Binding and Diffusion of Al Adatoms and Dimers on the Si(100)-2 × 1 Reconstructed Surface: A Hybrid QM/MM Embedded Cluster Study Zorn, Deborah Albao, Marvin Evans, James Gordon, Mark
dc.contributor.department Ames National Laboratory
dc.contributor.department Physics and Astronomy
dc.contributor.department Mathematics
dc.contributor.department Chemistry 2018-02-17T10:38:21.000 2020-06-30T06:17:42Z 2020-06-30T06:17:42Z Thu Jan 01 00:00:00 UTC 2009 2009-04-01
dc.description.abstract <p>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.</p>
dc.description.comments <p>Reprinted (adapted) with permission from <em>Journal of Physical Chemistry C</em> 113 (2009): 7277, doi:<a href="" target="_blank">10.1021/jp8105937</a>. Copyright 2009 American Chemical Society. </p>
dc.format.mimetype application/pdf
dc.identifier archive/
dc.identifier.articleid 1197
dc.identifier.contextkey 8006803
dc.identifier.s3bucket isulib-bepress-aws-west
dc.identifier.submissionpath physastro_pubs/198
dc.language.iso en
dc.source.bitstream archive/|||Fri Jan 14 22:00:00 UTC 2022
dc.source.bitstream archive/|||Fri Jan 14 22:00:01 UTC 2022
dc.source.uri 10.1021/jp8105937
dc.subject.disciplines Astrophysics and Astronomy
dc.subject.disciplines Mathematics
dc.subject.disciplines Physical Chemistry
dc.subject.disciplines Physics
dc.subject.keywords Ab-initio electronic structure calculations
dc.subject.keywords basis sets
dc.subject.keywords cluster calculations
dc.subject.keywords density functional theory calculations
dc.subject.keywords DFT study
dc.subject.keywords diradical
dc.subject.keywords effective core potential
dc.subject.keywords embedded cluster calculations
dc.subject.keywords extended surfaces
dc.subject.keywords Hybrid QM/MM
dc.subject.keywords Island growth
dc.subject.keywords Multiconfiguration self-consistent fields
dc.subject.keywords Multireference second order perturbation theories
dc.subject.keywords orbital molecular mechanics
dc.subject.keywords adatoms
dc.title Binding and Diffusion of Al Adatoms and Dimers on the Si(100)-2 × 1 Reconstructed Surface: A Hybrid QM/MM Embedded Cluster Study
dc.type article
dc.type.genre article
dspace.entity.type Publication
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