Temperature-Dependent Full Spectrum Optical Responses of Semiconductors from First Principles

Abstract

From ultraviolet to mid-infrared region, light-matter interaction mechanisms in semiconductors progressively shift from electronic transitions to phononic resonances and are affected by temperature. Here, we present a parallel temperature-dependent treatment of both electrons and phonons entirely from first principles, enabling the prediction of full-spectrum optical responses. At elevated temperatures, $\text{ab initio}$ molecular dynamics is employed to find thermal perturbations to electronic structures and construct effective force constants describing potential landscape. Four-phonon scattering and phonon renormalization are included in an integrated manner in this approach. As a prototype ceramic material, cerium dioxide (CeO${}_2$) is considered in this work. Our first-principles calculated refractive index of CeO${}_2$ agrees well with measured data from literature and our own temperature-dependent ellipsometer experiment.

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Cited by in corpus (1)

• Consistency between the Green-Kubo formula and Lorentz model for predicting the infrared dielectric function of polar materials