A first-principles molecular dynamics approach for predicting optical phonon lifetimes and far-infrared reflectance of polar materials

The Lorentz oscillator model is well-known for its effectiveness to describe the far-infrared optical properties of polar materials. The oscillator strength and damping factor in this model are usually obtained by fitting to experimental data. In this work, a method based on first-principles simulations is developed to parameterize the Lorentz oscillator model without any fitting parameters. The high frequency dielectric constant is obtained from density functional perturbation theory, while the optical phonon frequencies and damping factors are calculated using an analysis of ab initio molecular dynamics trajectories. This method is then used to predict the far-infrared properties of GaAs, and the results are in good agreement with experimental data.

► The relationship between the Lorentz oscillator model and the optical phonon properties is discussed. ► First-principles simulations are applied to parameterize the Lorentz model. ► The far-infrared reflectance of GaAs is predicted.