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Mar 08, 2024;13 (1): 70.

Transient stimulated Raman scattering spectroscopy and imaging.

Qiaozhi Yu, Zhengjian Yao, Jiaqi Zhou, Wenhao Yu, Chenjie Zhuang, Yafeng Qi, Hanqing Xiong
Author Information
  1. Qiaozhi Yu: National Biomedical Imaging Center, College of Future Technology, Peking University, Beijing, 100871, China.
  2. Zhengjian Yao: National Biomedical Imaging Center, College of Future Technology, Peking University, Beijing, 100871, China.
  3. Jiaqi Zhou: National Biomedical Imaging Center, College of Future Technology, Peking University, Beijing, 100871, China.
  4. Wenhao Yu: Biomedical Engineering Department, College of Future Technology, Peking University, Beijing, 100871, China.
  5. Chenjie Zhuang: Biomedical Engineering Department, College of Future Technology, Peking University, Beijing, 100871, China.
  6. Yafeng Qi: National Biomedical Imaging Center, College of Future Technology, Peking University, Beijing, 100871, China.
  7. Hanqing Xiong: National Biomedical Imaging Center, College of Future Technology, Peking University, Beijing, 100871, China. xiong.hanqing@pku.edu.cn. ORCID
PMID: 38453917 DOI: 10.1038/s41377-024-01412-6

Abstract

Stimulated Raman scattering (SRS) has been developed as an essential quantitative contrast for chemical imaging in recent years. However, while spectral lines near the natural linewidth limit can be routinely achieved by state-of-the-art spontaneous Raman microscopes, spectral broadening is inevitable for current mainstream SRS imaging methods. This is because those SRS signals are all measured in the frequency domain. There is a compromise between sensitivity and spectral resolution: as the nonlinear process benefits from pulsed excitations, the fundamental time-energy uncertainty limits the spectral resolution. Besides, the spectral range and acquisition speed are mutually restricted. Here we report transient stimulated Raman scattering (T-SRS), an alternative time-domain strategy that bypasses all these fundamental conjugations. T-SRS is achieved by quantum coherence manipulation: we encode the vibrational oscillations in the stimulated Raman loss (SRL) signal by femtosecond pulse-pair sequence excited vibrational wave packet interference. The Raman spectrum was then achieved by Fourier transform of the time-domain SRL signal. Since all Raman modes are impulsively and simultaneously excited, T-SRS features the natural-linewidth-limit spectral line shapes, laser-bandwidth-determined spectral range, and improved sensitivity. With ~150-fs laser pulses, we boost the sensitivity of typical Raman modes to the sub-mM level. With all-plane-mirror high-speed time-delay scanning, we further demonstrated hyperspectral SRS imaging of live-cell metabolism and high-density multiplexed imaging with the natural-linewidth-limit spectral resolution. T-SRS shall find valuable applications for advanced Raman imaging.

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Grants

  1. 62275004/National Natural Science Foundation of China (National Science Foundation of China)
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