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Control of the Stability, Electron-Transfer Kinetics, and pH-Dependent Energetics of Si/H_2O Interfaces through Methyl Termination of Si(111) Surfaces

Hamann, Thomas W. and Lewis, Nathan S. (2006) Control of the Stability, Electron-Transfer Kinetics, and pH-Dependent Energetics of Si/H_2O Interfaces through Methyl Termination of Si(111) Surfaces. Journal of Physical Chemistry B, 110 (45). pp. 22291-22294. ISSN 1520-6106. https://resolver.caltech.edu/CaltechAUTHORS:20170609-083755926

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Abstract

Methyl-terminated, n-type, (111)-oriented Si surfaces were prepared via a two-step chlorination-alkylation method. This surface modification passivated the Si surface toward electrochemical oxidation and thereby allowed measurements of interfacial electron-transfer processes in contact with aqueous solutions. The resulting semiconductor/liquid junctions exhibited interfacial kinetics behavior in accord with the ideal model of a semiconductor/liquid junction. In contrast to the behavior of H-terminated Si(111) surfaces, current density vs. potential measurements of CH_3-terminated Si(111) surfaces in contact with an electron acceptor having a pH-independent redox potential (methyl viologen^(2+/+)) were used to verify that the band edges of the modified Si electrode were fixed with respect to changes in solution pH. The results provide strong evidence that the energetics of chemically modified Si interfaces can be fixed with respect to pH and show that the band-edge energies of Si can be tuned independently of pH-derived variations in the electrochemical potential of the solution redox species.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/jp064401yDOIArticle
http://pubs.acs.org/doi/abs/10.1021/jp064401yPublisherArticle
ORCID:
AuthorORCID
Lewis, Nathan S.0000-0001-5245-0538
Additional Information:© 2006 American Chemical Society. Received 12 July 2006. Published online 24 October 2006. Published in print 1 November 2006. We acknowledge the NSF, grant CHE-0604894, for support of this work. XPS data were collected at the Molecular Materials Research Center of the Beckman Institute of the California Institute of Technology.
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Funding AgencyGrant Number
NSFCHE-0604894
Issue or Number:45
Record Number:CaltechAUTHORS:20170609-083755926
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20170609-083755926
Official Citation:Control of the Stability, Electron-Transfer Kinetics, and pH-Dependent Energetics of Si/H2O Interfaces through Methyl Termination of Si(111) Surfaces Thomas W. Hamann and Nathan S. Lewis The Journal of Physical Chemistry B 2006 110 (45), 22291-22294 DOI: 10.1021/jp064401y
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:78047
Collection:CaltechAUTHORS
Deposited By: Ruth Sustaita
Deposited On:09 Jun 2017 16:21
Last Modified:03 Oct 2019 18:04

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