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High-Resolution Soft X-ray Photoelectron Spectroscopic Studies and Scanning Auger Microscopy Studies of the Air Oxidation of Alkylated Silicon(111) Surfaces

Webb, Lauren J. and Michalak, David J. and Biteen, Julie S. and Brunschwig, Bruce S. and Chan, Ally S. Y. and Knapp, David W. and Meyer, Harry M.,III and Nemanick, Eric J. and Traub, Matthew C. and Lewis, Nathan S. (2006) High-Resolution Soft X-ray Photoelectron Spectroscopic Studies and Scanning Auger Microscopy Studies of the Air Oxidation of Alkylated Silicon(111) Surfaces. Journal of Physical Chemistry B, 110 (46). pp. 23450-23459. ISSN 1520-6106. https://resolver.caltech.edu/CaltechAUTHORS:20170607-132636106

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Abstract

High-resolution soft X-ray photoelectron spectroscopy was used to investigate the oxidation of alkylated silicon(111) surfaces under ambient conditions. Silicon(111) surfaces were functionalized through a two-step route involving radical chlorination of the H-terminated surface followed by alkylation with alkylmagnesium halide reagents. After 24 h in air, surface species representing Si^+, Si^(2+), Si^(3+), and Si^(4+) were detected on the Cl-terminated surface, with the highest oxidation state (Si^(4+)) oxide signal appearing at +3.79 eV higher in energy than the bulk Si 2p_(3/2) peak. The growth of silicon oxide was accompanied by a reduction in the surface-bound Cl signal. After 48 h of exposure to air, the Cl-terminated Si(111) surface exhibited 3.63 equivalent monolyers (ML) of silicon oxides. In contrast, after exposure to air for 48 h, CH_3-, C_2H_5-, or C_6H_5CH_2-terminated Si surfaces displayed <0.4 ML of surface oxide, and in most cases only displayed ≈0.20 ML of oxide. This oxide was principally composed of Si+ and Si^(3+) species with peaks centered at +0.8 and +3.2 eV above the bulk Si 2p_(3/2) peak, respectively. The silicon 2p SXPS peaks that have previously been assigned to surface Si−C bonds did not change significantly, either in binding energy or in relative intensity, during such air exposure. Use of a high miscut-angle surface (7° vs ≤0.5° off of the (111) surface orientation) yielded no increase in the rate of oxidation nor change in binding energy of the resultant oxide that formed on the alkylated Si surfaces. Scanning Auger microscopy indicated that the alkylated surfaces formed oxide in isolated, inhomogeneous patches on the surface.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/jp063366sDOIArticle
http://pubs.acs.org/doi/abs/10.1021/jp063366sPublisherArticle
ORCID:
AuthorORCID
Brunschwig, Bruce S.0000-0002-6135-6727
Lewis, Nathan S.0000-0001-5245-0538
Additional Information:© 2006 American Chemical Society. Received 31 May 2006. Published online 31 October 2006. Published in print 1 November 2006. We gratefully acknowledge the National Science Foundation for support of this work (grants CHE-0213589) and for providing a graduate research fellowship to L.J.W. A.C. acknowledges support from the Army Research Office. This research was carried out in part at the National Synchrotron Light Source, Brookhaven National Laboratory, which is supported by the U. S. Department of Energy, Division of Materials Sciences and Division of Chemical Sciences, under Contract No. DE-AC02-98CH10886. We thank Michael Sullivan for use of the N2(g)-purged glovebox at the NSLS. The scanning Auger microscopy was sponsored by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of FreedomCAR and Vehicle Technologies, as part of the High Temperature Materials Laboratory User Program, Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U. S. Department of Energy under contract number DE-AC05-00OR22725. We also thank Y. Chabal for sharing a preprint of his manuscript on the oxidation of silicon in air.
Funders:
Funding AgencyGrant Number
NSFCHE-0213589
Army Research Office (ARO)UNSPECIFIED
Department of Energy (DOE)DE-AC02-98CH10886
Department of Energy (DOE) DE-AC05-00OR22725
Issue or Number:46
Record Number:CaltechAUTHORS:20170607-132636106
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20170607-132636106
Official Citation:High-Resolution Soft X-ray Photoelectron Spectroscopic Studies and Scanning Auger Microscopy Studies of the Air Oxidation of Alkylated Silicon(111) Surfaces Lauren J. Webb, David J. Michalak, Julie S. Biteen, Bruce S. Brunschwig, Ally S. Y. Chan, David W. Knapp, Harry M. Meyer, III, Eric J. Nemanick, Matthew C. Traub, and Nathan S. Lewis The Journal of Physical Chemistry B 2006 110 (46), 23450-23459 DOI: 10.1021/jp063366s
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:78005
Collection:CaltechAUTHORS
Deposited By: Ruth Sustaita
Deposited On:07 Jun 2017 22:38
Last Modified:03 Oct 2019 18:04

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