Abstract

We report results of an optical and picosecond photon echo study on the zero-phonon line of photosite I of pentacene in benzoic acid. The results show that optical dephasing in this system proceeds via uncorrelated phonon scattering processes from the ground and optically excited state to singly-excited librational levels. It is also shown that the data can not be consistently interpreted using coherence exchange theory. The librational frequencies and lifetimes at low temperature are determined to be 12 cm and 18 psec in the ground state and 16.7 cm-1and 2.5 psec in the singlet excited state. It is argued that population decay of librational overtones proceeds in single quantum steps down the librational ladder which excludes these modes from playing a role in optical dephasing.

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