Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 34, Pages 18867-18875Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202102901
Keywords
femtochemistry; FL spectroscopy; time-resolved spectroscopy; transient absorption
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Funding
- Alexander von Humboldt foundation
- Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) [423942615]
- Projekt DEAL
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Fluorescence-detected pump-probe (F-PP) spectroscopy is a new approach to transient spectroscopy that overcomes limitations of traditional methods, providing background-free detection and unique extraction of excited-state dynamics under certain conditions. Despite incoherent detection, F-PP offers time resolution independent of fluorescence lifetime and is broadly applicable to chemical systems in different environments and spectral regimes.
We introduce a new approach to transient spectroscopy, fluorescence-detected pump-probe (F-PP) spectroscopy, that overcomes several limitations of traditional PP. F-PP suppresses excited-state absorption, provides background-free detection, removes artifacts resulting from pump-pulse scattering, from non-resonant solvent response, or from coherent pulse overlap, and allows unique extraction of excited-state dynamics under certain conditions. Despite incoherent detection, time resolution of F-PP is given by the duration of the laser pulses, independent of the fluorescence lifetime. We describe the working principle of F-PP and provide its theoretical description. Then we illustrate specific features of F-PP by direct comparison with PP, theoretically and experimentally. For this purpose, we investigate, with both techniques, a molecular squaraine heterodimer, core-shell CdSe/ZnS quantum dots, and fluorescent protein mCherry. F-PP is broadly applicable to chemical systems in various environments and in different spectral regimes.
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