4.8 Article

Monitoring the Electrochemistry of Single Molecules by Surface-Enhanced Raman Spectroscopy

Journal

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 132, Issue 51, Pages 18034-18037

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/ja108989b

Keywords

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Funding

  1. UNLP
  2. ANPCyT (Argentina) [PICT06-621, PAE 22711, PICT06-01061, PICT-CNPQ 08-019]
  3. MacDiarmid Institute (New Zealand)
  4. Royal Society of New Zealand under Marsden

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Coherent control of chemical species in complex systems is always subject to intrinsic inhomogeneities from the environment. For example, slight chemical modifications can decisively affect transport properties of molecules on surfaces. Hence, single-molecule (SM) studies are the best solution to avoid these problems and to study diverse phenomena in biology, physics, and chemistry. Along these lines, monitoring SM redox processes has always been a holy grail in electrochemistry. To date, claims of SM electrochemistry by spectroscopy have come only from fluorescence quenching of polymers and redox-fluorescent molecules. In unconnected developments, the potential of the bianalyte surface-enhanced Raman scattering (SERS) method as a technique with SM sensitivity has been demonstrated. Raman spectroscopy has the potential to explore SM detection of any molecule, independent of its chemical nature. We provide definitive proof of SM events following redox cycles using SERS. The superior sensitivity and spectral richness of SERS makes it general enough to study, in principle, SM electron transfer of any (label-free) molecule.

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