An experimental setup for molecular beam scattering from flat liquid sheets has been developed, with the goal of studying reactions at gas-liquid interfaces for volatile liquids. Specifically, a crossed molecular beam instrument that can measure angular and translational energy distributions of scattered products has been adapted for liquid jet scattering. A microfluidic chip is used to create a stable flat liquid sheet inside vacuum from which scattering occurs, and both evaporation and scattering from this sheet are characterized by a rotatable mass spectrometer that can measure product time-of-flight distributions. This manuscript describes the instrument and reports on first measurements of evaporation of dodecane and Ne from a Ne-doped dodecane flat jet, as well as scattering of Ne from a flat jet of pure dodecane.
Photofragment translational spectroscopy was used to study the photodissociation of fulvenallene, CH, and the fulvenallenyl radical, CH, at 248 nm and 193 nm. Starting from fulvenallene, only the H-atom loss channel producing the fulvenallenyl radical, CH, was observed. Fulvenallene dissociation occurs on the ground state surface with no exit barrier, and there is good agreement between our experimentally determined photofragment translational energy distribution and a prior distribution for a statistical process. Subsequent absorption at both wavelengths by fulvenallenyl enabled investigation of the photodissociation of this radical. Two channels were observed: CH + CH and CH + CH. The photofragment translational energy distributions for these channels are peaked away from 0 kcal mol, which is consistent with ground state dissociation over an exit barrier. At 248 nm, the CH-loss channel accounted for 85 ± 10% of fulvenallenyl dissociation, while at 193 nm it accounted for 80 ± 15%. The experimental branching between these channels is in reasonable agreement with Rice-Ramsperger-Kassel-Marcus theory calculations, which predict CH-loss to account for 70% and 63% of dissociation for 248 nm and 193 nm respectively.
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