BSE+ calculations for 2D materials: a unified description of excitons and plasmons

Abstract

The Bethe-Salpeter equation (BSE) accurately describes low-energy optical spectra in materials with strong excitonic effects, but its high computational cost limits the number of electron-hole transitions that can be included. Neglecting high-energy transitions leads to an underestimation of the real part of the dielectric function, often producing a spurious plasmon peak in the BSE electron energy loss spectrum (EELS). The recently introduced BSE+ method addresses this by combining a four-point BSE-like equation for the irreducible polarisability with a two-point Dyson equation that includes the high-energy transitions at the Random Phase Approximation (RPA) level. Here, we present a detailed account of the method, extend it to two-dimensional materials, and apply it to a set of transition metal dichalcogenide monolayers. BSE+ preserves the excitonic features of the BSE at low energies while reproducing the plasmonic structure of the RPA at higher energies, yielding good agreement with experimental EELS data across the full energy range and strongly suppressing the spurious plasmon. BSE+ converges much faster than BSE with respect to the electron-hole basis size, at a comparable computational cost, and is implemented in the GPAW code.