DOI: 10.1063/1.1309011. The ejection distribution of solvated electrons generated by the one-photon photodetachment of aqueous I− and two-photon ionization of the solvent

The ejection distribution of solvated electrons generated by the one-photon photodetachment of aqueous I− and two-photon ionization of the solvent

10.1063/1.1309011

Crossref journal-article

AIP Publishing

The Journal of Chemical Physics (317)

Abstract

The ultrafast dynamics following one-photon UV photodetachment of I− ions in aqueous solution are compared with those following two-photon ionization of the solvent. Ultrafast pump–probe experiments employing 50 fs ultraviolet pulses reveal similar and very rapid time scales for electron ejection. However, the electron ejection process from water pumped into the conduction band and from iodide ions detached at threshold are readily distinguishable. The observed picosecond timescale geminate recombination and electron escape dynamics are reconstructed using two different models, a diffusion-limited return of the electron from ∼15 Å to its parent and a competing kinetics model governed by the reverse electron transfer rate. We conclude that the “ejected” electron in the halide detachment is merely separated from the halogen atom within the same solvent shell. The assignment of detachment into a contact pair is based on the recombination profile rather than by the postulate of any new spectral absorption due to an electron in a contact pair. The contact pair is surprisingly long-lived and the nonadiabatic recombination is rather slow considering the proximity of the partners. Experiments in mixed solvents confirm our assignment of the two distinct ejection mechanisms. The detachment mechanism is therefore fundamentally different in the resonant (one photon) charge-transfer-to-solvent (CTTS) process from the multiphoton detachment of aqueous iodide ions, which bears more similarity to the direct solvent ionization.

Bibliography

Kloepfer, J. A., Vilchiz, V. H., Lenchenkov, V. A., Germaine, A. C., & Bradforth, S. E. (2000). The ejection distribution of solvated electrons generated by the one-photon photodetachment of aqueous Iâ and two-photon ionization of the solvent. The Journal of Chemical Physics, 113(15), 6288â6307.

Authors 5

J. A. Kloepfer (first)
V. H. Vilchiz (additional)
V. A. Lenchenkov (additional)
A. C. Germaine (additional)
S. E. Bradforth (additional)

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Dates

Type	When
Created	23 years, 1 month ago (July 26, 2002, 8:41 a.m.)
Deposited	2 years, 1 month ago (July 8, 2023, 11:21 a.m.)
Indexed	3 days, 21 hours ago (Aug. 23, 2025, 12:58 a.m.)
Issued	24 years, 10 months ago (Oct. 15, 2000)
Published	24 years, 10 months ago (Oct. 15, 2000)
Published Print	24 years, 10 months ago (Oct. 15, 2000)

Funders 0

None

BibTeX

@article{Kloepfer_2000, title={The ejection distribution of solvated electrons generated by the one-photon photodetachment of aqueous I− and two-photon ionization of the solvent}, volume={113}, ISSN={1089-7690}, url={http://dx.doi.org/10.1063/1.1309011}, DOI={10.1063/1.1309011}, number={15}, journal={The Journal of Chemical Physics}, publisher={AIP Publishing}, author={Kloepfer, J. A. and Vilchiz, V. H. and Lenchenkov, V. A. and Germaine, A. C. and Bradforth, S. E.}, year={2000}, month=oct, pages={6288–6307} }

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  "abstract": "<jats:p>The ultrafast dynamics following one-photon UV photodetachment of I\u2212 ions in aqueous solution are compared with those following two-photon ionization of the solvent. Ultrafast pump\u2013probe experiments employing 50 fs ultraviolet pulses reveal similar and very rapid time scales for electron ejection. However, the electron ejection process from water pumped into the conduction band and from iodide ions detached at threshold are readily distinguishable. The observed picosecond timescale geminate recombination and electron escape dynamics are reconstructed using two different models, a diffusion-limited return of the electron from \u223c15\u200a\u00c5 to its parent and a competing kinetics model governed by the reverse electron transfer rate. We conclude that the \u201cejected\u201d electron in the halide detachment is merely separated from the halogen atom within the same solvent shell. The assignment of detachment into a contact pair is based on the recombination profile rather than by the postulate of any new spectral absorption due to an electron in a contact pair. The contact pair is surprisingly long-lived and the nonadiabatic recombination is rather slow considering the proximity of the partners. Experiments in mixed solvents confirm our assignment of the two distinct ejection mechanisms. The detachment mechanism is therefore fundamentally different in the resonant (one photon) charge-transfer-to-solvent (CTTS) process from the multiphoton detachment of aqueous iodide ions, which bears more similarity to the direct solvent ionization.</jats:p>",
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