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Rapid scan white light two-dimensional electronic spectroscopy with 100 kHz shot-to-shot detection

Thomas, AS and Bhat, VN and Tiwari, V (2023) Rapid scan white light two-dimensional electronic spectroscopy with 100 kHz shot-to-shot detection. In: Journal of Chemical Physics, 159 (24).

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Official URL: https://doi.org/10.1063/5.0179474


We demonstrate an approach to two-dimensional electronic spectroscopy (2DES) that combines the benefits of shot-to-shot detection at high-repetition rates with the simplicity of a broadband white light continuum input and conventional optical elements to generate phase-locked pump pulse pairs. We demonstrate this through mutual synchronization between the laser repetition rate, the acousto-optical deflector, the pump delay stage, and the CCD line camera, which allows for rapid scanning of pump optical delay synchronously with the laser repetition rate, while the delay stage is moved at a constant velocity. The resulting shot-to-shot detection scheme is repetition rate scalable and only limited by the CCD line rate and the maximum stage velocity. Using this approach, we demonstrate the measurement of an averaged 2DES absorptive spectrum in as much as 1.2 s of continuous sample exposure per 2D spectrum. We achieve a signal-to-noise ratio of 6.8 for optical densities down to 0.05 with 11.6 s of averaging at 100 kHz laser repetition rate. Combining rapid scanning of mechanical delay lines with shot-to-shot detection as demonstrated here provides a viable alternative to acousto-optic pulse shaping approaches that is repetition-rate scalable, has comparable throughput and sensitivity, and minimizes sample exposure per 2D spectrum with promising micro-spectroscopy applications. © 2023 Author(s).

Item Type: Journal Article
Publication: Journal of Chemical Physics
Publisher: American Institute of Physics Inc.
Additional Information: The copyright for this article belongs to Author.
Keywords: Optical pumping; Pulse repetition rate; Signal to noise ratio, 2D spectra; CCD lines; Delay stages; Laser repetition rate; Rapid scan; Rapid scanning; Repetition rate; Shot detection; Two-dimensional electronic spectroscopies; White light, Pulse shaping, absorption; adolescent; article; camera; controlled study; laser; optical density; pharmaceutics; signal noise ratio; spectroscopy; velocity; white light
Department/Centre: Division of Chemical Sciences > Solid State & Structural Chemistry Unit
Date Deposited: 01 Mar 2024 09:31
Last Modified: 01 Mar 2024 09:31
URI: https://eprints.iisc.ac.in/id/eprint/84008

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