Campus Units

Physics and Astronomy, Ames Laboratory

Document Type

Article

Publication Version

Published Version

Publication Date

5-2014

Journal or Book Title

Journal of Chemical Physics

Volume

140

Issue

19

First Page

194704-1

Last Page

194704-13

DOI

10.1063/1.4875813

Abstract

We develop statistical mechanical models amenable to analytic treatment for the dissociative adsorption of O2 at hollow sites on fcc(100) metal surfaces. The models incorporate exclusion of nearest-neighbor pairs of adsorbed O. However, corresponding simple site-blocking models, where adsorption requires a large ensemble of available sites, exhibit an anomalously fast initial decrease in sticking. Thus, in addition to blocking, our models also incorporate more facile adsorption via orientational steering and funneling dynamics (features supported by ab initio Molecular Dynamics studies). Behavior for equilibrated adlayers is distinct from those with finite adspecies mobility. We focus on the low-temperature limited-mobility regime where analysis of the associated master equations readily produces exact results for both short- and long-time behavior. Kinetic Monte Carlo simulation is also utilized to provide a more complete picture of behavior. These models capture both the initial decrease and the saturation of the experimentally observed sticking versus coverage, as well as features of non-equilibrium adlayer ordering as assessed by surface-sensitive diffraction.

Comments

The following article appeared in Journal of Chemical Physics 140, 19 (2014): 194704 and may be found at doi: 10.1063/1.4875813.

Rights

Copyright 2014 American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics.

Copyright Owner

American Institute of Physics

Language

en

File Format

application/pdf

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