Data-Driven Approaches Can Overcome the Cost-Accuracy Trade-Off in Multireference Diagnostics.

Journal of Chemical Theory and Computation
Chenru DuanHeather J Kulik

Abstract

High-throughput computational screening typically employs methods (i.e., density functional theory or DFT) that can fail to describe challenging molecules, such as those with strongly correlated electronic structure. In such cases, multireference (MR) correlated wavefunction theory (WFT) would be the appropriate choice but remains more challenging to carry out and automate than single-reference (SR) WFT or DFT. Numerous diagnostics have been proposed for identifying when MR character is likely to have an effect on the predictive power of SR calculations, but conflicting conclusions about diagnostic performance have been reached on small data sets. We compute 15 MR diagnostics, ranging from affordable DFT-based to more costly MR-WFT-based diagnostics, on a set of 3165 equilibrium and distorted small organic molecules containing up to six heavy atoms. Conflicting MR character assignments and low pairwise linear correlations among diagnostics are also observed over this set. We evaluate the ability of existing diagnostics to predict the percent recovery of the correlation energy, %Ecorr. None of the DFT-based diagnostics are nearly as predictive of %Ecorr as the best WFT-based diagnostics. To overcome the limitation of this cost-a...Continue Reading

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Citations

Dec 3, 2020·The Journal of Chemical Physics·Alberto FabrizioClemence Corminboeuf
Nov 20, 2020·Chemical Reviews·Julia Westermayr, Philipp Marquetand
May 12, 2021·The Journal of Physical Chemistry Letters·Chenru DuanHeather J Kulik
Aug 11, 2021·The Journal of Physical Chemistry Letters·Daniel S KingLaura Gagliardi
Sep 1, 2020·The Journal of Physical Chemistry Letters·Fang LiuHeather J Kulik
Jul 22, 2020·The Journal of Physical Chemistry Letters·Chenru DuanHeather J Kulik

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