Transferable screened range-separated hybrid functionals for electronic and optical properties of van der Waals materials

Kavli Affiliate: Jeffrey B. Neaton

| First 5 Authors: María Camarasa-Gómez, Ashwin Ramasubramaniam, Jeffrey B. Neaton, Leeor Kronik,

| Summary:

The accurate description of electronic properties and optical absorption
spectra is a long-standing challenge for density functional theory. Recently,
the introduction of screened range-separated hybrid (SRSH) functionals for
solid-state materials has allowed for the calculation of fundamental band gaps
and optical absorption spectra that are in very good agreement with many-body
perturbation theory. However, since solid-state SRSH functionals are typically
tuned to reproduce the properties of bulk phases, their transferability to
low-dimensional structures, which experience substantially different screening
than in the bulk, remains an open question. In this work, we explore the
transferability of SRSH functionals to several prototypical van der Waals
materials, including transition-metal sulfides and selenides, indium selenide,
black phosphorus, and hexagonal boron nitride. Considering the bulk and a
monolayer of these materials as limiting cases, we show that the parameters of
the SRSH functional can be determined systematically, using only the band-edge
quasiparticle energies of these extremal structural phases as fitting targets.
The resulting SRSH functionals can describe both electronic bandstructures and
optical absorption spectra with accuracy comparable to more demanding ab initio
many-body perturbation theory (GW and Bethe-Salpeter equation) approaches.
Selected examples also demonstrate that the SRSH parameters, obtained from the
bulk and monolayer reference structures, display good accuracy for
bandstructures and optical spectra of bilayers, indicating a degree of
transferability that is independent of the fitting procedure.

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