Accurate Nonempirical Range-Separated Hybrid van der Waals Density Functional for Complex Molecular Problems, Solids, and Surfaces
Journal article, 2022

We introduce a new, general-purpose, range-separated hybrid van der Waals density functional termed vdW-DF2-ahbr within the nonempirical vdW-DF method [Hyldgaard, et al. J. Phys. Condens. Matter 32, 393001 (2020)]. It combines a correlation from vdW-DF2 with a screened Fock exchange that is fixed by a new model of exchange effects in the density-explicit vdW-DF-b86r or rev-vdW-DF2 functional [Hamada, Phys. Rev. B 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 bulk as well as layered materials, and it systematically and significantly improves the performance of the 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 succeeding at challenging problems. For example, it (1) correctly predicts both the substrate structure and the site preference for CO adsorption on Pt(111), (2) it outperforms existing nonempirical vdW-DFs for the description of CO2 adsorption in both a functionalized and in a simple metal-organic framework, and (3) it is highly accurate for the set of base-pair interactions in a model of DNA assembly.

Author

Vivekanand Shukla

Chalmers, Microtechnology and Nanoscience (MC2), Electronics Material and Systems

Yang Jiao

Chalmers, Microtechnology and Nanoscience (MC2), Electronics Material and Systems

Jung-Hoon Lee

Lawrence Berkeley National Laboratory

Korea Institute of Science and Technology (KITECH)

Elsebeth Schröder

Chalmers, Microtechnology and Nanoscience (MC2), Quantum Device Physics

Jeffrey B. Neaton

Lawrence Berkeley National Laboratory

Kavli Energy NanoSciences Institute

University of California at Berkeley

Per Hyldgaard

Chalmers, Microtechnology and Nanoscience (MC2), Electronics Material and Systems

Physical Review X

21603308 (eISSN)

Vol. 12 4 041003

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Sustainable development

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Nanoscience and Nanotechnology

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Energy

Life Science Engineering (2010-2018)

Materials Science

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Physical Chemistry

Other Physics Topics

Theoretical Chemistry

Condensed Matter Physics

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C3SE (Chalmers Centre for Computational Science and Engineering)

DOI

10.1103/PhysRevX.12.041003

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Latest update

10/25/2023