Time‐Dependent Density Functional Theory of Narrow Band Gap Semiconductors Using a Screened Range‐Separated Hybrid Functional

Abstract Predicting the band structure and optical absorption spectra of narrow band gap semiconductors is challenging for electronic structure methods. Here, it is shown shown that density functional theory can yield accurate band structures and time‐dependent density functional theory (TDDFT) can yield accurate optical absorption spectra for these systems. This is achieved by using a screened range‐separated hybrid (SRSH) functional with a single empirical parameter, fit to reproduce the experimental band gap. By comparing TDDFT results based on the SRSH approach with those obtained based on the Heyd–Scuseria–Ernzerhof functional it is shown that screened long‐range exact exchange improves the accuracy of the TDDFT spectra for these systems.