Abstract

A three-dimensional quantum mechanical study of the control of a branching photochemical reaction H+OD←DOH→D+OH is presented. It is shown that with two laser pulses, one pulse used to generate a superposition of the (0,2,0) and the (1,0,0) states, and the other, a VUV pulse, used to dissociate the molecule by exciting it to the B continuum, it is possible to control which of two chemical channels is preferred. The control parameters used are the center frequency of the excitation laser and the time delay between the two pulses. For the above superposition state, a combination of a 200 fs excitation pulse and a 50 fs dissociation pulse is found to yield the widest (10% to 90% yield in the H+OD channel) range of control, essentially irrespective of the photolysis wavelength.

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