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Title: Single Molecule Spectroscopy of Electron Transfer

Abstract

The objectives of this research are threefold: (1) to develop methods for the study electron transfer processes at the single molecule level, (2) to develop a series of modifiable and structurally well defined molecular and nanoparticle systems suitable for detailed single molecule/particle and bulk spectroscopic investigation, (3) to relate experiment to theory in order to elucidate the dependence of electron transfer processes on molecular and electronic structure, coupling and reorganization energies. We have begun the systematic development of single molecule spectroscopy (SMS) of electron transfer and summaries of recent studies are shown. There is a tremendous need for experiments designed to probe the discrete electronic and molecular dynamic fluctuations of single molecules near electrodes and at nanoparticle surfaces. Single molecule spectroscopy (SMS) has emerged as a powerful method to measure properties of individual molecules which would normally be obscured in ensemble-averaged measurement. Fluctuations in the fluorescence time trajectories contain detailed molecular level statistical and dynamical information of the system. The full distribution of a molecular property is revealed in the stochastic fluctuations, giving information about the range of possible behaviors that lead to the ensemble average. In the case of electron transfer, this level of understanding is particularly important tomore » the field of molecular and nanoscale electronics: from a device-design standpoint, understanding and controlling this picture of the overall range of possible behaviors will likely prove to be as important as designing ia the ideal behavior of any given molecule.« less

Authors:
; ; ;
Publication Date:
Research Org.:
The Trustees of Columbia University in the City of New York
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
966129
Report Number(s):
DOE-ER15375-03
TRN: US1000772
DOE Contract Number:  
FG02-02ER15373
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; DISTRIBUTION; ELECTRODES; ELECTRON TRANSFER; ELECTRONIC STRUCTURE; FLUCTUATIONS; FLUORESCENCE; PROBES; SPECTROSCOPY; TRAJECTORIES

Citation Formats

Michael Holman, Ling Zang, Ruchuan Liu, and David M. Adams. Single Molecule Spectroscopy of Electron Transfer. United States: N. p., 2009. Web. doi:10.2172/966129.
Michael Holman, Ling Zang, Ruchuan Liu, & David M. Adams. Single Molecule Spectroscopy of Electron Transfer. United States. doi:10.2172/966129.
Michael Holman, Ling Zang, Ruchuan Liu, and David M. Adams. Tue . "Single Molecule Spectroscopy of Electron Transfer". United States. doi:10.2172/966129. https://www.osti.gov/servlets/purl/966129.
@article{osti_966129,
title = {Single Molecule Spectroscopy of Electron Transfer},
author = {Michael Holman and Ling Zang and Ruchuan Liu and David M. Adams},
abstractNote = {The objectives of this research are threefold: (1) to develop methods for the study electron transfer processes at the single molecule level, (2) to develop a series of modifiable and structurally well defined molecular and nanoparticle systems suitable for detailed single molecule/particle and bulk spectroscopic investigation, (3) to relate experiment to theory in order to elucidate the dependence of electron transfer processes on molecular and electronic structure, coupling and reorganization energies. We have begun the systematic development of single molecule spectroscopy (SMS) of electron transfer and summaries of recent studies are shown. There is a tremendous need for experiments designed to probe the discrete electronic and molecular dynamic fluctuations of single molecules near electrodes and at nanoparticle surfaces. Single molecule spectroscopy (SMS) has emerged as a powerful method to measure properties of individual molecules which would normally be obscured in ensemble-averaged measurement. Fluctuations in the fluorescence time trajectories contain detailed molecular level statistical and dynamical information of the system. The full distribution of a molecular property is revealed in the stochastic fluctuations, giving information about the range of possible behaviors that lead to the ensemble average. In the case of electron transfer, this level of understanding is particularly important to the field of molecular and nanoscale electronics: from a device-design standpoint, understanding and controlling this picture of the overall range of possible behaviors will likely prove to be as important as designing ia the ideal behavior of any given molecule.},
doi = {10.2172/966129},
journal = {},
number = ,
volume = ,
place = {United States},
year = {2009},
month = {10}
}