Screening nature of the van der Waals density functional method: a review and analysis of the many-body physics foundation

2019/06/30 by Per Hyldgaard, Yang Jiao, Vivekanand Shukla
Physics and Astronomy · #Advanced Chemical Physics Studies #Molecule #Physics #Quantum and electron transport phenomena #Quantum mechanics #Spectroscopy and Quantum Chemical Studies #Statistical physics #cond-mat.mtrl-sci #physics.chem-ph #van der Waals force

paper · pdf · doi:10.1088/1361-648x/ab8250

published as Journal of Physics: Condensed Matter 32, 393001 (2020) · 57 pages, 16 figures, 4 Tables. Published as an invited Topical review in IOP Journal of Physics: Condensed Matter

openalex publication_date 2020/03/26 · arxiv created 2021/12/29 · arxiv updated 2021/12/30 · openalex created_date 2025/10/10 · openalex updated_date 2026/08/05

Abstract

We review the screening nature and many-body physics foundation of the van der Waals density functional (vdW-DF) method [Berland K et al 2015 Rep. Prog.Phys.78 066501], a systematic approach to construct truly nonlocal exchange-correlation energy density functionals.To that end we define and focus on a class of consistent vdW-DF versions that adhere to the Lindhard screening logic of the full method formulation.The consistent-exchange vdW-DF-cx version [Berland K and Hyldgaard P 2014 Phys.Rev. B 89 035412] and its spin extension [Thonhauser T et al 2015 Phys.Rev. Lett.115 136402] represent the first examples of this class; in general, consistent vdW-DFs reflect a concerted expansion of a formal recast of the adiabatic-connection formula [Hyldgaard P et al 2014 Phys.Rev. B 90 075148], an exponential summation of contributions to the local-field response, and the Dyson equation.We argue that the screening emphasis is essential because the exchange-correlation energy reflects an effective electrodynamics set by a long-range interaction.Two consequences are that (1) there are, in principle, no wiggle room in how one balances exchange and correlation, for example, in vdW-DF-cx, and that (2) consistent vdW-DFs have a formal structure that allows them to incorporate vertex-correction effects, at least in the case of levels that experience recoil-less interactions (for example, near the Fermi surface).We explore the extent to which the strictly nonempirical vdW-DF-cx formulation can serve as a systematic extension of the constraint-based semilocal functionals.For validation, we provide a complete survey of vdW-DF-cx performance for broad molecular processes, for the full set of 55 benchmarks in GMTKN55 [Goerigk L et al 2017 Phys.Chem.Chem.Phys.19 32184] and comparing to the quantum-chemistry calculations that are summarized in that paper.We also provide new vdW-DF-cx results for metal surface energies and work functions that we compare to experiment.Finally, we use the screening insight to separate the vdW-DF nonlocal-correlation term into pure-vdW-interaction and local-field-susceptibility effects and present tools to compute and map the binding signatures.

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