Machine-Learned Energy Functionals for Strongly Correlated Systems

We introduce multiconfiguration data-driven functional theory (MC-DDFT) as a new approach to multiconfiguration nonclassical functional theory (MC-NCFT), in which the classical energy of a multiconfigurational wave function is combined with a machine-learned functional for the nonclassical exchange-correlation energy. We also present results obtained by a related approach, multiconfiguration energy-correcting functional theory (MC-ECFT), in which the total energy of a wave function method (e.g. CASSCF or NEVPT2) is corrected with a machine-learned functional. On a dataset of carbene singlet-triplet energy splittings, we demonstrate that these new multiconfiguration data-driven functional methods (MC-DDFMs) are able to achieve near-benchmark performance on systems not used for training while being less active-space dependent than multiconfiguration pair-density functional theory using currently available translated functionals.