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Chemical Physics Letters

Large amplitude ground state vibrational coherence induced by impulsive absorption in CsI. A computer simulation

Bernd Hartke, Ronnie Kosloff, Sanford Ruhman

Published Jun 1, 1989• 91 citations
Publisher
DOI
10.1016/0009-2614(89)87328-2

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Computer simulations are presented to show that frequency-chirped ultrashort pulses, when properly employed, may be more effective than their compressed analogs for generating large-amplitude vibrational coherence in molecular systems. A one-dimensional model, which was used previously to simulate impulsive optical excitation of CsI, is used [ Chem. Phys. Lett.158, 238 ( 1988)]. A negatively chirped pulse (for which the light is red-shifted with time) is devised to excite the population initially onto the excited surface. As this population propagates in the repulsive upper state, the later red-shifted portions of the pulse follow the change in the resonance conditions and effectively dump the population back down into excited vibrational states of the ground surface. These results are compared with the dynamics simulated with the compressed and positively chirped analogs, and the experimental realization of this scheme is discussed.
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.