Chemical control of charge transfer and recombination at semiconductor photoelectrode surfaces

Research output: Contribution to journalArticle

103 Citations (Scopus)

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.

Original languageEnglish
Pages (from-to)6900-6911
Number of pages12
JournalInorganic Chemistry
Volume44
Issue number20
DOIs
Publication statusPublished - Oct 3 2005

Fingerprint

Charge transfer
charge transfer
Semiconductor materials
solar energy conversion
Energy conversion
Solar energy
Rate constants
inorganic chemistry
Alkylation
chemical energy
alkylation
Contacts (fluid mechanics)
sunlight
Electric properties
electrical properties
Electrodes
Liquids
electrodes
liquids

ASJC Scopus subject areas

  • Inorganic Chemistry

Cite this

Chemical control of charge transfer and recombination at semiconductor photoelectrode surfaces. / Lewis, Nathan S.

In: Inorganic Chemistry, Vol. 44, No. 20, 03.10.2005, p. 6900-6911.

Research output: Contribution to journalArticle

@article{18a4885d7d094f23a831779f831a2d4e,
title = "Chemical control of charge transfer and recombination at semiconductor photoelectrode surfaces",
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.",
author = "Lewis, {Nathan S}",
year = "2005",
month = "10",
day = "3",
doi = "10.1021/ic051118p",
language = "English",
volume = "44",
pages = "6900--6911",
journal = "Inorganic Chemistry",
issn = "0020-1669",
publisher = "American Chemical Society",
number = "20",

}

TY - JOUR

T1 - Chemical control of charge transfer and recombination at semiconductor photoelectrode surfaces

AU - Lewis, Nathan S

PY - 2005/10/3

Y1 - 2005/10/3

N2 - 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.

AB - 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.

UR - http://www.scopus.com/inward/record.url?scp=26944441222&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=26944441222&partnerID=8YFLogxK

U2 - 10.1021/ic051118p

DO - 10.1021/ic051118p

M3 - Article

C2 - 16180845

AN - SCOPUS:26944441222

VL - 44

SP - 6900

EP - 6911

JO - Inorganic Chemistry

JF - Inorganic Chemistry

SN - 0020-1669

IS - 20

ER -