Fluorescence-Encoded Infrared Vibrational Spectroscopy with Single-Molecule Sensitivity
Fluorescence-Encoded Infrared Vibrational Spectroscopy with Single-Molecule Sensitivity
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DOI：
10.1021/jacs.1c00542
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发表时间：
2021-02-17
影响因子：
15
通讯作者：
Tokmakoff, Andrei
中科院分区：
文献类型：
--
作者：
Whaley-Mayda, Lukas;Guha, Abhirup;Tokmakoff, Andrei
单分子方法已经彻底改变了分子科学，但具有化学问题所需的结构灵敏度的技术-例如振动光谱-仍然难以应用于解决方案。在这里，我们描述了如何耦合红外振动吸收的荧光电子跃迁（荧光编码红外（FEIR）光谱）可以实现单分子的灵敏度与传统的远场光学解决方案。使用荧光团香豆素6，我们说明的原则，FEIR光谱测量振动光谱和弛豫，并介绍FEIR相关光谱，荧光相关光谱的振动模拟，以证明单分子的灵敏度。随着进一步的改进，FEIR光谱可能成为溶液或凝聚相中单分子振动研究的有力工具。
Single-molecule methods have revolutionized molecular science, but techniques possessing the structural sensitivity required for chemical problems-e.g. vibrational spectroscopy-remain difficult to apply in solution. Here, we describe how coupling infrared-vibrational absorption to a fluorescent electronic transition (fluorescence-encoded infrared (FEIR) spectroscopy) can achieve single-molecule sensitivity in solution with conventional far-field optics. Using the fluorophore Coumarin 6, we illustrate the principles by which FEIR spectroscopy measures vibrational spectra and relaxation and introduce FEIR correlation spectroscopy, a vibrational analogue of fluorescence correlation spectroscopy, to demonstrate single-molecule sensitivity. With further improvements, FEIR spectroscopy could become a powerful tool for single-molecule vibrational investigations in the solution or condensed phase.