MIXED QUANTUM/CLASSICAL APPROACH TO PHOTODISSOCIATION OF $H_{2}O$ AND $Ar - H_{2}O$

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2003

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Ohio State University

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Recently, experimental studies of the vibrationally mediated photodissociation of $H_{2}O$ in $Ar - H_{2}O$ van der Waal complexes have been reported. In these studies, the OH rotational distributions were measured and compared with the ones that resulted from the photodissociation of $H_{2}O$ at the same photolysis $wavelengths.^{a}$ Much warmer OH rotational distributions were obtained from photolysis of the $Ar - H_{2}O$ clusters. In order to understand the physical origins of these results we have simulated the photodissociation of $H_{2}O$ and $Ar - H_{2}O$ using a multiple configuration mixed quantum/classical approach. By comparing the rotational distribution of the OH products that are obtained from photodissociation of the complexed and uncomplexed water molecules, we find that the Ar atom has a strong effect on the rotational distribution of the OH fragment in intracluster collisions. The simulations provide insights to the dynamics of photodissociation in clusters.

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$^{a}$Votava, O.; Plusquellic, D. F.; Myers, T. L.; Nesbitt, D. J. J. Chem. Phys. 112, 7449 (2002).
Author Institution: Department of Chemistry, The Ohio State University

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