Campus Units

Chemistry, Mathematics, Physics and Astronomy, Ames Laboratory

Document Type

Article

Publication Version

Published Version

Publication Date

11-2011

Journal or Book Title

Journal of Physical Chemistry C

Volume

115

Issue

47

First Page

23488

Last Page

23500

DOI

10.1021/jp208410t

Abstract

Ab initio electronic structure theory was used to model systems that depict Ga and Ga2adsorbed on the Si(100)-2 × 1 reconstructed surface. The prototypical Si15H16 molecular cluster based on quantum mechanics (QM) was used to model the Si(100)-2 × 1 reconstructed surface. A larger Si199H92 molecular cluster based on a hybrid quantum mechanics molecular mechanics (QM/MM) methodology was used to incorporate bulk substrate effects on the adsorbed species. Since the Si(100)-2 × 1 reconstructed surface is comprised of Si dimers that exhibit significant diradical character, multiconfiguration self-consistent field (MCSCF) methodology was used to treat the relevant potential energy surfaces. Hessian calculations were used to characterize all structures, while intrinsic reaction coordinate (minimum energy path) computations were performed to validate the potential energy surface. Dynamic correlation effects were computed at MCSCF optimized structures by multireference second-order perturbation theory. Results from the two cluster models were compared to assess the need to include bulk effects in the surface model.

Comments

Reprinted (adapted) with permission from Journal of Physical Chemistry C 115 (2011): 23488, doi:10.1021/jp208410t. Copyright 2011 American Chemical Society.

Copyright Owner

American Chemical Society

Language

en

File Format

application/pdf

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