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Optimal Sequences for Chirped-Pulse Stimulated Raman Preparation of Large Amplitude Vibrational Motion

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Abstract

Recent calculations [1, see also 2-5] indicate that suitably timed sequences of electronically preresonant femtosecond laser pulses can induce large amplitude coherent molecular vibrations of dilute chromophores in low temperature hosts, without undue electronic absorption or other loss processes. Here we demonstrate that frequency modulation, in the forms of variable pulse center frequency and variable chirp rate, can significantly further enhance the efficiency of impulsive stimulated Raman preparation of coherent vibrations in the electronic ground state.

© 1996 Optical Society of America

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