Optical properties of bulk semiconductors and graphene/boron-nitride: The Bethe-Salpeter equation with derivative discontinuity-corrected DFT energies

Abstract

We present an efficient implementation of the Bethe-Salpeter equation (BSE) for optical properties of materials in the projector augmented wave method GPAW. Single-particle energies and wave functions are obtained from the GLLBSC functional which explicitly includes the derivative discontinuity, is computationally inexpensive, and yields excellent fundamental gaps. Electron-hole interactions are included through the BSE using the statically screened interaction evaluated in the random phase approximation. For a representative set of semiconductors and insulators we find excellent agreement with experiments for the dielectric functions, onset of absorption, and lowest excitonic features. For the two-dimensional systems of graphene and hexagonal boron-nitride (h-BN) we find good agreement with previous many-body calculations. For the graphene/h-BN interface, we find that the fundamental and optical gaps of the h-BN layer are reduced by 2.0 eV and 0.7 eV, respectively, compared to freestanding h-BN. This reduction is due to image charge screening which shows up in the GLLBSC calculation as a reduction (vanishing) of the derivative discontinuity.

arXiv comment12 pages, 2 tables, 5 figures

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• Interlayer excitons and Band Alignment in MoS${}_2$/hBN/WSe${}_2$ van der Waals Heterostructures
• Quasiparticle GW calculations for solids, molecules and 2D materials
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• High-throughput Density Functional Perturbation Theory and Machine Learning Predictions of Infrared, Piezoelectric and Dielectric Responses
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• Assessment of the GLLB-SC potential for solid-state properties and attempts for improvement
• Dimensionality of excitons in stacked van der Waals materials: The example of hexagonal boron nitride
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• A method to restore the intrinsic dielectric functions of 2D materials in periodic calculations and its applications to the dielectric and optical properties of ultrathin h-BN and MoS2
• Ab initio study of electromagnatic modes in two-dimensional semiconductors: Application to doped phosphorene
• Structural, electronic, and optical properties of periodic graphene/h-BN van der Waals heterostructures
• Computing Optical Properties of Ultra-thin Crystals
• Gap control in phosphorene/BN structures from first principles calculations
• Cavity exciton-polaritons in two-dimensional semiconductors from first principles
• Expeditious computation of nonlinear optical properties of arbitrary order with native electronic interactions in the time domain
• Graphics Processing Unit acceleration of the Random Phase Approximation in the projector augmented wave method
• Electron energy-loss spectrum and exciton band structure of ${\mathrm{WSe}}_2$ monolayer studied by ab initio Bethe-Salpeter equation calculations
• Strong 1D localization and highly anisotropic electron-hole masses in heavy-halogen functionalized graphenes
• Chemical potential, derivative discontinuity, fractional electrons, jump of the Kohn-Sham potential, atoms as thermodynamic open systems, and other (mis)conceptions of the density functional theory of electrons in molecules