Shukla, Vivekanand Jiao, Yang Lee, Jung-Hoon Schroeder, Elsebeth Neaton, Jeffrey B. Hyldgaard, Per 2024-01-19T11:01:30Z 2024-01-19T11:01:30Z 2022-11-10 2022-10 2160-3308 https://pubs.kist.re.kr/handle/201004/114457 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. English American Physical Society Accurate Nonempirical Range-Separated Hybrid van der Waals Density Functional for Complex Molecular Problems, Solids, and Surfaces Article 10.1103/PhysRevX.12.041003 1 Physical Review X, v.12, no.4 Physical Review X 12 4 Y scie scopus 000871102200001 Physics, Multidisciplinary Physics Article GENERALIZED GRADIENT APPROXIMATION EXCHANGE-CORRELATION ENERGY METAL-ORGANIC FRAMEWORKS MAIN-GROUP THERMOCHEMISTRY CARBON-DIOXIDE ELECTRON-GAS NONCOVALENT INTERACTIONS AB-INITIO ADSORPTION DFT