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Efficient optical plasmonic tweezer-controlled single-molecule SERS characterization of pH-dependent amylin species in aqueous milieus

Author

Listed:
  • Wenhao Fu

    (The Hong Kong University of Science and Technology, Clear Water Bay)

  • Huanyu Chi

    (The Hong Kong University of Science and Technology, Clear Water Bay)

  • Xin Dai

    (The Hong Kong University of Science and Technology, Clear Water Bay
    Health@InnoHK, Hong Kong Science Park)

  • Hongni Zhu

    (The Hong Kong University of Science and Technology, Clear Water Bay)

  • Vince St. Dollente Mesias

    (The Hong Kong University of Science and Technology, Clear Water Bay)

  • Wei Liu

    (The University of Hong Kong, Pokfulam Road)

  • Jinqing Huang

    (The Hong Kong University of Science and Technology, Clear Water Bay)

Abstract

It is challenging to characterize single or a few biomolecules in physiological milieus without excluding the influences of surrounding environment. Here we utilize optical plasmonic trapping to construct a dynamic nanocavity, which reduces the diffraction-limited detection volume and provides reproducible electromagnetic field enhancements to achieve high-throughput single-molecule surface-enhanced Raman spectroscopy (SERS) characterizations in aqueous environments. Specifically, we study human Islet Amyloid Polypeptide (amylin, hIAPP) under different physiological pH conditions by combining spectroscopic experiments and molecular dynamics (MD) simulations. Based on a statistically significant amount of time-dependent SERS spectra, two types of low-populated transient species of hIAPP containing either turn or β-sheet structure among its predominant helix-coil monomers are characterized during the early-stage incubation at neutral condition, which play a crucial role in driving irreversible amyloid fibril developments even after a subsequent adjustment of pH to continue the prolonged incubation at acidic condition. Our results might provide profound mechanistic insight into the pH-regulated amyloidogenesis and introduce an alternative approach for investigating complex biological processes at the single-molecule level.

Suggested Citation

  • Wenhao Fu & Huanyu Chi & Xin Dai & Hongni Zhu & Vince St. Dollente Mesias & Wei Liu & Jinqing Huang, 2023. "Efficient optical plasmonic tweezer-controlled single-molecule SERS characterization of pH-dependent amylin species in aqueous milieus," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-42812-3
    DOI: 10.1038/s41467-023-42812-3
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    References listed on IDEAS

    as
    1. Jian-An Huang & Mansoureh Z. Mousavi & Yingqi Zhao & Aliaksandr Hubarevich & Fatima Omeis & Giorgia Giovannini & Moritz Schütte & Denis Garoli & Francesco De Angelis, 2019. "SERS discrimination of single DNA bases in single oligonucleotides by electro-plasmonic trapping," Nature Communications, Nature, vol. 10(1), pages 1-10, December.
    2. Xin Dai & Wenhao Fu & Huanyu Chi & Vince St. Dollente Mesias & Hongni Zhu & Cheuk Wai Leung & Wei Liu & Jinqing Huang, 2021. "Optical tweezers-controlled hotspot for sensitive and reproducible surface-enhanced Raman spectroscopy characterization of native protein structures," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    3. 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.
    4. Changjun Min & Zhe Shen & Junfeng Shen & Yuquan Zhang & Hui Fang & Guanghui Yuan & Luping Du & Siwei Zhu & Ting Lei & Xiaocong Yuan, 2013. "Focused plasmonic trapping of metallic particles," Nature Communications, Nature, vol. 4(1), pages 1-7, December.
    5. Joonhee Lee & Kevin T. Crampton & Nicholas Tallarida & V. Ara Apkarian, 2019. "Visualizing vibrational normal modes of a single molecule with atomically confined light," Nature, Nature, vol. 568(7750), pages 78-82, April.
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