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Harnessing Chemical Raman Enhancement for Understanding Organic Adsorbate Binding on Metal Surfaces

Zayak, Alexey T. and Choo, Hyuck and Hu, Ying S. and Gargas, Daniel J. and Cabrini, Stefano and Bokor, Jeffrey and Schuck, P. James and Neaton, Jeffrey B. (2012) Harnessing Chemical Raman Enhancement for Understanding Organic Adsorbate Binding on Metal Surfaces. Journal of Physical Chemistry Letters, 3 (10). pp. 1357-1362. ISSN 1948-7185. doi:10.1021/jz300374d.

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Surface-enhanced Raman spectroscopy (SERS) is a known approach for detecting trace amounts of molecular species. Whereas SERS measurements have focused on enhancing the signal for sensing trace amounts of a chemical moiety, understanding how the substrate alters molecular Raman spectra can enable optical probing of analyte binding chemistry. Here we examine binding of trans-1,2-two(4- pyridyl) ethylene (BPE) to Au surfaces and understand variations in experimental data that arise from differences in how the molecule binds to the substrate. Monitoring differences in the SERS as a function of incubation time, a period of several hours in our case, reveals that the number of BPE molecules that chemically binds with the Au substrate increases with time. In addition, we introduce a direct method of accessing relative chemical enhancement from experiments that is in quantitative agreement with theory. The ability to probe optically specific details of metal/molecule interfaces opens up possibilities for using SERS in chemical analysis.

Item Type:Article
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URLURL TypeDescription
Zayak, Alexey T.0000-0002-5741-3864
Choo, Hyuck0000-0002-8903-7939
Neaton, Jeffrey B.0000-0001-7585-6135
Additional Information:© 2012 American Chemical Society. Received: March 26, 2012; Accepted: May 3, 2012; Published: May 3, 2012. We thank M. Moskovits, G. Haran, and R. P. Van Duyne for discussions as well as our colleagues at Molecular Foundry and UC Berkeley. This work was supported by the AFOSR/ DARPA Project BAA07-61 “SERS S&T Fundamentals” under contract FA9550-08-1-0257 and the Molecular Foundry through the Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy under Contract No. DEAC02- 05CH11231. Computational resources were provided by DOE (LBNL Lawrencium, NERSC Franklin) and DOD (HPCMP ARL MJM).
Funding AgencyGrant Number
AFOSR/DARPA Project BAA07-61FA9550-08-1-0257
Department of Energy (DOE) Office of Basic Energy Sciences, Office of Science, Molecular FoundryDE-AC02-05CH11231
Subject Keywords:Spectroscopy, Photochemistry, Excited States
Issue or Number:10
Record Number:CaltechAUTHORS:20120614-115559004
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Official Citation:Harnessing Chemical Raman Enhancement for Understanding Organic Adsorbate Binding on Metal Surfaces Alexey T. Zayak, Hyuck Choo, Ying S. Hu, Daniel J. Gargas, Stefano Cabrini, Jeffrey Bokor, P. James Schuck, and Jeffrey B. Neaton The Journal of Physical Chemistry Letters 2012 3 (10), 1357-1362
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:31905
Deposited By: Aucoeur Ngo
Deposited On:14 Jun 2012 20:00
Last Modified:09 Nov 2021 20:02

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