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

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 correlation from vdW-DF2 with screened Fock exchange that is fixed by new model of effects in density-explicit vdW-DF-b86r or rev-vdW-DF2 [Hamada, Rev. B 89, 121103(R) (2014)]. The prevents spurious binding and has small-density-gradient form set many-body perturbation analysis. accurate for bulk as well layered materials, it systematically significantly improves performance present vdW-DFs molecular problems. Importantly, also outperforms present-standard (dispersion-corrected) hybrids on broad collection noncovalent-interaction benchmark sets, while at same time successfully mitigating density-driven errors often affect description transition states isomerization calculations. furthermore state-of-the-art density-functional-theory approaches succeeding challenging For example, (1) correctly predicts both substrate structure site preference CO adsorption Pt(111), (2) existing CO2 functionalized simple metal-organic framework, (3) highly base-pair interactions DNA assembly.5 MoreReceived 24 March 2022Revised 14 August 2022Accepted 8 September 2022DOI:https://doi.org/10.1103/PhysRevX.12.041003Published American Physical Society under terms Creative Commons Attribution 4.0 International license. Further distribution this work must maintain attribution to author(s) published article’s title, journal citation, DOI.Published SocietyPhysics Subject Headings (PhySH)Research AreasAdhesionAdsorptionChemical bondingElectronic structureFirst-principles calculationsTechniquesDensity theoryMaterials modelingCondensed Matter, Materials & Applied Physics