Observation of the fastest chemical processes in the radiolysis of water

Z. H. Loh; G. Doumy; C. Arnold; L. Kjellsson; S. H. Southworth; A. Al Haddad; Y. Kumagai; M. F. Tu; P. J. Ho; A. M. March; R. D. Schaller; M. S. Bin Mohd Yusof; T. Debnath; M. Simon; R. Welsch; L. Inhester; K. Khalili; K. Nanda; A. I. Krylov; S. Moeller; G. Coslovich; J. Koralek; M. P. Minitti; W. F. Schlotter; J. E. Rubensson; R. Santra; L. Young

doi:10.1126/science.aaz4740

Observation of the fastest chemical processes in the radiolysis of water

Z. H. Loh^*, G. Doumy, C. Arnold, L. Kjellsson, S. H. Southworth, A. Al Haddad, Y. Kumagai, M. F. Tu, P. J. Ho, A. M. March, R. D. Schaller, M. S. Bin Mohd Yusof, T. Debnath, M. Simon, R. Welsch, L. Inhester, K. Khalili, K. Nanda, A. I. Krylov, S. MoellerG. Coslovich, J. Koralek, M. P. Minitti, W. F. Schlotter, J. E. Rubensson, R. Santra, L. Young

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

161 Scopus citations

Abstract

Elementary processes associated with ionization of liquid water provide a framework for understanding radiation-matter interactions in chemistry and biology. Although numerous studies have been conducted on the dynamics of the hydrated electron, its partner arising from ionization of liquid water, H₂O⁺, remains elusive. We used tunable femtosecond soft x-ray pulses from an x-ray free electron laser to reveal the dynamics of the valence hole created by strong-field ionization and to track the primary proton transfer reaction giving rise to the formation of OH. The isolated resonance associated with the valence hole (H₂O⁺/OH) enabled straightforward detection. Molecular dynamics simulations revealed that the x-ray spectra are sensitive to structural dynamics at the ionization site. We found signatures of hydrated-electron dynamics in the x-ray spectrum.

Original language	English (US)
Pages (from-to)	179-182
Number of pages	4
Journal	Science
Volume	367
Issue number	6474
DOIs	https://doi.org/10.1126/science.aaz4740
State	Published - Jan 10 2020

Funding

Funding: Supported by the U.S. Department of Energy (DOE) Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, which supports the Argonne group under contract DE-AC02-06CH11357. Use of the LCLS, SLAC National Accelerator Laboratory, and resources of the Center for Nanoscale Materials, Argonne National Laboratory, are supported by DOE Office of Science, Office of Basic Energy Sciences under contracts DE-AC02-76SF00515 and DE-AC02-06CH11357. Also supported by Laboratory Directed Research and Development funding from Argonne National Laboratory for conceptual design and proposal preparation (L.Y.); Singapore Ministry of Education grants MOE2014-T2-2-052 and RG105/17 (Z.-H.L., M.S.B.M.Y., and T.D.); Swedish Science Council grant 2018-04088 (L.K. and J.-E.R.); the CNRS GotoXFEL program (M.S.); the Deutsche Forschungsgemeinschaft Cluster of Excellence “Advanced Imaging of Matter” (EXC 2056, project ID 390715994) (C.A., R.W., and R.S.); DOE Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division grant DE-SC0019451 (L.I. and R.S.); the European Research Council under the European Union's Horizo 2020 research and innovation program (grant agreement 681881) (K.K.); NSF grant CHE-1856342 (A.I.K. and K.N.); and a Simons Fellowship in Theoretical Physics and Mildred Dresselhaus Award from the Hamburg Centre for Ultrafast Imaging, which supported a sabbatical at DESY in Germany (A.I.K.)

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Loh, Z. H., Doumy, G., Arnold, C., Kjellsson, L., Southworth, S. H., Al Haddad, A., Kumagai, Y., Tu, M. F., Ho, P. J., March, A. M., Schaller, R. D., Bin Mohd Yusof, M. S., Debnath, T., Simon, M., Welsch, R., Inhester, L., Khalili, K., Nanda, K., Krylov, A. I., ... Young, L. (2020). Observation of the fastest chemical processes in the radiolysis of water. Science, 367(6474), 179-182. https://doi.org/10.1126/science.aaz4740

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title = "Observation of the fastest chemical processes in the radiolysis of water",

abstract = "Elementary processes associated with ionization of liquid water provide a framework for understanding radiation-matter interactions in chemistry and biology. Although numerous studies have been conducted on the dynamics of the hydrated electron, its partner arising from ionization of liquid water, H2O+, remains elusive. We used tunable femtosecond soft x-ray pulses from an x-ray free electron laser to reveal the dynamics of the valence hole created by strong-field ionization and to track the primary proton transfer reaction giving rise to the formation of OH. The isolated resonance associated with the valence hole (H2O+/OH) enabled straightforward detection. Molecular dynamics simulations revealed that the x-ray spectra are sensitive to structural dynamics at the ionization site. We found signatures of hydrated-electron dynamics in the x-ray spectrum.",

author = "Loh, {Z. H.} and G. Doumy and C. Arnold and L. Kjellsson and Southworth, {S. H.} and {Al Haddad}, A. and Y. Kumagai and Tu, {M. F.} and Ho, {P. J.} and March, {A. M.} and Schaller, {R. D.} and {Bin Mohd Yusof}, {M. S.} and T. Debnath and M. Simon and R. Welsch and L. Inhester and K. Khalili and K. Nanda and Krylov, {A. I.} and S. Moeller and G. Coslovich and J. Koralek and Minitti, {M. P.} and Schlotter, {W. F.} and Rubensson, {J. E.} and R. Santra and L. Young",

year = "2020",

month = jan,

day = "10",

doi = "10.1126/science.aaz4740",

language = "English (US)",

volume = "367",

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Loh, ZH, Doumy, G, Arnold, C, Kjellsson, L, Southworth, SH, Al Haddad, A, Kumagai, Y, Tu, MF, Ho, PJ, March, AM, Schaller, RD, Bin Mohd Yusof, MS, Debnath, T, Simon, M, Welsch, R, Inhester, L, Khalili, K, Nanda, K, Krylov, AI, Moeller, S, Coslovich, G, Koralek, J, Minitti, MP, Schlotter, WF, Rubensson, JE, Santra, R & Young, L 2020, 'Observation of the fastest chemical processes in the radiolysis of water', Science, vol. 367, no. 6474, pp. 179-182. https://doi.org/10.1126/science.aaz4740

TY - JOUR

T1 - Observation of the fastest chemical processes in the radiolysis of water

AU - Loh, Z. H.

AU - Doumy, G.

AU - Arnold, C.

AU - Kjellsson, L.

AU - Southworth, S. H.

AU - Al Haddad, A.

AU - Kumagai, Y.

AU - Tu, M. F.

AU - Ho, P. J.

AU - March, A. M.

AU - Schaller, R. D.

AU - Bin Mohd Yusof, M. S.

AU - Debnath, T.

AU - Simon, M.

AU - Welsch, R.

AU - Inhester, L.

AU - Khalili, K.

AU - Nanda, K.

AU - Krylov, A. I.

AU - Moeller, S.

AU - Coslovich, G.

AU - Koralek, J.

AU - Minitti, M. P.

AU - Schlotter, W. F.

AU - Rubensson, J. E.

AU - Santra, R.

AU - Young, L.

PY - 2020/1/10

Y1 - 2020/1/10

N2 - Elementary processes associated with ionization of liquid water provide a framework for understanding radiation-matter interactions in chemistry and biology. Although numerous studies have been conducted on the dynamics of the hydrated electron, its partner arising from ionization of liquid water, H2O+, remains elusive. We used tunable femtosecond soft x-ray pulses from an x-ray free electron laser to reveal the dynamics of the valence hole created by strong-field ionization and to track the primary proton transfer reaction giving rise to the formation of OH. The isolated resonance associated with the valence hole (H2O+/OH) enabled straightforward detection. Molecular dynamics simulations revealed that the x-ray spectra are sensitive to structural dynamics at the ionization site. We found signatures of hydrated-electron dynamics in the x-ray spectrum.

AB - Elementary processes associated with ionization of liquid water provide a framework for understanding radiation-matter interactions in chemistry and biology. Although numerous studies have been conducted on the dynamics of the hydrated electron, its partner arising from ionization of liquid water, H2O+, remains elusive. We used tunable femtosecond soft x-ray pulses from an x-ray free electron laser to reveal the dynamics of the valence hole created by strong-field ionization and to track the primary proton transfer reaction giving rise to the formation of OH. The isolated resonance associated with the valence hole (H2O+/OH) enabled straightforward detection. Molecular dynamics simulations revealed that the x-ray spectra are sensitive to structural dynamics at the ionization site. We found signatures of hydrated-electron dynamics in the x-ray spectrum.

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AN - SCOPUS:85077680035

SN - 0036-8075

VL - 367

SP - 179

EP - 182

JO - Science

JF - Science

IS - 6474

ER -

Observation of the fastest chemical processes in the radiolysis of water

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