First-principles predictions of temperature-dependent infrared dielectric function of polar materials by including four-phonon scattering and phonon frequency shift

Recently, first-principles calculations based on density functional theory have been widely used to predict the temperature-dependent infrared spectrum of polar materials, but the calculations are usually limited to the harmonic frequency (0 K) and three-phonon scattering damping for the zone-center infrared-active optical phonon modes, and fail to predict the high-temperature infrared optical properties of materials such as sapphire (alpha-Al2O3), GaAs, TiO2, etc., due to the neglect of high-order phonon scattering damping and phonon frequency shift. In this work, we implemented first-principles calculations to predict the temperature-dependent infrared dielectric function of polar materials by including four-phonon scattering and phonon frequency shift. The temperature-dependent phonon damping by including three- and four-phonon scattering as well as the phonon frequency shift by including cubic and quartic anharmonicity and the thermal expansion effect are calculated based on anharmonic lattice dynamics method. The infrared dielectric function of alpha-Al2O3 is parameterized, and then the temperature-dependent infrared optical reflectance is determined. We find that our predictions agree better with the experimental data than the previous density functional theory-based methods. This work will help to effectively predict the thermal radiative properties of polar materials at elevated temperature, which is generally difficult to measure, and will enable predictive design of new materials for radiative applications.