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Abstract
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.
Supplementary materials
Title
Supporting Information
Description
Names of the carbenes included in the training, validation, test, and test subsets. Histograms showing systematic errors in reference methods. Basis set dependence of MC-DDFMs. Per- formance and active space and basis set dependence of MC-DDFMs trained solely on density features or solely on on-top density features. Individual performances on benzene, cyclobu- tadiene, and 1,3-bis(methylene)-cyclobutadiene.
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