Diamond two-phonon infrared absorption spectrum calculated from first principles using the finite displacement method

Abstract

We calculate the two-phonon contribution to the dielectric susceptibility of diamond at room and elevated temperatures, utilizing a general ab initio model that can be extended to higher n phonon processes. We calculate the second-order dipole moments using a finite displacement method to calculate the derivatives of the Born effective charge tensor. Specifically, we use results obtained from density-functional theory and density-functional perturbation theory in this finite displacement method to calculate the dipole moments of diamond in the two-phonon case. We use the calculated dipole moment to determine the contribution of two-phonon processes to the dielectric susceptibility. We then calculate the absorption curve as a function of wave-number at room or elevated temperatures. Our results indicate that the calculated absorption is in good agreement with previous calculations, and that it increases in magnitude with temperature while maintaining a consistent shape.