One-shot calculation of temperature-dependent optical spectra and phonon-induced band-gap renormalization

Electron-phonon interactions are of fundamental importance in the study of the optical properties of solids at finite temperatures. Here we present a new first-principles computational technique based on the Williams-Lax theory for performing predictive calculations of the optical spectra, including quantum zero-point renormalization and indirect absorption [1]. The calculation of the Williams-Lax optical spectra is computationally challenging, as it involves the sampling over all possible nuclear quantum states. We develop an efficient computational strategy for performing "one-shot" finite-temperature calculations [2]. These require only a single optimal configuration of the atomic positions. We demonstrate our methodology for the case of Si, C, and GaAs, yielding absorption coefficients in good agreement with experiment. This work opens the way for systematic calculations of optical spectra at finite temperature. [1] M. Zacharias, C. E. Patrick, and F. Giustino, Phys. Rev. Lett. 115, 177401 (2015). [2] M. Zacharias and F. Giustino, Phys. Rev. B 94, 075125 (2016).