Wigner-Seitz truncated TDDFT approach for the calculation of exciton binding energies in solids

Abstract

Time-Dependent Density Functional Theory (TDDFT) has been currently established as a computationally cheaper, yet effective, alternative to the Many-Body Perturbation Theory (MBPT) for calculating the optical properties of solids. Within the Linear Response formalism, the optical absorption spectra are in good agreement with experiments, as well as the direct determination of the exciton binding energies. However, the family of exchange-correlation kernels known as long-range corrected (LRC) kernels that correctly capture excitonic features have difficulties simultaneously producing good-looking spectra and accurate exciton binding energies. More recently, this discrepancy has been partially overcome by a hybrid-TDDFT approach. We show that the key resides in the numerical treatment of the long-range Coulomb singular term. We carefully study the effect of this term, both in the pure-TDDFT and hybrid approach using a Wigner-Seitz truncated kernel. We find that computing this term presents technical difficulties that are hard to overcome in both approaches, and that points to the need for a better description of the electron-hole interaction.

References in corpus (15)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• BerkeleyGW: A Massively Parallel Computer Package for the Calculation of the Quasiparticle and Optical Properties of Materials and Nanostructures
• The Quantum-Mechanical Position Operator in Extended Systems
• Bootstrap approximation for the exchange-correlation kernel of time-dependent density functional theory
• Ideal regularization of the Coulomb singularity in exact exchange by Wigner-Seitz truncated interactions: towards chemical accuracy in non-trivial systems
• Excitonic optical spectrum of semiconductors obtained by time-dependent density-functional theory with the exact-exchange kernel
• Exact Kohn-Sham exchange kernel for insulators and its long-wavelength behavior
• Estimating Excitonic Effects in the Absorption Spectra of Solids: Problems and Insight from a Guided Iteration Scheme
• Direct calculation of exciton binding energies with time-dependent density-functional theory
• Time-dependent density-functional approach for exciton binding energies
• Assessment of long-range-corrected exchange-correlation kernels for solids: accurate exciton binding energies via an empirically scaled Bootstrap kernel
• Fully parameter-free calculation of optical spectra for insulators, semiconductors and metals from a simple polarization functional
• Optical properties of CsCu${}_2$X${}_3$ (X=Cl, Br and I): A comparative study between hybrid time-dependent density-functional theory and the Bethe-Salpeter equation
• Accurate optical spectra of solids from pure time-dependent density-functional theory
• Excitonic effects in time-dependent density functional theory from zeros of the density response