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Chemical Physics

Vibrationally state-selective laser pulse control of electronic branching in OH (X/A) photoassociation

M. V. Korolkov, Burkhard Schmidt

Published Oct 1, 1998• 13 citations
Publisher
DOI
10.1016/s0301-0104(98)00219-5

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Photoassociation via reverse ladder transition controlled by two and four laser pulses is investigated using the time-dependent quantum wave packet method. The calculated results show that the amplitudes of the pulses have an enormous effect on the target population and total yield of association. For the target state with a high energy level, the population of background states can reduce the state-selectivity. Although, the total yield of association is decreased, the four pulses can induce the population transferring to low vibrational levels, and the state-selectivity of the target state is high.
Laser-controlled ultrafast state-selective vibrational dynamics of diatomic molecules, which are coupled to an unobserved quasiresonant environment is investigated using the reduced density-matrix formalism beyond and within a Markov-type approximation. Dissipative quantum dynamics in a classical electric field of shaped infrared ultrashort laser pulses is simulated for a one-dimensional nondissociative Morse oscillator, representing the local OH bond in the H2{\mathrm{H}}_{2}H2​ O and HOD molecules in the electronic ground state. Localization of population at a prescribed vibrational target level of OH up to v=10 with probability of about 90% is demonstrated on a picosecond time scale, while the strength of the quasiresonant molecule-environment coupling results in subpicosecond lifetimes of the vibrational states. The laser-controlled stabilization of selective excitation in the restricted set of vibrational states against a background of strongly diminished relaxation to lower vibrational states is also shown. The laser-control scheme may include a superposition of several laser pulses. A Markov-type approximation results in slightly increased lifetimes of the vibrational states, along with decreased predicted probability of state-selective excitation of a molecule by about 20--30%. Several results obtained within the fourth-order perturbation theory in interaction of a molecule with an environment are in a good agreement with the non-Markov analysis.