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Attosecond-pump attosecond-probe x-ray spectroscopy of liquid water.

Shuai LiLixin LuSwarnendu BhattacharyyaCarolyn I PearceKai LiEmily T NienhuisGilles DoumyRichard D SchallerStefan MoellerMing-Fu LinG DakovskiDavid J HoffmanDouglas GarrattKirk A LarsenJake D KoralekC Y HamptonD CesarJoseph DurisZhen ZhangNicholas SudarJames P CryanAgostino MarinelliXiaosong LiLudger InhesterRobin SantraLinda Young
Published in: Science (New York, N.Y.) (2024)
Attosecond-pump/attosecond-probe experiments have long been sought as the most straightforward method for observing electron dynamics in real time. Although there has been much success with overlapped near-infrared femtosecond and extreme ultraviolet attosecond pulses combined with theory, true attosecond-pump/attosecond-probe experiments have been limited. We used a synchronized attosecond x-ray pulse pair from an x-ray free-electron laser to study the electronic response to valence ionization in liquid water through all x-ray attosecond transient absorption spectroscopy (AX-ATAS). Our analysis showed that the AX-ATAS response is confined to the subfemtosecond timescale, eliminating any hydrogen atom motion and demonstrating experimentally that the 1b 1 splitting in the x-ray emission spectrum is related to dynamics and is not evidence of two structural motifs in ambient liquid water.
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