Campus Units
Chemistry, Physics and Astronomy, Mathematics, Ames Laboratory
Document Type
Article
Publication Version
Published Version
Publication Date
4-2009
Journal or Book Title
Journal of Physical Chemistry C
Volume
113
Issue
17
First Page
7277
Last Page
7289
DOI
10.1021/jp8105937
Abstract
When group III metals are deposited onto the Si(100)-2 × 1 reconstructed surface they are observed to self-assemble into chains of atoms that are one atom high by one atom wide. To better understand this one-dimensional island growth, ab initio electronic structure calculations on the structures of Al atoms on silicon clusters have been performed. Natural orbital occupation numbers show that these systems display significant diradical character, suggesting that a multireference method is needed. A multiconfiguration self-consistent field (MCSCF) calculation with a 6-31G(d) basis set and effective core potentials was used to optimize geometries. The surface integrated molecular orbital molecular mechanics embedded cluster method was used to take the surface chemistry into account, as well as the structure of an extended surface region. Potential energy surfaces for binding of Al adatoms and Al−Al dimers on the surface were determined, and the former was used to obtain a preliminary assessment of the surface diffusion of adatoms. Hessians were calculated to characterize stationary points, and improved treatment of dynamic electron correlation was accomplished using multireference second order perturbation theory (MRMP2) single-point energy calculations. Results from the MRMP2//MCSCF embedded cluster calculations are compared with those from QM-only cluster calculations, embedded cluster unrestricted density functional theory calculations, and previous Car−Parrinello DFT studies.
Copyright Owner
American Chemical Society
Copyright Date
2009
Language
en
File Format
application/pdf
Recommended Citation
Zorn, Deborah; Albao, Marvin Argulla; Evans, James W.; and Gordon, Mark S., "Binding and Diffusion of Al Adatoms and Dimers on the Si(100)-2 × 1 Reconstructed Surface: A Hybrid QM/MM Embedded Cluster Study" (2009). Physics and Astronomy Publications. 198.
https://lib.dr.iastate.edu/physastro_pubs/198
Included in
Astrophysics and Astronomy Commons, Mathematics Commons, Physical Chemistry Commons, Physics Commons
Comments
Reprinted (adapted) with permission from Journal of Physical Chemistry C 113 (2009): 7277, doi:10.1021/jp8105937. Copyright 2009 American Chemical Society.