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Electronic Resonant Stimulated Raman Scattering Micro-Spectroscopy

Shi, Lixue and Xiong, Hanqing and Shen, Yihui and Long, Rong and Wei, Lu and Min, Wei (2018) Electronic Resonant Stimulated Raman Scattering Micro-Spectroscopy. Journal of Physical Chemistry B, 122 (39). pp. 9218-9224. ISSN 1520-6106. PMCID PMC6425473. doi:10.1021/acs.jpcb.8b07037.

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[img] PDF (Synthesis of SiR845 and results of er-SRS power dependence study, including Figures S1–S6 of electronic background from competing pump–probe processes, simulations of er-SRS band shapes, power dependence study for SiR845, power dependence study for SiR845) - Supplemental Material
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Recently we have reported electronic pre-resonance stimulated Raman scattering (epr-SRS) microscopy as a powerful technique for super-multiplex imaging (Wei, L.; Nature 2017, 544, 465−470). However, under rigorous electronic resonance, background signal, which mainly originates from pump–probe process, overwhelms the desired vibrational signature of the chromophores. Here we demonstrate electronic resonant stimulated Raman scattering (er-SRS) microspectroscopy and imaging through suppression of electronic background and subsequent retrieval of vibrational peaks. We observed a change of the vibrational band shapes from normal Lorentzian, through dispersive shapes, to inverted Lorentzian as the electronic resonance was approached, in agreement with theoretical prediction. In addition, resonant Raman cross sections have been determined after power-dependence study as well as Raman excitation profile calculation. As large as 10⁻²³ cm² of resonance Raman cross section is estimated in er-SRS, which is about 100 times higher than previously reported in epr-SRS. These results of er-SRS microspectroscopy pave the way for the single-molecule Raman detection and ultrasensitive biological imaging.

Item Type:Article
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URLURL TypeDescription CentralArticle
Wei, Lu0000-0001-9170-2283
Min, Wei0000-0003-2570-3557
Additional Information:© 2018 American Chemical Society. Received: July 22, 2018. Revised: September 8, 2018. Published: September 12, 2018. Published as part of The Journal of Physical Chemistry virtual special issue “Young Scientists”. W.M. acknowledges support from the US Army Research Office (W911NF-12-1-0594) and R01 (EB020892) and the Camille and Henry Dreyfus Foundation. The authors declare no competing financial interest.
Funding AgencyGrant Number
Army Research Office (ARO)W911NF-12-1-0594
NIHR01 EB020892
Camille and Henry Dreyfus FoundationUNSPECIFIED
Issue or Number:39
PubMed Central ID:PMC6425473
Record Number:CaltechAUTHORS:20181119-102039172
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Official Citation:Electronic Resonant Stimulated Raman Scattering Micro-Spectroscopy Lixue Shi, Hanqing Xiong, Yihui Shen, Rong Long, Lu Wei, and Wei Min The Journal of Physical Chemistry B 2018 122 (39), 9218-9224 DOI: 10.1021/acs.jpcb.8b07037
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:91008
Deposited By: George Porter
Deposited On:19 Nov 2018 21:55
Last Modified:18 Nov 2021 17:37

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