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Coherent effects of intense ultrashort optical pulses on diatomic molecules

Karen E. Hill

Published Jan 1, 1990• 0 citations
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Physical Review A•Mar 25, 2008•19 citations
In the present work we analyze the dipole response of a diatomic heteronuclear molecule on the nonperturbative action of the external low-frequency laser field. Main results are obtained by numerical solution of the time-dependent Schrodinger equation for the nuclear subsystem of the molecule. We study the spectrum of polarization response and the influence of the coherent repopulation of the ro-vibrational states on it. Generally, we consider two cases: repopulation due to Raman-type transitions leading to the interference stabilization of the molecule and repopulation arising as a result of extremely short pulse action. We also study the transformation of a weak probe pulse propagating through the highly excited medium of the studied molecules.
In this paper, I discuss the selective and efficient vibrational population transfer between electronic states of diatomic molecules by a weak, ultrashort pulse train. The spectrum of each individual pulse in the train is wide enough to simultaneously excite several vibrational levels of the molecule. However, selectivity is achieved by mismatching the frequency comb, associated with the pulse train, to the excited vibrational levels. Efficiency results from the coherent accumulation of population from one pulse in the train to the next.