Repository: Freie Universit├Ąt Berlin, Math Department

Effect of Rotations and Shape Resonances on Photoassociation and Photoacceleration by Ultrashort Infrared Laser Pulses

Backhaus, P. and Manz, J. and Schmidt, B. (1998) Effect of Rotations and Shape Resonances on Photoassociation and Photoacceleration by Ultrashort Infrared Laser Pulses. J. Phys. Chem. A, 102 (23). pp. 4118-4128.

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Official URL: http://dx.doi.org/10.1021/jp9800057

Abstract

A quantum dynamical description of an atomic collision pair interacting with the electric field of a short infrared laser pulse is developed. Inelastic processes in the electronic ground state are due to stimulated emission resulting in photoassociation, or absorption leading to photoacceleration. A perturbative approach based on a state space representation is compared with a numerical treatment using a grid representation in coordinate space. Special emphasis is on the role of rotations and, in particular, of shape resonances. It is shown that these quasibound states which are supported by the centrifugal barrier (for J> 0) can be used as initial states to effectively populate a selected bound state with specific vibrational and rotational quantum number (photoassociation), or a partial wave of a scattering state with defined energy and rotational quantum number (photoacceleration). Simulations are carried out for the prototype H + Cl collision pair. Also the effect of averaging over initial conditions (velocity, angular momenta) is investigated for a supersonic beam experiment. For a narrow velocity distribution, we predict the presence of a resonance structure of the association and acceleration probability as a function of the mean collision energy.

Item Type:Article
Subjects:Physical Sciences > Physics > Mathematical & Theoretical Physics > Computational Physics
Physical Sciences > Chemistry > Physical Chemistry
Physical Sciences > Physics > Chemical Physics
ID Code:857
Deposited By: Burkhard Schmidt
Deposited On:15 Mar 2010 09:21
Last Modified:03 Mar 2017 14:40

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