Coherent anti-Stokes Raman scattering with single-molecule sensitivity using a plasmonic Fano resonance

Yu Zhang, Yu-Rong Zhen, Oara Neumann, Jared K. Day, Peter Nordlander and Naomi J. Halas ()
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Yu Zhang: Rice University
Yu-Rong Zhen: Rice University
Oara Neumann: Laboratory for Nanophotonics, Rice University
Jared K. Day: Laboratory for Nanophotonics, Rice University
Peter Nordlander: Rice University
Naomi J. Halas: Rice University

Nature Communications, 2014, vol. 5, issue 1, 1-7

Abstract: Abstract Plasmonic nanostructures are of particular interest as substrates for the spectroscopic detection and identification of individual molecules. Single-molecule sensitivity Raman detection has been achieved by combining resonant molecular excitation with large electromagnetic field enhancements experienced by a molecule associated with an interparticle junction. Detection of molecules with extremely small Raman cross-sections (~10−30 cm2 sr−1), however, has remained elusive. Here we show that coherent anti-Stokes Raman spectroscopy (CARS), a nonlinear spectroscopy of great utility and potential for molecular sensing, can be used to obtain single-molecule detection sensitivity, by exploiting the unique light harvesting properties of plasmonic Fano resonances. The CARS signal is enhanced by ~11 orders of magnitude relative to spontaneous Raman scattering, enabling the detection of single molecules, which is verified using a statistically rigorous bi-analyte method. This approach combines unprecedented single-molecule spectral sensitivity with plasmonic substrates that can be fabricated using top-down lithographic strategies.

Date: 2014
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DOI: 10.1038/ncomms5424

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