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High-sensitivity fluorescence-detected multidimensional electronic spectroscopy through continuous pump-probe delay scan

Sahu, A and Bhat, VN and Patra, S and Tiwari, V (2023) High-sensitivity fluorescence-detected multidimensional electronic spectroscopy through continuous pump-probe delay scan. In: Journal of Chemical Physics, 158 (2).

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Official URL: https://doi.org/10.1063/5.0130887


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.

Item Type: Journal Article
Publication: Journal of Chemical Physics
Publisher: American Institute of Physics Inc.
Additional Information: The copyright for this article belongs to the Authors.
Keywords: Probes; Quantum theory; Room temperature; Spectrometers, Conventional approach; Electronic spectroscopy; Fluorescence detection; High sensitivity; Is-enabled; Pump-probe delays; Sensitivity enhancements; Spatial resolution; Spectroscopy:spectrometers; White-light continuum, Fluorescence, electronics; optics; spectrofluorometry, Electronics; Optics and Photonics; Spectrometry, Fluorescence
Department/Centre: Division of Chemical Sciences > Solid State & Structural Chemistry Unit
Date Deposited: 09 Feb 2023 05:42
Last Modified: 09 Feb 2023 05:42
URI: https://eprints.iisc.ac.in/id/eprint/80108

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