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

Abstract

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.

arXiv comment14 pages + 8 figures; Supporting Information (21 pages + 18 figures)

References in corpus (41)

• Electric Field Effect in Atomically Thin Carbon Films
• Two Dimensional Atomic Crystals
• Van der Waals heterostructures
• 2D materials and van der Waals heterostructures
• High-mobility transport anisotropy and linear dichroism in few-layer black phosphorus
• Wannier90: A Tool for Obtaining Maximally-Localised Wannier Functions
• Tunable Band Gap and Anisotropic Optical Response in Few-layer Black Phosphorus
• Optical Spectrum of MoS${}_2$: Many-body Effects and Diversity of Exciton States
• The Renaissance of Black Phosphorus
• High Electron Mobility, Quantum Hall Effect and Anomalous Optical Response in Atomically Thin InSe
• The Computational 2D Materials Database: High-Throughput Modeling and Discovery of Atomically Thin Crystals
• Ab initio calculation of excitonic effects in the optical spectra of semiconductors
• Interfacial Ferroelectricity by van-der-Waals Sliding
• Exciton Binding Energy of Monolayer WS2
• Recent Progress of the Computational 2D Materials Database (C2DB)
• Quasiparticle band structure based on a generalized Kohn-Sham scheme
• The GW compendium: A practical guide to theoretical photoemission spectroscopy
• Screening and Many-Body Effects in Two-Dimensional Crystals: Monolayer MoS${}_2$
• Measurement of high exciton binding energy in the monolayer transition-metal dichalcogenides WS2 and WSe2
• Quasiparticle spectra from a non-empirical optimally-tuned range-separated hybrid density functional
• Combining GW calculations with exact-exchange density-functional theory: An analysis of valence-band photoemission for compound semiconductors
• Solid-state optical absorption from optimally-tuned time-dependent range-separated hybrid density functional theory
• The dielectric genome of van der Waals heterostructures
• Toward a realistic description of multilayer black phosphorus: from $GW$ approximation to large-scale tight-binding simulations
• Cumulative Polarization Coexisting with Conductivity at Interfacial Ferroelectrics
• Electronic structure and phase stability of oxide semiconductors: Performance of dielectric-dependent hybrid functional DFT, benchmarked against $GW$ band structure calculations and experiments
• All-electron GW approximation with the mixed basis expansion based on the full-potential LMTO method
• Adequacy of Approximations in GW Theory
• Controlling interlayer excitons in MoS2 layers grown by chemical vapor deposition
• Native point defects in few-layer phosphorene
• The long-wavelength behaviour of the exchange-correlation kernel in the Kohn-Sham theory of periodic systems
• Out-of-plane orientation of luminescent excitons in atomically thin indium selenide flakes
• Band gaps of crystalline solids from Wannier-localization based optimal tuning of a screened range-separated hybrid functional
• Experimental and theoretical electronic structure of quinacridone
• Exciton states in monolayer MoSe2 and MoTe2 probed by upconversion spectroscopy
• Accurate optical spectra through time-dependent density functional theory based on screening-dependent hybrid functionals
• Towards predictive band gaps for halide perovskites: Lessons from one-shot and eigenvalue self-consistent GW
• Band Structure, Band Offsets, Substitutional Doping, and Schottky Barriers in InSe
• An Optimally-Tuned Starting Point for Single-Shot $GW$ Calculations of Solids
• Range-Separated Hybrid Functionals for Mixed-Dimensional Heterojunctions: Application to Phthalocyanines/MoS2
• Interlayer and intralayer excitons in AlN/WS${}_2$ heterostructure

Cited by in corpus (8)

• Optical absorption spectra of metal oxides from time-dependent density functional theory and many-body perturbation theory based on optimally-tuned hybrid functionals
• Critical assessment of $G_0{W}_0$ calculations for 2D materials: the example of monolayer MoS${}_2$
• Low-scaling GW algorithm applied to twisted transition-metal dichalcogenide heterobilayers
• Spin-orbit torque in single-molecule junctions from ab initio
• Accurate and efficient prediction of the band gaps and optical spectra of chalcopyrite semiconductors from a non-empirical range-separated dielectric-dependent hybrid: Comparison with many-body perturbation theory
• Advancing excited-state properties of two-dimensional materials using a dielectric-dependent hybrid functional
• Many-body perturbation theory with hybrid density functional theory starting points accelerated by adaptively compressed exchange
• Optical excitations in nanographenes from the Bethe-Salpeter equation and time-dependent density functional theory: absorption spectra and spatial descriptors