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- W4313421710 abstract "Fluorescence-detected multidimensional electronic spectroscopy (fMES) promises high sensitivity compared to conventional approaches and is an emerging spectroscopic approach toward combining the advantages of MES with the spatial resolution of a microscope. Here, we present a visible white light continuum-based fMES spectrometer and systematically explore the sensitivity enhancement expected from fluorescence detection. As a demonstration of sensitivity, we report room temperature two-dimensional coherence maps of vibrational quantum coherences in a laser dye at optical densities of ∼2-3 orders of magnitude lower than conventional approaches. This high sensitivity is enabled by a combination of biased sampling along the optical coherence time axes and a rapid scan of the pump-probe waiting time T at each sample. A combination of this approach with acousto-optic phase modulation and phase-sensitive lock-in detection enables measurements of room temperature vibrational wavepackets even at the lowest ODs. Alternative faster data collection schemes, which are enabled by the flexibility of choosing a non-uniform undersampled grid in the continuous T scanning approach, are also demonstrated." @default.
- W4313421710 created "2023-01-06" @default.
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- W4313421710 date "2023-01-14" @default.
- W4313421710 modified "2023-10-05" @default.
- W4313421710 title "High-sensitivity fluorescence-detected multidimensional electronic spectroscopy through continuous pump–probe delay scan" @default.
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- W4313421710 doi "https://doi.org/10.1063/5.0130887" @default.
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