The electronic dephasing of large molecules in solution is investigated with three-pulse photon echoes generated by 6-fs optical pulses. The observed dephasing behavior, which is analyzed with a model based on a stochastic coupling of the molecules with their heat bath, is clearly shown to be non-Markovian. Moreover, the correlation function of the fluctuations asymptotically approaches an exponential with characteristic times varying from 20 to 80 fs, depending on the solvent environment.

• Received 6 September 1990

DOI:https://doi.org/10.1103/PhysRevLett.66.1138