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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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.
| Item Type: | Journal Article |
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| 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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