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Chemical Control of Charge Transfer and Recombination at Semiconductor Photoelectrode Surfaces

Lewis, Nathan S. (2005) Chemical Control of Charge Transfer and Recombination at Semiconductor Photoelectrode Surfaces. Inorganic Chemistry, 44 (20). pp. 6900-6911. ISSN 0020-1669. doi:10.1021/ic051118p. https://resolver.caltech.edu/CaltechAUTHORS:20170315-141210704

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Abstract

Semiconductor/liquid contacts provide very efficient systems for converting sunlight into electrical and/or chemical energy. Until recently, relatively little was understood about the factors that control the rates of interfacial charge transfer in such systems. This Forum Article summarizes recent results that have elucidated the key factors that control such charge-transfer rates, including verification of the Marcus inverted region, identification of the maximum charge-transfer rate constant for outer-sphere, nonadsorbing redox couples at optimal exoergicity, the role of nuclear reorganization on the value of the interfacial charge-transfer rate constant at semiconductor electrodes, and the effects of pH-induced changes in the driving force on the rates of such systems. In addition, we discuss methods for using main group inorganic chemistry to control the electrical properties of surfaces of important semiconductors for solar energy conversion, with specific emphasis on alkylation of the (111)-oriented surface of Si. Control of the rates at which carriers cross such interfaces, along with control of the rates at which carriers recombine at such interfaces, forms the basis for exerting chemical control over the key solar energy conversion properties of semiconductor photoelectrode-based devices.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/ic051118pDOIArticle
http://pubs.acs.org/doi/abs/10.1021/ic051118pPublisherArticle
ORCID:
AuthorORCID
Lewis, Nathan S.0000-0001-5245-0538
Additional Information:© 2005 American Chemical Society. Received July 6, 2005; Publication Date (Web): September 26, 2005. We acknowledge NSF Grant CHE-0213589 and the Office of Basic Energy Sciences, Department of Energy, for the sustained support that has made the research discussed herein possible. In addition, the author is extremely indebted to Tom W. Hamann and David J. Michalak for their invaluable help during the preparation of this manuscript.
Funders:
Funding AgencyGrant Number
NSFCHE-0213589
Department of Energy (DOE)UNSPECIFIED
Issue or Number:20
DOI:10.1021/ic051118p
Record Number:CaltechAUTHORS:20170315-141210704
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20170315-141210704
Official Citation:Chemical Control of Charge Transfer and Recombination at Semiconductor Photoelectrode Surfaces Nathan S. Lewis Inorganic Chemistry 2005 44 (20), 6900-6911 DOI: 10.1021/ic051118p
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:75153
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:16 Mar 2017 17:06
Last Modified:15 Nov 2021 16:31

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