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Bond-Breaking in Quantum State Selected Clusters: Inelastic and Nonadiabatic Intracluser Collision Dynamics in Ar-H2O -> Ar + (2S)+ OH(2Π 1/2, 3/2;N)



O Votava, David F. Plusquellic, T L. Myers, David Nesbitt


High resolution vibrationally mediated IR + UV photodissociation methods are used to investigate the dvnamics of H-OH bond breaking in quantum state selected H2O and Ar-H2O van der Waal complexes prepared in a slit supersonic jet expansion. This capability is based on the following strategy: (i) Specific rovibrational quantum states of AR-H2O dimer and H2O monomer are optically selected in the second overtone (vOH = 3-0) region with an injection seeded, Fourierr transform limited (δŅ nearly equal to} 160 MHz) optical parametric oscillator. (ii) Selective H-OH bond cleavage of the vibrationally excited H2O subunit in the cluster is achieved by 248 nm UV photolysis. (iii) Multibody collision dynamics between the H. OH, and Ar photofragments are probed via laser induced fluorescence (LIF) on the asymptotic OH rotational,lambda-doublet and spin-orbit distributions. Comparison between cIuster (Ar-H2O) and monomer (H2,O) data explicitly samples the influenceof the Ar solvent on the UV photolysis dynamics and in particular highlights the dominant role of intracluster collisions as the fragments recoil. Most importantly the OH fine structure distributions are found to be dramatically different for Ar-H_O vs H_O photolysis, indicating the major contribution on non-adiabatic surface hopping events in the photofragmentation dynamics.
Journal of Chemical Physics
No. 17


collision dynamics, laser-induced fluorescence, photodissociation, quantum state clusters


Votava, O. , Plusquellic, D. , Myers, T. and Nesbitt, D. (2000), Bond-Breaking in Quantum State Selected Clusters: Inelastic and Nonadiabatic Intracluser Collision Dynamics in Ar-H<sub>2</sub>O -> Ar + (<sup>2</sup>S)+ OH(<sup>2</sup>&#928;<sup> </sup>1/2, 3/2;N), Journal of Chemical Physics (Accessed July 15, 2024)


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Created April 30, 2000, Updated October 12, 2021