Oscillatory femtosecond relaxation of photoexcited organic molecules

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Abstract
The ultrafast relaxation of large organic molecules in solution has been investigated with the transmission correlation technique. The existence of damped sinusoidal decays after photoexcitation has been verified for several organic dyes. This behavior (the first such decay observed on a femtosecond time scale for any material) is explained as quantum beats. For all molecules examined, we have also observed fast initial exponential decays (<100 fs) in addition to previously known picosecond processes.