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F+OH reactive collisions on new excited 3A" and 3A' potential-energy surfaces.

Global three-dimensional adiabatic potential-energy surfaces for the excited 2(3)A" and 1(3)A' triplet states of OHF are obtained to study the F(2P)+OH(2pi)-->O(3P)+HF(1sigma+) reaction. Highly accurate ab initio calculations are obtained for the two excited electronic states and fitted to analytical functions with small deviations. The reaction dynamics is studied using a wave-packet treatment within a centrifugal sudden approach, which is justified by the linear transition state of the two electronic states studied. The reaction efficiency presents a marked preference for perpendicular orientation of the initial relative velocity vector and the angular momentum of the OH reagent, consistent in the body-fixed frame used with an initial collinear geometry which facilitates the access to the transition state. It is also found that the reaction cross section presents a rather high threshold so that, in an adiabatic picture, the two excited triplet states do not contribute to the rate constant at room temperature. Thus, only the lowest triplet state leads to reaction under these conditions and the simulated rate constants are too low as compared with the experimental ones. Such disagreement is likely to be due to nonadiabatic transitions occurring at the conical intersections near the transition state for this reaction.