Double Resonance Excitation of Fluorescence by Stimulated Raman Scattering

Lee, S. H.; Nguyen, Dinh C.; Wright, John

doi:10.1366/0003702834634974

Cited by 10 publications

(17 citation statements)

References 5 publications

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“…We found that, even with a quantum amplification up to 10 8 achieved under modern SRS microscopy 10 , the effective SRS excitation cross sections are still less than 10 −20 cm 2 for typical chromophores including coumarin, resulting in much less efficient vibrational pumping rate compared to the rapid vibrational relaxation (subpicosecond) of molecules in condensed phases 7 . As a result, this SREF pathway is easily overwhelmed by other competing processes such as two-photon fluorescence background, which was observed in our attempt on coumarin and previous unsuccessful trial on perylene dye 11 .…”

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confidence: 83%

“…That is why 2-ps pulses were chosen to be short enough to compete favorably with vibrational relaxation yet long enough to maintain the fine spectral selectivity. In contrast, an inefficient pulse width of 5-ns was used in the previous unsuccessful attempt 11 . Numerically, we modeled the SREF process with a three-level rate equation, and obtained 20% upconversion efficiency, close to the result from steady-state approximation (see Methods and Supplementary Fig.…”

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confidence: 99%

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Stimulated Raman excited fluorescence spectroscopy and imaging

et al. 2019

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Powerful optical tools have revolutionized science and technology. The prevalent fluorescence detection offers superb sensitivity down to single molecules but lacks sufficient chemical information [1][2][3] . In contrast, Raman-based vibrational spectroscopy provides exquisite chemical specificity about molecular structure, dynamics and coupling, but is notoriously insensitive [3][4][5] . Here we report a hybrid technique of Stimulated Raman Excited Fluorescence (SREF) that integrates superb detection sensitivity and fine chemical specificity. Through stimulated Raman pumping to an intermediate vibrational eigenstate followed by an upconversion to an electronic fluorescent state, SREF encodes vibrational resonance into the excitation spectrum of fluorescence emission. By harnessing narrow vibrational linewidth, we demonstrated multiplexed SREF imaging in cells, breaking the "color barrier" of fluorescence. By leveraging superb sensitivity of SREF, we achieved all-far-field single-molecule Raman spectroscopy and imaging without plasmonic enhancement, a long-sought-after goal in photonics. Thus, through merging Raman and fluorescence spectroscopy, SERF would be a valuable tool for chemistry and biology.

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confidence: 83%

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Stimulated Raman excited fluorescence spectroscopy and imaging

et al. 2019

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“…In light of the revolutionary success of single-molecule fluorescence spectroscopy in the subsequent decades 25–27 , Winterhalder et al were also optimistic and proposed in 2011 that this method might offer the single-molecule sensitivity of vibrational spectroscopy at optical far-field 28 . However, the first experimental attempt by Wright’s group in 1983 was hindered by overwhelming two-photon fluorescence background from perylene dye 29 . To the best of our knowledge, no further experimental studies have been published about this type of spectroscopy since 1983.…”

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confidence: 99%

“…6) also lends support to this insight. On one hand, such a relatively narrow range might appear stringent and thus partly explain why experimental progress on this line has been slow during the past three decades 29 . On the other hand, the successful SREF detection of all 8 cases falling within the proper electronic pre-resonance window strongly supports the generality and robustness of SREF spectroscopy (Table 1).…”

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confidence: 99%

Stimulated Raman Excited Fluorescence Spectroscopy of Visible Dyes

Xiong

Qian

Miao

et al. 2019

J. Phys. Chem. Lett.

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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) as a new hybrid spectroscopy that combines the vibrational specificity of Raman spectroscopy with the superb sensitivity of fluorescence spectroscopy (down to 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 pre-resonance condition is lacking. Herein 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 of 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 pre-resonance 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 super-multiplex vibrational imaging.

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“…10 6 by the resonance Raman technique. However, in the case of fluorescent molecules or in the presence of fluorescent impurities, the strong fluorescence signal can overwhelm the resonance Raman signal[72,73,74,75,76,77,78]. Fluorescence appears on the red side of the Raman excitation wavelength, and fluorescence rejection requires a technique that records spectra on the blue side of the Raman excitation wavelength.…”

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Theoretical studies and model calculations of femtosecond stimulated Raman spectroscopy

Qiu¹

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I would like to thank my supervisor Prof. Lee Soo-Ying for his guidance and assistance throughout this entire project. Prof. Lee taught me how to find a scientific problem and to solve the problem. During the research, he provided invaluable advice on constructing models, data analysis, and paper writing. He is knowledgable and his ability of focusing on big picture kept me from overthinking technicalities. I am thankful for all the skills he has taught me. I would like to express my genuine gratitude to Dr. Sun Zhigang and Dr. Lu Yunpeng for their assistance and support. Dr. Sun Zhigang was an excellent tutor, without his help and patience it would be very hard for me to get close to these projects. Dr. Lu Yunpeng helped me a lot on debugging the codes and he gave me some wonderful suggestions. Thanks to all the talented and pleasant colleague Dr. Niu Kai, Zhao Bin, Li Xiuting, Song Hongwei and others in the Physics and Applied Physics department. I gratefully acknowledge the helpful discussions with them. Without them, life as a PhD student for these years would be very dull and monotonous. Finally, I would like to express my deepest gratitude to my family for their emotional support and encouragement. My parents, my husband and my brother, they are a great source of inspiration throughout the duration of my studies.

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Double Resonance Excitation of Fluorescence by Stimulated Raman Scattering

Cited by 10 publications

References 5 publications

Stimulated Raman excited fluorescence spectroscopy and imaging

Stimulated Raman excited fluorescence spectroscopy and imaging

Stimulated Raman Excited Fluorescence Spectroscopy of Visible Dyes

Theoretical studies and model calculations of femtosecond stimulated Raman spectroscopy

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