Estimating Excitonic Effects in the Absorption Spectra of Solids: Problems and Insight from a Guided Iteration Scheme

Abstract

A major obstacle for computing optical spectra of solids is the lack of reliable approximations for capturing excitonic effects within time-dependent density-functional theory. We show that the trustful prediction of strongly bound electron-hole pairs within this framework using simple approximations is still a challenge and that available promising results have to be revisited. Deriving a set of analytical formula we analyze and explain the difficulties. We deduce an alternative approximation from an iterative scheme guided by previously available knowledge, significantly improving the description of exciton binding energies. Finally, we show how one can "read" exciton binding energies from spectra determined in the random phase approximation, without any further calculation.

arXiv comment5 pages, 2 figures plus supplemental material

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Cited by in corpus (20)

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• All-electron quasi-particle self-consistent $GW$ band structures for SrTiO${}_3$ including lattice polarization corrections in different phase
• 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
• Non-local and non-adiabatic effects in the charge-density response of solids: a time-dependent density functional approach
• Dielectrics in a time-dependent electric field: a real-time approach based on density-polarization functional theory
• Accurate optical spectra of solids from pure time-dependent density-functional theory
• All-electron full-potential implementation of real-time TDDFT in exciting
• Intricate modulation of interlayer coupling at GO/MoSe2 interface: application in time-dependent optics and device transport
• A Snapshot of Time-Dependent Density-Functional Theory
• 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
• Exact exchange-correlation kernels for optical spectra of model systems
• Optical spectra of 2D monolayers from time-dependent density functional theory
• Including many-body effects into the Wannier-interpolated quadratic photoresponse tensor
• First-principles study of excitons in the optical spectra of silver chloride
• Excitonic effects in time-dependent density functional theory from zeros of the density response
• Wigner-Seitz truncated TDDFT approach for the calculation of exciton binding energies in solids
• Progress towards understanding ultranonlocality through the wavevector and frequency dependence of approximate exchange-correlation kernels
• Comparison of long-range corrected kernels and range-separated hybrids for excitons in solids