Accurate non-empirical range-separated hybrid van der Waals density functional for complex molecular problems, solids, and surfaces

Kavli Affiliate: Jeffrey B. Neaton

| First 5 Authors: Vivekanand Shukla, Yang Jiao, Jung-Hoon Lee, Elsebeth Schroder, Jeffrey B. Neaton

| Summary:

We introduce a new, general-purpose, range-separated hybrid van der Waals
density ph{functional, termed vdW-DF-ahbr,} within the non-empirical vdW-DF
method [JPCM 32, 393001 (2020)]. It combines correlation from vdW-DF2 with a
screened Fock exchange that is fixed by ph{a new model of exchange effects} in
the density-explicit vdW-DF2-b86r functional [PRB 89, 121103(R) (2014)]. The
new vdW-DF2-ahbr prevents spurious exchange binding and has a
small-density-gradient form set from many-body perturbation analysis. It is
accurate for ph{bulk as well as layered materials} and it systematically and
significantly improves the performance of present vdW-DFs for molecular
problems. Importantly, vdW-DF2-ahbr also outperforms present-standard
(dispersion-corrected) range-separated hybrids on a broad collection of
noncovalent-interaction benchmark sets, while at the same time successfully
mitigating the density-driven errors that often affect the description of
molecular transition states and isomerization calculations. vdW-DF2-ahbr
furthermore improves on state of the art density functional theory approaches
by 1) correctly predicting both the substrate structure and the site preference
for CO adsorption on Pt(111), 2) outperforming existing non-empirical vdW-DFs
for the description of CO$_2$ adsorption in both a functionalized and in a
simple metal-organic framework, and 3) being highly accurate ph{for the} set
of base-pair interactions in a model of DNA assembly.

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