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

doi:10.1021/jp109799e

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

California Institute of Technology

Research output: Contribution to journal › Article

29 Citations (Scopus)

Abstract

The open-circuit potentials of p-Si/((MV²⁺/MV⁺) _(aq)) junctions with Si(111) surfaces functionalized with H-, CH ₃-, CH₂CHCH₂-, or mixed CH₃-/CH ₂CHCH₂- 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 CH₃-, CH ₂CHCH₂-, or mixed CH₃-/CH₂CHCH 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.

Original language	English
Pages (from-to)	8594-8601
Number of pages	8
Journal	Journal of Physical Chemistry C
Volume	115
Issue number	17
DOIs	https://doi.org/10.1021/jp109799e
Publication status	Published - May 5 2011

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
Energy(all)
Physical and Theoretical Chemistry
Surfaces, Coatings and Films

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Johansson, E., Boettcher, S. W., O'Leary, L. E., Poletayev, A. D., Maldonado, S., Brunschwig, B. S., & Lewis, N. 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), 8594-8601. https://doi.org/10.1021/jp109799e

Control of the pH-dependence of the band edges of Si(111) surfaces using mixed methyl/allyl monolayers. / Johansson, Erik; Boettcher, Shannon W.; O'Leary, Leslie E.; Poletayev, Andrey D.; Maldonado, Stephen; Brunschwig, Bruce S.; Lewis, Nathan S.

In: Journal of Physical Chemistry C, Vol. 115, No. 17, 05.05.2011, p. 8594-8601.

Research output: Contribution to journal › Article

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abstract = "The open-circuit potentials of p-Si/((MV2+/MV+) (aq)) junctions with Si(111) surfaces functionalized with H-, CH 3-, CH2CHCH2-, or mixed CH3-/CH 2CHCH2- 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 CH3-, CH 2CHCH2-, or mixed CH3-/CH2CHCH 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.",

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