ArticleThe journal of physical chemistry letters2025
Fluorescence-Detected Pump-Probe Spectroscopy for Artifact-Free Detection of Stokes Shift Dynamics.
Article in The journal of physical chemistry letters, 2025. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Not yet cited in PubMed.
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Abstract
Fluorescence-detected pump-probe (F-PP) spectroscopy is a recently developed method to study excited-state dynamics. F-PP combines the temporal resolution of conventional transient absorption (TA) spectroscopy with the sensitivity of fluorescence detection. In this work, we demonstrate inherently phase-stable F-PP spectroscopy using 20 fs pulses to monitor the ultrafast Stokes shift dynamics of a solvated fluorophore (Y12). We observed a shift in the stimulated emission maximum with a time constant of 84 fs. In contrast to TA, F-PP provides a coherent artifact-free view of this process. Using quantitative signal background subtraction, as discussed in this work, F-PP uncovers the pure stimulated emission spectrum and its ultrafast dynamics. This signal isolation is a clear advantage over TA, where different contributions often overlap heavily. We compare results from F-PP and TA on an equal footing using the same excitation pulses, emphasizing the features and advantages of the F-PP technique.
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