Vibrational dephasing in crystals: Theory and experiment

Abstract

Vibrational lineshapes of molecules in crystals are determined to a large extent by the vibration-phonon coupling. We show how our previously developed nonperturbative theory of optical pure dephasing can be applied to the vibrational dephasing problem. We consider two cases: dephasing in a pure crystal, and dephasing of a substitutional impurity. We compare our theoretical results to temperature-dependent linewidth and lineshift measurements on the 766 cm −1 mode in pure naphthalene, and the V 3 mode of ReO 4 − in KI.