Deep Mind 21 functional does not extrapolate to transition metal chemistry

Abstract

The development of density functional approximations stands at a crossroads: while machine-learned functionals show potential to surpass their human-designed counterparts, their extrapolation to unseen chemistry lags behind. Here we assess how well the recent Deep Mind 21 (DM21) machine-learned functional [Science, 2021, 374, 1385–1389], trained on main-group chemistry, extrapolates to transition metal chemistry (TMC). We show that DM21 demonstrates comparable or occasionally superior accuracy to B3LYP for TMC, but consistently struggles with achieving self-consistent field convergence for TMC molecules. We also compare main-group and TMC machine-learning DM21 features to shed light on DM21's challenges in TMC. We finally propose strategies to overcome limitations in the extrapolative capabilities of machine-learned functionals in TMC.