American Chemical Society
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Accurate Hybrid Density Functionals with UW12 Correlation

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posted on 2020-09-09, 19:09 authored by Zack M. Williams, Timothy C. Wiles, Frederick R. Manby
In previous work, we suggested a single-parameter hybrid functional containing a novel correlation contribution based on the Unsöld approximation, UW12. This model resembles the explicitly correlated part of MP2-F12 theory and can be written as an explicit formula in terms of the single-particle reduced density matrix. Here, we further investigate hybrid functionals containing UW12 correlation and in particular look at functionals with a large fraction of exact exchange to reduce the self-interaction error. We suggest two new hybrid functionals B-LYP-osUW12 and fB-LYP-osUW12. On the test sets we use, our best hybrid functional overall (B-LYP-osUW12) is of similar accuracy to the best double hybrids considered while eliminating the need for virtual orbitals.