Super-resolution vibrational microscopy by stimulated Raman excited fluorescence

Hanqing Xiong; Naixin Qian; Yupeng Miao; Zhilun Zhao; Chen Chen; Wei Min

doi:10.1038/s41377-021-00518-5

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Super-resolution vibrational microscopy by stimulated Raman excited fluorescence

Articles

- Super-resolution vibrational microscopy by stimulated Raman excited fluorescence
- Light: Science & Applications Vol. 10, Issue 5, Pages: 906-915(2021)
- Affiliations：
  
  Department of Chemistry, Columbia University, New York, NY, 10027, USA
- Author bio：
  
  Wei Min (wm2256@columbia.edu)
- Funds：
- DOI：10.1038/s41377-021-00518-5
  CLC：
- Published：31 May 2021，
  
  Published Online：20 April 2021，
  
  Received：29 December 2020，
  
  Revised：24 March 2021，
  
  Accepted：26 March 2021
- Accepted：
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Xiong, H. Q. et al. Super-resolution vibrational microscopy by stimulated Raman excited fluorescence. Light: Science & Applications, 10, 906-915 (2021).
DOI：

Xiong, H. Q. et al. Super-resolution vibrational microscopy by stimulated Raman excited fluorescence. Light: Science & Applications, 10, 906-915 (2021). DOI： 10.1038/s41377-021-00518-5.

摘要

Abstract

Inspired by the revolutionary impact of super-resolution fluorescence microscopy

super-resolution Raman imaging has been long pursued because of its much higher chemical specificity than the fluorescence counterpart. However

vibrational contrasts are intrinsically less sensitive compared with fluorescence

resulting in only mild resolution enhancement beyond the diffraction limit even with strong laser excitation power. As such

it is still a great challenge to achieve biocompatible super-resolution vibrational imaging in the optical far-field. In 2019 Stimulated Raman Excited Fluorescence (SREF) was discovered as an ultrasensitive vibrational spectroscopy that combines the high chemical specificity of Raman scattering and the superb sensitivity of fluorescence detection. Herein we developed a novel super-resolution vibrational imaging method by harnessing SREF as the contrast mechanism. We first identified the undesired role of anti-Stokes fluorescence background in preventing direct adoption of super-resolution fluorescence technique. We then devised a frequency-modulation (FM) strategy to remove the broadband backgrounds and achieved high-contrast SREF imaging. Assisted by newly synthesized SREF dyes

we realized multicolor FM-SREF imaging with nanometer spectral resolution. Finally

by integrating stimulated emission depletion (STED) with background-free FM-SREF

we accomplished high-contrast super-resolution vibrational imaging with STED-FM-SREF whose spatial resolution is only determined by the signal-to-noise ratio. In our proof-of-principle demonstration

more than two times of resolution improvement is achieved in biological systems with moderate laser excitation power

which shall be further refined with optimized instrumentation and imaging probes. With its super resolution

high sensitivity

vibrational contrast

and mild laser excitation power

STED-FM-SREF microscopy is envisioned to aid a wide variety of applications.

关键词

Keywords

references

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