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Bulletin of the American Physical Society

Characterization of transient molecular vibrations on the way towards coherently controlled vibrational target state

Stanislav O. Konorov, Xiaoji G. Xu, John W. Hepburn, Valery Milner

Published May 20, 2009• 0 citations
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A model of two-level weakly interacting quantum systems is used to demonstrate that the phase of molecular vibrations excited through stimulated Raman scattering can be controlled by the relative phase of time-separated laser pulses, allowing synchronization and amplitude control of coherence excitation in a medium. For transients with a phase relaxation time less than the field cycle, the field half-cycle can serve as a subfemtosecond probe of coherent vibrations. In this regime, the high-frequency field-induced modulation of molecular dipole moments gives rise to a detectable modulation of the optical response of a medium at the frequency $2\ensuremath{\omega}$, $\ensuremath{\omega}$ being the frequency of the laser field.