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

Author

Listed:
  • Yu Zhang

    (Rice University
    Laboratory for Nanophotonics, Rice University)

  • Yu-Rong Zhen

    (Rice University
    Laboratory for Nanophotonics, Rice University)

  • Oara Neumann

    (Laboratory for Nanophotonics, Rice University
    Rice University)

  • Jared K. Day

    (Laboratory for Nanophotonics, Rice University
    Rice University)

  • Peter Nordlander

    (Rice University
    Laboratory for Nanophotonics, Rice University
    Rice University)

  • Naomi J. Halas

    (Rice University
    Laboratory for Nanophotonics, Rice University
    Rice University)

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.

Suggested Citation

  • Yu Zhang & Yu-Rong Zhen & Oara Neumann & Jared K. Day & Peter Nordlander & Naomi J. Halas, 2014. "Coherent anti-Stokes Raman scattering with single-molecule sensitivity using a plasmonic Fano resonance," Nature Communications, Nature, vol. 5(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:5:y:2014:i:1:d:10.1038_ncomms5424
    DOI: 10.1038/ncomms5424
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    Cited by:

    1. Yang Luo & Alberto Martin-Jimenez & Michele Pisarra & Fernando Martin & Manish Garg & Klaus Kern, 2023. "Imaging and controlling coherent phonon wave packets in single graphene nanoribbons," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    2. Mingu Kang & Hyunwoo Kim & Elham Oleiki & Yeonjeong Koo & Hyeongwoo Lee & Huitae Joo & Jinseong Choi & Taeyong Eom & Geunsik Lee & Yung Doug Suh & Kyoung-Duck Park, 2022. "Conformational heterogeneity of molecules physisorbed on a gold surface at room temperature," Nature Communications, Nature, vol. 13(1), pages 1-9, December.

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