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Stimulated Raman Excited Fluorescence Spectroscopy of Visible Dyes
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2019-06-11 00:00:00 , DOI: 10.1021/acs.jpclett.9b01289 Hanqing Xiong 1 , Naixin Qian 1 , Yupeng Miao 1 , Zhilun Zhao 1 , Wei Min 1
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2019-06-11 00:00:00 , DOI: 10.1021/acs.jpclett.9b01289 Hanqing Xiong 1 , Naixin Qian 1 , Yupeng Miao 1 , Zhilun Zhao 1 , Wei Min 1
Affiliation
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Fluorescence spectroscopy and Raman spectroscopy are two major classes of spectroscopy methods in physical chemistry. Very recently, stimulated Raman excited fluorescence (SREF) has been demonstrated (Xiong, H.; et al. Nature Photonics, 2019, 13, 412−417) as a new hybrid spectroscopy that combines the vibrational specificity of Raman spectroscopy with the superb sensitivity of fluorescence spectroscopy (down to the single-molecule level). However, this proof-of-concept study was limited by both the tunability of the commercial laser source and the availability of the excitable molecules in the near-infrared. As a result, the generality of SREF spectroscopy remains unaddressed, and the understanding of the critical electronic preresonance condition is lacking. In this work, we built a modified excitation source to explore SREF spectroscopy in the visible region. Harnessing a large palette of red dyes, we have systematically studied SREF spectroscopy on a dozen different cases with a fine spectral interval of several nanometers. The results not only establish the generality of SREF spectroscopy for a wide range of molecules but also reveal a tight window of proper electronic preresonance for the stimulated Raman pumping process. Our theoretical modeling and further experiments on newly synthesized dyes also support the obtained insights, which would be valuable in designing and optimizing future SREF experiments for single-molecule vibrational spectroscopy and supermultiplex vibrational imaging.
中文翻译：
可见染料的受激拉曼激发荧光光谱
荧光光谱和拉曼光谱是物理化学中两大类光谱方法。最近，受激拉曼激发荧光（SREF）已被证明（Xiong, H.; et al. Nature Photonics , 2019 , 13 , 412−417）作为一种新型混合光谱，将拉曼光谱的振动特异性与卓越的灵敏度相结合荧光光谱（低至单分子水平）。然而，这项概念验证研究受到商业激光源的可调谐性和近红外可激发分子的可用性的限制。因此，SREF 光谱的通用性仍未得到解决，并且缺乏对关键电子预共振条件的理解。在这项工作中，我们构建了一个改进的激发源来探索可见光区域的 SREF 光谱。利用大量红色染料，我们系统地研究了十几种不同情况下的 SREF 光谱，其光谱间隔为几纳米。结果不仅确立了 SREF 光谱对于各种分子的通用性，而且还揭示了受激拉曼泵浦过程的适当电子预共振的紧密窗口。我们的理论模型和对新合成染料的进一步实验也支持了所获得的见解，这对于设计和优化未来单分子振动光谱和超多重振动成像的 SREF 实验非常有价值。
更新日期：2019-06-11
中文翻译：
可见染料的受激拉曼激发荧光光谱
荧光光谱和拉曼光谱是物理化学中两大类光谱方法。最近，受激拉曼激发荧光（SREF）已被证明（Xiong, H.; et al. Nature Photonics , 2019 , 13 , 412−417）作为一种新型混合光谱，将拉曼光谱的振动特异性与卓越的灵敏度相结合荧光光谱（低至单分子水平）。然而，这项概念验证研究受到商业激光源的可调谐性和近红外可激发分子的可用性的限制。因此，SREF 光谱的通用性仍未得到解决，并且缺乏对关键电子预共振条件的理解。在这项工作中，我们构建了一个改进的激发源来探索可见光区域的 SREF 光谱。利用大量红色染料，我们系统地研究了十几种不同情况下的 SREF 光谱，其光谱间隔为几纳米。结果不仅确立了 SREF 光谱对于各种分子的通用性，而且还揭示了受激拉曼泵浦过程的适当电子预共振的紧密窗口。我们的理论模型和对新合成染料的进一步实验也支持了所获得的见解，这对于设计和优化未来单分子振动光谱和超多重振动成像的 SREF 实验非常有价值。
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