Accurate non-empirical range-separated hybrid van der Waals density functional for complex molecular problems, solids, and surfaces
arXiv:2203.06682 · doi:10.1103/PhysRevX.12.041003
Abstract
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 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.
54 pages and 14 figures
References in corpus (33)
- Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
- Restoring the density-gradient expansion for exchange in solids and surfaces
- Generalized gradient approximation for solids and their surfaces
- Advanced capabilities for materials modelling with Quantum ESPRESSO
- A Higher-Accuracy van der Waals Density Functional
- Development of Novel Density Functionals for Thermochemical Kinetics
- Nonlocal van der Waals density functional: The simpler the better
- Van der Waals bonding in layered compounds from advanced first-principles calculations
- Perspective: Advances and challenges in treating van der Waals dispersion forces in density functional theory
- van der Waals forces in density functional theory: The vdW-DF method
- Self-consistent hybrid functional for condensed systems
- Van der Waals interactions in DFT made easy by Wannier functions
- DFT: A Theory Full of Holes?
- Are we van der Waals ready?
- Piecewise Linearity of Approximate Density Functionals Revisited: Implications for Frontier Orbital Energies
- Electrostatics in Periodic Boundary Conditions and Real-space Corrections
- The random phase approximation applied to solids, molecules, and graphene-metal interfaces: From weak to strong binding regimes
- Next-generation non-local van der Waals density functional
- van der Waals density functionals built upon the electron-gas tradition: Facing the challenge of competing interactions
- Towards a working density-functional theory for polymers: First-principles determination of the polyethylene crystal structure
- Band gaps of crystalline solids from Wannier-localization based optimal tuning of a screened range-separated hybrid functional
- Gedanken Densities and Exact Constraints in Density Functional Theory
- Nonlocal van der Waals functionals for solids: Choosing an appropriate one
- What types of chemical problems benefit from density-corrected DFT? A probe using an extensive and chemically diverse test suite
- Energy Level Alignment at Molecule-Metal Interfaces from an Optimally-Tuned Range-Separated Hybrid Functional
- Interpretation of van der Waals density functionals
- Study of van der Waals bonding and interactions in metal organic framework materials
- Nature and strength of bonding in a crystal of semiconducting nanotubes: van der Waals density functional calculations and analytical results
- Theoretical and experimental analysis of H2 binding in a prototype metal organic framework material
- Photoluminescence Lineshapes for Color Centers in Silicon Carbide from Density Functional Theory Calculations
- A theoretical study of the hydrogen-storage potential of (H_2)_4CH_4 in metal organic framework materials and carbon nanotubes
- vdW-DF-ahcx: a range-separated van der Waals density functional hybrid
- Improved proton-transfer barriers with van der Waals density functionals: Role of repulsive non-local correlation