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Observation of the fastest chemical processes in the radiolysis of water.

Zhi-Heng LohGilles DoumyCaroline ArnoldLudvig KjellssonStephen H SouthworthA Al HaddadYoshiaki KumagaiMing-Feng TuP J HoAnne-Marie MarchRichard D SchallerM S Bin Mohd YusofTushar DebnathM SimonRalph WelschLudger InhesterKhadijeh KhaliliKaushik D NandaAnna I KrylovS MoellerGiacomo CoslovichJake D KoralekMichael P MinittiWilliam SchlotterJan-Erik RubenssonRobin SantraLinda Young
Published in: Science (New York, N.Y.) (2020)
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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