What Determines the Sticking Probability of Water Molecules on Ice?

Enrique R. Batista, Patrick Ayotte, Ante Bilić, Bruce D. Kay, and Hannes Jónsson

Phys. Rev. Lett. 95, 223201 – Published 22 November 2005

Abstract

We present both experimental and theoretical studies of the sticking of water molecules on ice. The sticking probability is unity over a wide range in energy (0.5 eV–1.5 eV) when the molecules are incident along the surface normal, but drops as the angle increases at high incident energy. This is explained in terms of the strong orientational dependence of the interaction of the molecule with the surface and the time required for the reorientation of the molecule. The sticking probability is found to scale with the component of the incident velocity in the plane of the surface, unlike the commonly assumed normal or total energy scaling.

Received 15 July 2005

DOI:https://doi.org/10.1103/PhysRevLett.95.223201

Authors & Affiliations

Enrique R. Batista^1,*, Patrick Ayotte^2,†, Ante Bilić^1,‡, Bruce D. Kay², and Hannes Jónsson^1,3

¹Department of Chemistry 351700, University of Washington, Seattle, Washington 98195-1700, USA
²Chemical Sciences Division, Fundamental Science Directorate, Pacific Northwest National Laboratory, Richland, Washington 99352, USA
³Faculty of Science, VR-II, University of Iceland, 107 Reykjavík, Iceland

^*Current address: Los Alamos National Laboratory, Theoretical Division, MS B268, Los Alamos, NM 87545.
^†Current address: Dpt. de Chimie, Université de Sherbrooke, Sherbrooke, Canada, J1K 2R1.
^‡Current address: Nanochemistry Research Institute, Curtin U. of Technology, Perth 6845 WA, Australia.

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Issue

Vol. 95, Iss. 22 — 25 November 2005

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Images

Figure 1
Measured and calculated sticking coefficient as a function of incident angle at two different values of the incident kinetic energy. The filled circles and boxes show the experimental results for 0.5 eV and 1.5 eV, respectively. The open circles and boxes show the corresponding results of classical dynamics calculations. At high energy, the sticking coefficient decreases with incident angle, opposite to the commonly assumed normal energy scaling.Reuse & Permissions
Figure 2
Experimental and theoretical results on the sticking probability of a water molecule impinging on an ice surface as a function of the incident velocity component that lies in the surface plane. The incident energy ranged from 0.5 eV to 1.5 eV and incident angle from 0 to 75 degrees. The drop in the sticking probability at large incident energy and angle is found to scale well with the component of the incident velocity in the plane of the surface. The error bars (omitted for clarity) in the experimental measurements are estimated to be $\pm 0.02$ . The apparent scatter in the experimental data lies within this uncertainty.Reuse & Permissions
Figure 3
Left: side view of the two types of binding sites for a water admolecule (shown in blue) on the surface of antiferroelectric ice, the A and B sites. In the former the admolecule points both of its H atoms towards the surface. In the B site one points towards the surface and the other points away from the surface. Right: on-top view of the minimum energy path between the two sites. The three underlying water molecules are shown in light blue and marked with the site type.Reuse & Permissions
Figure 4
An illustration of the variation of the molecule-surface interaction energy as the $H_{2} O$ molecule moves from one site to another on the ice surface. The lower energy curve shows the energy along the minimum energy path (MEP) between the A and B sites as a function of the total displacement of all the atoms in the system. The higher energy curve shows the variation in the potential energy as the O atom of the admolecule moves in the same way as in the minimum energy path, but the orientation of the molecule remains fixed as in the A site. This results in a large repulsive barrier. The variation of the potential energy with the distance of the admolecule from the surface is shown in the inset. Here, the orientation of the molecule is fixed at the one giving minimum energy at the A site. If the molecule is brought to the B site with that orientation, the interaction with the surface is purely repulsive. A molecule that does not have time to reorient as it moves from one site to another will, therefore, be subject to a large repulsive interaction with the surface.Reuse & Permissions

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