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Real-time structural dynamics of the ultrafast solvation process around photo-excited aqueous halides.

ABSTRACT: This work investigates and describes the structural dynamics taking place following charge-transfer-to-solvent photo-abstraction of electrons from I^- and Br^- ions in aqueous solution following single- and 2-photon excitation at 202 nm and 400 nm, respectively. A Time-Resolved X-ray Solution Scattering (TR-XSS) approach with direct sensitivity to the structure of the surrounding solvent as the water molecules adopt a new equilibrium configuration following the electron-abstraction process is utilized to investigate the structural dynamics of solvent shell expansion and restructuring in real-time. The structural sensitivity of the scattering data enables a quantitative evaluation of competing models for the interaction between the nascent neutral species and surrounding water molecules. Taking the I⁰-O distance as the reaction coordinate, we find that the structural reorganization is delayed by 0.1 ps with respect to the photoexcitation and completes on a time scale of 0.5-1 ps. On longer time scales we determine from the evolution of the TR-XSS difference signal that I⁰: e^- recombination takes place on two distinct time scales of ∼20 ps and 100 s of picoseconds. These dynamics are well captured by a simple model of diffusive evolution of the initial photo-abstracted electron population where the charge-transfer-to-solvent process gives rise to a broad distribution of electron ejection distances, a significant fraction of which are in the close vicinity of the nascent halogen atoms and recombine on short time scales.

SUBMITTER: Markmann V

PROVIDER: S-EPMC11268492 | biostudies-literature | 2024 Jul

REPOSITORIES: biostudies-literature

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Real-time structural dynamics of the ultrafast solvation process around photo-excited aqueous halides.

Markmann Verena V Pan Jaysree J Hansen Bianca L BL Haubro Morten L ML Nimmrich Amke A Lenzen Philipp P Levantino Matteo M Katayama Tetsuo T Adachi Shin-Ichi SI Gorski-Bilke Simone S Temps Friedrich F Dohn Asmus O AO Møller Klaus B KB Nielsen Martin M MM Haldrup Kristoffer K

Chemical science 20240612 29

This work investigates and describes the structural dynamics taking place following charge-transfer-to-solvent photo-abstraction of electrons from I<sup>-</sup> and Br<sup>-</sup> ions in aqueous solution following single- and 2-photon excitation at 202 nm and 400 nm, respectively. A Time-Resolved X-ray Solution Scattering (TR-XSS) approach with direct sensitivity to the structure of the surrounding solvent as the water molecules adopt a new equilibrium configuration following the electron-abstr ...[more]

PMID: 39055005

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Dataset Information

Real-time structural dynamics of the ultrafast solvation process around photo-excited aqueous halides.

Publications

Real-time structural dynamics of the ultrafast solvation process around photo-excited aqueous halides.

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