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Control of the pH-Dependence of the Band Edges of Si(111) Surfaces Using Mixed Methyl/Allyl Monolayers

Johansson, Erik and Boettcher, Shannon W. and O'Leary, Leslie E. and Poletayev, Andrey D. and Maldonado, Stephen and Brunschwig, Bruce S. and Lewis, Nathan S. (2011) Control of the pH-Dependence of the Band Edges of Si(111) Surfaces Using Mixed Methyl/Allyl Monolayers. Journal of Physical Chemistry C, 115 (17). pp. 8594-8601. ISSN 1932-7447.

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The open-circuit potentials of p-Si/((MV^(2+)/MV^(+))(aq)) junctions with Si(111) surfaces functionalized with H−, CH_(3)−, CH_(2)CHCH_(2)−, or mixed CH_(3)−/CH_(2)CHCH_(2)− monolayers have been investigated as the solution pH was changed from 2.5 to 11. The pH sensitivity of the open-circuit potentials, and therefore the band-edge positions, was anticorrelated with the total fraction of Si atop sites that were terminated by Si−C bonds. This behavior is consistent with the hypothesis that the non Si−C terminated atop sites were initially H-terminated and were unstable to oxide growth under aqueous conditions with the oxidation-product inducing a pH-dependent dipole. Metal-semiconductor junctions between Hg and CH_(3)-, CH_(2)CHCH_(2)-, or mixed CH_(3)-/CH_(2)CHCH_(2)-terminated n-Si(111) surfaces formed rectifying Hg/Si Schottky junctions and exhibited mutually similar barrier-heights (~0.9 V), suggesting similar magnitudes and direction of the surface dipoles on all of these functionalized surfaces.

Item Type:Article
Related URLs:
URLURL TypeDescription
Boettcher, Shannon W.0000-0001-8971-9123
Maldonado, Stephen0000-0002-2917-4851
Brunschwig, Bruce S.0000-0002-6135-6727
Lewis, Nathan S.0000-0001-5245-0538
Additional Information:© 2011 American Chemical Society. Received: October 12, 2010; revised: February 22, 2011; published: April 8, 2011. This work was supported by the National Science Foundation (CHE-0911682) and the Molecular Materials Research Center of the Beckman Institute at the California Institute of Technology. The Kavli Nanoscience Institute (S.W.B) and the Betty and Gordon Moore Foundation (S. M.) are gratefully acknowledged for postdoctoral fellowship support.
Group:Kavli Nanoscience Institute
Funding AgencyGrant Number
Caltech Beckman InstituteUNSPECIFIED
Kavli Nanoscience InstituteUNSPECIFIED
Gordon and Betty Moore FoundationUNSPECIFIED
Issue or Number:17
Record Number:CaltechAUTHORS:20110510-104428314
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Official Citation:Control of the pH-Dependence of the Band Edges of Si(111) Surfaces Using Mixed Methyl/Allyl Monolayers Erik Johansson, Shannon W. Boettcher, Leslie E. O’Leary, Andrey D. Poletayev, Stephen Maldonado, Bruce S. Brunschwig, Nathan S. Lewis The Journal of Physical Chemistry C 2011 115 (17), 8594-8601
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:23608
Deposited By: Jason Perez
Deposited On:10 May 2011 22:49
Last Modified:09 Mar 2020 13:19

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