Chemical Bonding in Metallic Glasses from Machine Learning and Crystal Orbital Hamilton Population

Abstract: The chemistry (composition and bonding information) of metallic glasses (MGs) is at least as important as structural topology for understanding their properties and production/processing peculiarities. This article reports a ML-based approach that brings an unprecedented "big picture" view of chemical bond strengths in MGs of a prototypical alloy system. The connection between electronic structure and chemical bonding is given by crystal orbital Hamilton population (COHP) analysis; within the framework of density functional theory (DFT). The stated comprehensive overview is made possible through a combination of: efficient quantitative estimate of bond strengths supplied by COHP analysis; representative statistics regarding structure in terms of atomic configurations achieved with classical molecular dynamics simulations; and the smooth overlap of atomic positions (SOAP) descriptor. The study is supplemented by an application of that ML model under the scope of mechanical loading; in which the resulting overview of chemical bond strengths revealed a chemical/structural heterogeneity that is in line with the tendency to bond exchange verified for atomic local environments. The encouraging results pave the way towards alternative approaches applicable in plenty of other contexts in which atom categorization (from the perspective of chemical bonds) plays a key role.