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.
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14 January 2023
Research Article|
January 09 2023
High-sensitivity fluorescence-detected multidimensional electronic spectroscopy through continuous pump–probe delay scan
Special Collection:
2022 JCP Emerging Investigators Special Collection
Amitav Sahu
;
Amitav Sahu
(Formal analysis, Methodology, Software, Writing – original draft, Writing – review & editing)
Solid State and Structural Chemistry Unit, Indian Institute of Science
, Bangalore, Karnataka, 560012, India
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Vivek N. Bhat
;
Vivek N. Bhat
(Formal analysis, Methodology)
Solid State and Structural Chemistry Unit, Indian Institute of Science
, Bangalore, Karnataka, 560012, India
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Sanjoy Patra
;
Sanjoy Patra
(Formal analysis, Methodology, Writing – original draft)
Solid State and Structural Chemistry Unit, Indian Institute of Science
, Bangalore, Karnataka, 560012, India
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Vivek Tiwari
Vivek Tiwari
a)
(Conceptualization, Funding acquisition, Methodology, Software, Supervision, Writing – original draft, Writing – review & editing)
Solid State and Structural Chemistry Unit, Indian Institute of Science
, Bangalore, Karnataka, 560012, India
a)Author to whom correspondence should be addressed: vivektiwari@iisc.ac.in
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a)Author to whom correspondence should be addressed: vivektiwari@iisc.ac.in
Note: This paper is part of the 2022 JCP Emerging Investigators Special Collection.
J. Chem. Phys. 158, 024201 (2023)
Article history
Received:
October 15 2022
Accepted:
December 19 2022
Citation
Amitav Sahu, Vivek N. Bhat, Sanjoy Patra, Vivek Tiwari; High-sensitivity fluorescence-detected multidimensional electronic spectroscopy through continuous pump–probe delay scan. J. Chem. Phys. 14 January 2023; 158 (2): 024201. https://doi.org/10.1063/5.0130887
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