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Issue 12, 2012
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State-resolved velocity map imaging of surface-scattered molecular flux

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Abstract

This work describes a novel surface-scattering technique which combines resonance enhanced multiphoton ionization (REMPI) with velocity-map imaging (VMI) to yield quantum-state and 2D velocity component resolved distributions in the scattered molecular flux. As an initial test system, we explore hyperthermal scattering (Einc = 21(5) kcal mol−1) of jet cooled HCl from Au(111) on atomically flat mica surfaces at 500 K. The resulting images reveal 2D (vin-plane and vout-of-plane) velocity distributions dominated by two primary features: trapping/thermal-desorption (TD) and a hyperthermal, impulsively scattering (IS) distribution. In particular, the IS component is strongly forward scattered and largely resolved in the velocity map images, which allows us to probe correlations between rotational and translational degrees of freedom in the IS flux without any model dependent deconvolution from the TD fraction. These correlations reveal that HCl molecules which have undergone a large decrease in velocity parallel to scattering plane have actually gained the most rotational energy, reminiscent of a dynamical energy constraint between these two degrees of freedom. The data are reduced to a rotational energy map that correlates 〈Erot〉 with velocity along and normal to the scattering plane, revealing that exchange occurs primarily between rotation and the in-plane kinetic energy component, with vout-of-plane playing a relatively minor role.

Graphical abstract: State-resolved velocity map imaging of surface-scattered molecular flux

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Article information


Submitted
14 Sep 2011
Accepted
16 Nov 2011
First published
09 Dec 2011

Phys. Chem. Chem. Phys., 2012,14, 4070-4080
Article type
Paper

State-resolved velocity map imaging of surface-scattered molecular flux

J. R. Roscioli, D. J. Bell, D. J. Nelson and D. J. Nesbitt, Phys. Chem. Chem. Phys., 2012, 14, 4070
DOI: 10.1039/C1CP22938A

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