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Published May 17, 2012 | Supplemental Material
Journal Article Open

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

Abstract

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.

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).

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