Abstract

Optical control of elementary molecular motion through impulsive stimulated Raman scattering is enhanced by means of timed sequences of femtosecond pulses that are produced by pulse-shaping techniques. In particular, terahertz-rate trains of femtosecond pulses are used for repetitive impulsive excitation of individual phonon modes in an α-perylene molecular crystal. When the pulse repetition rate is matched to the desired phonon frequency, mode-selective vibrational amplification is achieved. A comparison of data acquired with the transient-grating and the pump–probe experimental geometries reveals the timing dynamics of the induced phonon oscillations with respect to the driving femtosecond pulse sequence.

© 1991 Optical Society of America

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