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Plasmon-enhanced stimulated Raman scattering microscopy with single-molecule detection sensitivity

Author

Listed:
  • Cheng Zong

    (Boston University
    Xiamen University)

  • Ranjith Premasiri

    (Boston University
    Boston University)

  • Haonan Lin

    (Boston University)

  • Yimin Huang

    (Boston University)

  • Chi Zhang

    (Boston University)

  • Chen Yang

    (Boston University
    Boston University)

  • Bin Ren

    (Xiamen University)

  • Lawrence D. Ziegler

    (Boston University
    Boston University)

  • Ji-Xin Cheng

    (Boston University
    Boston University
    Boston University)

Abstract

Stimulated Raman scattering (SRS) microscopy allows for high-speed label-free chemical imaging of biomedical systems. The imaging sensitivity of SRS microscopy is limited to ~10 mM for endogenous biomolecules. Electronic pre-resonant SRS allows detection of sub-micromolar chromophores. However, label-free SRS detection of single biomolecules having extremely small Raman cross-sections (~10−30 cm2 sr−1) remains unreachable. Here, we demonstrate plasmon-enhanced stimulated Raman scattering (PESRS) microscopy with single-molecule detection sensitivity. Incorporating pico-Joule laser excitation, background subtraction, and a denoising algorithm, we obtain robust single-pixel SRS spectra exhibiting single-molecule events, verified by using two isotopologues of adenine and further confirmed by digital blinking and bleaching in the temporal domain. To demonstrate the capability of PESRS for biological applications, we utilize PESRS to map adenine released from bacteria due to starvation stress. PESRS microscopy holds the promise for ultrasensitive detection and rapid mapping of molecular events in chemical and biomedical systems.

Suggested Citation

  • Cheng Zong & Ranjith Premasiri & Haonan Lin & Yimin Huang & Chi Zhang & Chen Yang & Bin Ren & Lawrence D. Ziegler & Ji-Xin Cheng, 2019. "Plasmon-enhanced stimulated Raman scattering microscopy with single-molecule detection sensitivity," Nature Communications, Nature, vol. 10(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-13230-1
    DOI: 10.1038/s41467-019-13230-1
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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. Hao He & Maofeng Cao & Yun Gao & Peng Zheng & Sen Yan & Jin-Hui Zhong & Lei Wang & Dayong Jin & Bin Ren, 2024. "Noise learning of instruments for high-contrast, high-resolution and fast hyperspectral microscopy and nanoscopy," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

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