DOI: 10.1126/science.1103527. Hydrated Electron Dynamics: From Clusters to Bulk

Hydrated Electron Dynamics: From Clusters to Bulk

10.1126/science.1103527

Crossref journal-article

American Association for the Advancement of Science (AAAS)

Science (221)

Abstract

The electronic relaxation dynamics of size-selected (H 2 O) n – /(D 2 O) n [25 ≤ n ≤ 50] clusters have been studied with time-resolved photoelectron imaging. The excess electron ( \batchmode \documentclass[fleqn,10pt,legalpaper]{article} \usepackage{amssymb} \usepackage{amsfonts} \usepackage{amsmath} \pagestyle{empty} \begin{document} \(e_{c}^{-}\) \end{document} ) was excited through the \batchmode \documentclass[fleqn,10pt,legalpaper]{article} \usepackage{amssymb} \usepackage{amsfonts} \usepackage{amsmath} \pagestyle{empty} \begin{document} \(e_{c}^{-}(p){\leftarrow}e_{c}^{-}(s)\) \end{document} transition with an ultrafast laser pulse, with subsequent evolution of the excited state monitored with photodetachment and photoelectron imaging. All clusters exhibited p-state population decay with concomitant s-state repopulation (internal conversion) on time scales ranging from 180 to 130 femtoseconds for (H 2 O) n – and 400 to 225 femtoseconds for (D 2 O) n – ; the lifetimes decrease with increasing cluster sizes. Our results support the “nonadiabatic relaxation” mechanism for the bulk hydrated electron ( \batchmode \documentclass[fleqn,10pt,legalpaper]{article} \usepackage{amssymb} \usepackage{amsfonts} \usepackage{amsmath} \pagestyle{empty} \begin{document} \(e_{aq}^{-}\) \end{document} ), which invokes a 50-femtosecond \batchmode \documentclass[fleqn,10pt,legalpaper]{article} \usepackage{amssymb} \usepackage{amsfonts} \usepackage{amsmath} \pagestyle{empty} \begin{document} \(e_{aq}^{-}(p){\rightarrow}e_{aq}^{-}(s^{{\dagger}})\) \end{document} internal conversion lifetime.

Bibliography

Bragg, A. E., Verlet, J. R. R., Kammrath, A., Cheshnovsky, O., & Neumark, D. M. (2004). Hydrated Electron Dynamics: From Clusters to Bulk. Science, 306(5696), 669â671.

Authors 5

A. E. Bragg (first)
J. R. R. Verlet (additional)
A. Kammrath (additional)
O. Cheshnovsky (additional)
D. M. Neumark (additional)

References 30 Referenced 249

10.1021/ja00880a025
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J. R. R. Verlet A. Kammrath A. E. Bragg D. M. Neumark unpublished data.
This research is supported by the National Science Foundation under grant no. CHE-0350585. Additional support from the U.S.-Israel Binational Science Foundation is gratefully acknowledged.

Dates

Type	When
Created	20 years, 11 months ago (Sept. 16, 2004, 8:33 p.m.)
Deposited	1 year, 7 months ago (Jan. 9, 2024, 11:31 p.m.)
Indexed	1 month ago (Aug. 2, 2025, 12:19 a.m.)
Issued	20 years, 10 months ago (Oct. 22, 2004)
Published	20 years, 10 months ago (Oct. 22, 2004)
Published Print	20 years, 10 months ago (Oct. 22, 2004)

Funders 0

None

BibTeX

@article{Bragg_2004, title={Hydrated Electron Dynamics: From Clusters to Bulk}, volume={306}, ISSN={1095-9203}, url={http://dx.doi.org/10.1126/science.1103527}, DOI={10.1126/science.1103527}, number={5696}, journal={Science}, publisher={American Association for the Advancement of Science (AAAS)}, author={Bragg, A. E. and Verlet, J. R. R. and Kammrath, A. and Cheshnovsky, O. and Neumark, D. M.}, year={2004}, month=oct, pages={669–671} }

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  "abstract": "<jats:p>\n            The electronic relaxation dynamics of size-selected (H\n            <jats:sub>2</jats:sub>\n            O)\n            <jats:sub>\n              <jats:italic>n</jats:italic>\n            </jats:sub>\n            <jats:sup>\u2013</jats:sup>\n            /(D\n            <jats:sub>2</jats:sub>\n            O)\n            <jats:sub>\n              <jats:italic>n</jats:italic>\n            </jats:sub>\n            [25 \u2264\n            <jats:italic>n</jats:italic>\n            \u2264 50] clusters have been studied with time-resolved photoelectron imaging. The excess electron (\n            <jats:inline-formula>\n              <jats:tex-math notation=\"LaTeX\">\\batchmode \\documentclass[fleqn,10pt,legalpaper]{article} \\usepackage{amssymb} \\usepackage{amsfonts} \\usepackage{amsmath} \\pagestyle{empty} \\begin{document} \\(e_{c}^{-}\\) \\end{document}</jats:tex-math>\n            </jats:inline-formula>\n            ) was excited through the\n            <jats:inline-formula>\n              <jats:tex-math notation=\"LaTeX\">\\batchmode \\documentclass[fleqn,10pt,legalpaper]{article} \\usepackage{amssymb} \\usepackage{amsfonts} \\usepackage{amsmath} \\pagestyle{empty} \\begin{document} \\(e_{c}^{-}(p){\\leftarrow}e_{c}^{-}(s)\\) \\end{document}</jats:tex-math>\n            </jats:inline-formula>\n            transition with an ultrafast laser pulse, with subsequent evolution of the excited state monitored with photodetachment and photoelectron imaging. All clusters exhibited p-state population decay with concomitant s-state repopulation (internal conversion) on time scales ranging from 180 to 130 femtoseconds for (H\n            <jats:sub>2</jats:sub>\n            O)\n            <jats:sub>\n              <jats:italic>n</jats:italic>\n            </jats:sub>\n            <jats:sup>\u2013</jats:sup>\n            and 400 to 225 femtoseconds for (D\n            <jats:sub>2</jats:sub>\n            O)\n            <jats:sub>\n              <jats:italic>n</jats:italic>\n            </jats:sub>\n            <jats:sup>\u2013</jats:sup>\n            ; the lifetimes decrease with increasing cluster sizes. Our results support the \u201cnonadiabatic relaxation\u201d mechanism for the bulk hydrated electron (\n            <jats:inline-formula>\n              <jats:tex-math notation=\"LaTeX\">\\batchmode \\documentclass[fleqn,10pt,legalpaper]{article} \\usepackage{amssymb} \\usepackage{amsfonts} \\usepackage{amsmath} \\pagestyle{empty} \\begin{document} \\(e_{aq}^{-}\\) \\end{document}</jats:tex-math>\n            </jats:inline-formula>\n            ), which invokes a 50-femtosecond\n            <jats:inline-formula>\n              <jats:tex-math notation=\"LaTeX\">\\batchmode \\documentclass[fleqn,10pt,legalpaper]{article} \\usepackage{amssymb} \\usepackage{amsfonts} \\usepackage{amsmath} \\pagestyle{empty} \\begin{document} \\(e_{aq}^{-}(p){\\rightarrow}e_{aq}^{-}(s^{{\\dagger}})\\) \\end{document}</jats:tex-math>\n            </jats:inline-formula>\n            internal conversion lifetime.\n          </jats:p>",
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