Optical Dephasing Due to Virtual Transfer of Excitation Energy as Observed in Photon Echo Experiments of Pentacene Molecules in Crystals

Abstract

Optical dephasing due to intermolecular interaction is studied for pentacence molecules introduced in naphthalene and p-terphenyl crystals by measuring the ordinary photon echo and the accumulated three-pulse echo. It is found that the reciprocal of pure dephasing time increases linearly with the guest molecule concentration at low temperature where pure dephasing is known to be temperature-independent. A new model based on virtual transfer of excitation energy, i.e. energy transfer without phonon asistance, between guest molecules is presented to interpret this dephasing process. It is shown that observed linear dependence of the line width representing pure dephasing is well interpreted by this model, and that the calculated relationship between the line width and concentration agrees with the experimental one within a factor of about two.