Double modulation SRS and SREF microscopy : signal contributions under pre-resonance conditions

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Physical Chemistry Chemical Physics (PCCP). Royal Society of Chemistry (RSC). 2020, 22(37), pp. 21421-21427. ISSN 1463-9076. eISSN 1463-9084. Available under: doi: 10.1039/d0cp03221b
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Abstract Pre-electronic resonance enhancement can increase the sensitivity of non-linear Raman microscopy to the single molecule detection limit. A major problem, however, is the generation of background signal due to unwanted linear and non-linear photophysical processes. In this work, we report the setup of a novel detection scheme for stimulated Raman scattering microspectroscopy based on the simultaneous modulation of pump and Stokes beam. Apart from allowing the parallel detection of stimulated Raman loss and gain (SRL and SRG), the setup gives access to the quantitative analysis of different sources of background signal. We report spectrally and temporally resolved measurements on three exemplary rhodamine dyes and derive the contributions of two-photon absorption and stimulated emission to their SRL, SRG, and stimulated Raman excited fluorescence signals. These results give guidelines for the further improvement of the sensitivity of non-linear Raman micospectroscopy under electronic pre-resonance conditions.

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ISO 690FIMPEL, Peter, Ashwin J. X. CHOORAKUTTIL, Andrea PRUCCOLI, Lukas EBNER, Shunji TANAKA, Yasuyuki OZEKI, Martin WINTERHALDER, Andreas ZUMBUSCH, 2020. Double modulation SRS and SREF microscopy : signal contributions under pre-resonance conditions. In: Physical Chemistry Chemical Physics (PCCP). Royal Society of Chemistry (RSC). 2020, 22(37), pp. 21421-21427. ISSN 1463-9076. eISSN 1463-9084. Available under: doi: 10.1039/d0cp03221b
BibTex
@article{Fimpel2020-09-30Doubl-51446,
  year={2020},
  doi={10.1039/d0cp03221b},
  title={Double modulation SRS and SREF microscopy : signal contributions under pre-resonance conditions},
  number={37},
  volume={22},
  issn={1463-9076},
  journal={Physical Chemistry Chemical Physics (PCCP)},
  pages={21421--21427},
  author={Fimpel, Peter and Choorakuttil, Ashwin J. X. and Pruccoli, Andrea and Ebner, Lukas and Tanaka, Shunji and Ozeki, Yasuyuki and Winterhalder, Martin and Zumbusch, Andreas}
}
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