Transient Grating Investigations at Liquid–Liquid Interfaces

Punzi, Angela; Brodard, Pierre; Vauthey, Eric

doi:10.2533/000942905777676777

Cited by 3 publications

(4 citation statements)

References 8 publications

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“…49 Finally, the excited-state lifetime of R6G at the decaline/methanol interface measured using the evanescent transient grating technique was found to be twice as small as that in bulk methanol at the same concentration. 50,51 However, this technique, like total internal reflection fluorescence, 52 is not intrinsically selective to the interface as it probes a layer close to the interface that is several hundreds of nanometers thick, and thus dye populations in both the interfacial and the bulk regions contribute to the signal.…”

Section: ■ Introductionmentioning

confidence: 99%

Excited-State Dynamics of Rhodamine 6G in Aqueous Solution and at the Dodecane/Water Interface

2014

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The excited-state dynamics of rhodamine 6G (R6G) has been investigated in aqueous solution using ultrafast transient absorption spectroscopy and at the dodecane/water interface using the femtosecond time-resolved surface second harmonic generation (SSHG) technique. As the R6G concentration exceeds ca. 1 mM in bulk water, both R6G monomers and aggregates are excited to a different extent when using pump pulses at 500 and 530 nm. The excited-state lifetime of the monomers is shortened compared to dilute solutions because of the occurrence of excitation energy transfer to the aggregates, which themselves decay nonradiatively to the ground state with a ca. 70 ps time constant. At the dodecane/water interface, both monomers and aggregates contribute to the SSHG signal to an extent that depends on the bulk concentration, the pump and probe wavelengths, and the polarization of probe and signal beams. The excited-state lifetime of the monomers at the interface is of the order of a few picoseconds even at bulk concentrations where it is as large as several nanoseconds. This is explained by the relatively high interfacial affinity of R6G that leads to a large interfacial concentration, favoring aggregation and thus rapid excitation energy transfer from monomers to aggregates.

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Section: ■ Introductionmentioning

confidence: 99%

Excited-State Dynamics of Rhodamine 6G in Aqueous Solution and at the Dodecane/Water Interface

2014

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“…Moving beyond linear spectroscopy, many nonlinear techniques have also previously integrated TIR to take advantage of the evanescent wave’s depth into a sample to measure properties of interfacial regions. Most nonlinear applications have relied on a prism based configuration with only one of the two beams that interact with the sample in a TIR geometry. − For example, two-photon fluorescence, second harmonic generation, transient grating, and transient absorption , have previously used a focused pump with only the probe beam incident in the TIR geometry. Shimosaka et al introduced only the pump beam onto the sample in the TIR geometry for their photothermal spectroscopy experiment while Sugimoto et al used both a pump and probe in TIR for their transient lens, albeit in a prism configuration .…”

Section: Introductionmentioning

confidence: 99%

Total Internal Reflection Transient Absorption Microscopy: An Online Detection Method for Microfluidics

et al. 2020

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Microreactors have garnered widespread attention for their tunability and precise control of synthetic parameters to efficiently produce target species. Despite associated advances, a lack of online detection and optimization methods has stalled the progression of microfluidic reactors. Here we employ and characterize a total internal reflection transient absorption microscopy (TIRTAM) instrument to image excited state dynamics on a continuous flow device. The experiments presented demonstrate the capability to discriminate between different chromophores as well as in differentiating the effects of local chemical environments that a chromophore experiences. This work presents the first such online transient absorption measurements and provides a new direction for the advancement and optimization of chemical reactions in microfluidic devices.

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“…This difficulty could be partially alleviated by measuring different tensor elements of χ (2) by varying the polarization of the pump, probe, and signal fields. Finally, if the interfacial concentration of probe molecules is high, the hopping of the excitation energy between nearby molecules might be wrongly interpreted as diffusional reorientation …”

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confidence: 99%

“…Finally, if the interfacial concentration of probe molecules is high, the hopping of the excitation energy between nearby molecules might be wrongly interpreted as diffusional reorientation. 30 Although this might not be as evident as solvent and orientation relaxation, the excited-state dynamics of a wellchosen probe can also yield precious information on its local environment. For example, the dynamics of nonradiative deactivation processes involving an intramolecular coordinate with large-amplitude motion is very sensitive to local friction, and in bulk solution, the viscosity dependence of the measured decay time can be expressed as τ nr ∝ η ∝ , where α varies between 0.1 and 1 depending on the molecule.…”

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confidence: 99%

Ultrafast Photoinduced Dynamics at Air/Liquid and Liquid/Liquid Interfaces

Richert

Fedoseeva

Vauthey

2012

J. Phys. Chem. Lett.

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Although liquid/liquid and air/liquid interfaces are omnipresent, very little is known up to now about the dynamics of processes occurring at such interfaces. As a detailed understanding of these processes could be of invaluable technological, environmental, and medical importance, considerable effort has been invested over the last two decades in developing new interface-selective techniques that allow for gaining further insight into the dynamics of these processes. Whereas several major results have been achieved that helped to contribute to a deeper understanding, there are still many aspects concerning the properties of liquid interfaces that are not yet fully understood. In this Perspective, the work that has been carried out so far on photoinduced interfacial dynamics will be reviewed and the current challenges in this still emerging field of research discussed.

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Transient Grating Investigations at Liquid–Liquid Interfaces

Abstract: A new four-wave-mixing technique with evanescent optical fields generated by total internal reflection at a liquid-liquid interface is described. Several applications of this method to measure thermoacoustic and dynamic properties near liquid-liquid interfaces are presented.

Cited by 3 publications

References 8 publications

Excited-State Dynamics of Rhodamine 6G in Aqueous Solution and at the Dodecane/Water Interface

Excited-State Dynamics of Rhodamine 6G in Aqueous Solution and at the Dodecane/Water Interface

Total Internal Reflection Transient Absorption Microscopy: An Online Detection Method for Microfluidics

Ultrafast Photoinduced Dynamics at Air/Liquid and Liquid/Liquid Interfaces

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