Abstract
Vibronic relaxation processes of large molecules in the condensed phase, which occur on an ultrafast time scale, have been the subject of numerous time-resolved experiments in the regime between 100 fs and several picoseconds,1 Recently, high-repetition-rate solid-state lasers have become available for the generation of pulses of less than 30-fs duration,2·3 allowing the investigation of relaxation steps in time intervals of several tens of femtoseconds, i.e., comparable to vibrational periods of the molecules. In this paper we describe a study of the relaxation of high-lying singlet S„ states in organic-dye molecules in two-color pump-probe measurements with an unprecedented time resolution of about 20 fs, providing new insight into femtosecond material excitations and ultrafast internal conversion processes.
© 1995 Optical Society of America
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