemble of independently trained Kernel Ridge or symbolic regression models combined with sequential feature selection. The obtained models are compared to a previous symbolic-regression model using the same set of \emph{ab initio} calculations for octet binaries as training data. We find a significant improvement in the prediction of the formation energy difference of $AB$ compounds as compared to previous works and demonstrate that an increasing amount of bond-informed recursion features improves the predictive accuracy.