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

Sahu, Amitav; Bhat, Vivek Nagendra; Patra, Sanjoy; Tiwari, Vivek

doi:10.1063/5.0130887

Cited by 9 publications

(2 citation statements)

References 118 publications

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“…The derivation presented above suggests that the diagonal node-like feature is not specific to BChl a . Recent real rephasing CMs for Oxazine 720 monomers are consistent with this expectation. In a broader context, a node-like DP lineshape is a direct readout that distinguishes spectator vibrational modes that survive electronic relaxation from promoter modes that do not.…”

supporting

confidence: 65%

Vibrations That Do Not Promote Vibronic Coupling Can Dominate Observed Lineshapes in Two-Dimensional Electronic Spectroscopy

Sahu

Tiwari

2023

J. Phys. Chem. Lett.

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Impulsively generated wavepackets can report on vibronic couplings underlying ultrafast electronic relaxation. Coherence maps (CMs) in multidimensional spectroscopy resolve beating amplitudes of such wavepackets as two-dimensional contour maps. A precise understanding of how these wavepackets manifest spectroscopically is vital for unambiguously deciphering their mechanistic significance and establishing CMs as a powerful tool for guiding the synthetic design of functional vibronic couplings. Here we take a step in this direction. We establish physically distinct origins of recently reported apparent similarities between diagonal node-like CM lineshapes in bacteriochlorophyll monomers and multichromophoric photosynthetic reaction centers (RCs). The former arise when vibrational wavepackets survive on both ground and excited electronic states, while nodal lines in RCs arise when vibrational wavepackets that do not participate in energy transfer are coherently transferred to the acceptor. We resolve recent spectroscopic observations and illustrate new mechanistic insights gained by connecting microscopic interference between electronic relaxation pathways and observed CMs.

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supporting

confidence: 65%

Vibrations That Do Not Promote Vibronic Coupling Can Dominate Observed Lineshapes in Two-Dimensional Electronic Spectroscopy

Sahu

Tiwari

2023

J. Phys. Chem. Lett.

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“…By scanning through the pump–probe time-delay, the change in total detected photons reports on the temporal evolution of the stimulated emission within the spectral window of the probe. Comparable measurements have been performed using white light …”

Section: Scientific Insights and Instrumental Achievements In Transie...mentioning

confidence: 99%

Progress and Prospects in Optical Ultrafast Microscopy in the Visible Spectral Region: Transient Absorption and Two-Dimensional Microscopy

Gross,

Kuhs,

Ostovar

et al. 2023

J. Phys. Chem. C

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Ultrafast optical microscopy, generally employed by incorporating ultrafast laser pulses into microscopes, can provide spatially resolved mechanistic insight into scientific problems ranging from hot carrier dynamics to biological imaging. This Review discusses the progress in different ultrafast microscopy techniques, with a focus on transient absorption and twodimensional microscopy. We review the underlying principles of these techniques and discuss their respective advantages and applicability to different scientific questions. We also examine in detail how instrument parameters such as sensitivity, laser power, and temporal and spatial resolution must be addressed. Finally, we comment on future developments and emerging opportunities in the field of ultrafast microscopy.

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

Thomas,

Bhat,

Tiwari

2023

The Journal of Chemical Physics

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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.

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

Cited by 9 publications

References 118 publications

Vibrations That Do Not Promote Vibronic Coupling Can Dominate Observed Lineshapes in Two-Dimensional Electronic Spectroscopy

Vibrations That Do Not Promote Vibronic Coupling Can Dominate Observed Lineshapes in Two-Dimensional Electronic Spectroscopy

Progress and Prospects in Optical Ultrafast Microscopy in the Visible Spectral Region: Transient Absorption and Two-Dimensional Microscopy

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

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