Spatiotemporal control of degenerate multiphoton fluorescence microscopy with delay-tunable femtosecond pulse pairs

Three new stilbenyl‐azopyrroles 3 a–c were synthesized through a Mizoroki‐Heck C−C‐type coupling reaction between the 2‐(4′‐iodophenyl‐azo)‐N‐methyl pyrrole (1), and three different para‐substituted styrene derivatives. Inclusion of additional NO2 and NMe2 groups at the para‐position of the stilbenyl section resulted in significant changes of their linear and non‐linear optical properties. The photoisomerization behavior was studied through ultrafast laser techniques for single‐ and two‐photon excitation. The time‐resolved studies indicate that, despite the drastic changes in conjugation, the typical path for photoisomerization is maintained in these systems for both single and biphotonic excitation. In particular, the NO2 substituted molecule showed improved two‐photon absorption capacities, together with a significant trans−cis isomerization channel, implying that the photoswitching process can be controlled with high spatial precision through non‐linear optical excitation.

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Synthesis and Photodynamics of Stilbenyl‐Azopyrroles: Two‐Photon Controllable Photoswitching Systems

Muñoz‐Rugeles

Gallardo‐Rosas

Durán-Hernández

et al. 2019

ChemPhotoChem

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Concurrent biomineralization of silver ions into Ag0 and AgxO by Leptolyngbya strain JSC-1 and the establishment of its axenic culture

et al. 2019

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Probing solvent dependent femtosecond transient coherent oscillations to reveal interfacial dynamics

Das

Makhal

Goswami

2022

J. Opt.

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Probing transient states in molecules having vibronic transitions with femtosecond laser pulses often results in coherent oscillations either in the ground state, the excited states, or both. We find such coherent oscillations are highly solvent-dependent and provide a holistic overview of the pump-probe experiments for ultrafast dye dynamics at interfaces. For molecules dissolved in single solvents, modulations in oscillations occur due to transitions in the sub-vibrational levels of the electronic state. For binary solvents, in particular, these modulations are strongly sensitive to solvent compositions. The changes induced by various solvent compositions are drastic enough to act as a control parameter for dynamical control processes. We demonstrate an end-to-end understanding of ground-state coherent oscillations, vibrational cooling, ground-state recovery processes, and excited-state dynamics through a series of experiments. We further present a methodology for establishing such control using near-infrared dyes to measure the oscillations with femtosecond pump-probe techniques. In the case of immiscible binary solvents, the same method allows us to investigate the liquid-liquid interface. Our control methodology is validated by an experiment using a cyanine dye dissolved in dimethyl sulfoxide, interfaced with neat diethyl-ether. The dye dynamics are retarded on moving from the bulk dye solution towards the interface with the neat diethyl-ether. When sampled along the direction of the vector pointing from the bulk towards the near interface, monotonically decreasing time constants are obtained. This result strongly suggests the importance of microheterogeneity in interfacial dynamics.

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Spatiotemporal control of degenerate multiphoton fluorescence microscopy with delay-tunable femtosecond pulse pairs

Cited by 3 publications

References 27 publications

Synthesis and Photodynamics of Stilbenyl‐Azopyrroles: Two‐Photon Controllable Photoswitching Systems

Synthesis and Photodynamics of Stilbenyl‐Azopyrroles: Two‐Photon Controllable Photoswitching Systems

Concurrent biomineralization of silver ions into Ag0 and AgxO by Leptolyngbya strain JSC-1 and the establishment of its axenic culture

Probing solvent dependent femtosecond transient coherent oscillations to reveal interfacial dynamics

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