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; Khadijeh 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, Khadijeh Khalili, K Nanda, A I Krylov, S MoellerG Coslovich, J Koralek, M P Minitti, W F Schlotter, J-E Rubensson, R Santra, L Young

Department of Energy Conversion and Storage

German Electron Synchrotron

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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
Journal	Science
Volume	367
Issue number	6474
Pages (from-to)	179-182
ISSN	0036-8075
DOIs	https://doi.org/10.1126/science.aaz4740
Publication status	Published - 2020

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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 = "Z-H Loh and G Doumy and C Arnold and L Kjellsson and Southworth, {S H} and {Al Haddad}, A and Y Kumagai and M-F Tu 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 Khadijeh 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 J-E Rubensson and R Santra and L Young",

year = "2020",

doi = "10.1126/science.aaz4740",

language = "English",

volume = "367",

pages = "179--182",

journal = "Science",

issn = "0036-8075",

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Loh, Z-H, Doumy, G, Arnold, C, Kjellsson, L, Southworth, SH, Al Haddad, A, Kumagai, Y, Tu, M-F, 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, J-E, 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, Khadijeh

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

Y1 - 2020

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.

U2 - 10.1126/science.aaz4740

DO - 10.1126/science.aaz4740

M3 - Journal article

C2 - 31919219

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

Abstract

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