TY - JOUR
T1 - Tracking Cavity Formation in Electron Solvation
T2 - Insights from X-ray Spectroscopy and Theory
AU - Sopena Moros, Arturo
AU - Li, Shuai
AU - Li, Kai
AU - Doumy, Gilles
AU - Southworth, Stephen H.
AU - Otolski, Christopher
AU - Schaller, Richard D.
AU - Kumagai, Yoshiaki
AU - Rubensson, Jan Erik
AU - Simon, Marc
AU - Dakovski, Georgi
AU - Kunnus, Kristjan
AU - Robinson, Joseph S.
AU - Hampton, Christina Y.
AU - Hoffman, David J.
AU - Koralek, Jake
AU - Loh, Zhi Heng
AU - Santra, Robin
AU - Inhester, Ludger
AU - Young, Linda
N1 - Publisher Copyright:
© 2024 The Authors. Published by American Chemical Society
PY - 2024/2/7
Y1 - 2024/2/7
N2 - We present time-resolved X-ray absorption spectra of ionized liquid water and demonstrate that OH radicals, H3O+ ions, and solvated electrons all leave distinct X-ray-spectroscopic signatures. Particularly, this allows us to characterize the electron solvation process through a tool that focuses on the electronic response of oxygen atoms in the immediate vicinity of a solvated electron. Our experimental results, supported by ab initio calculations, confirm the formation of a cavity in which the solvated electron is trapped. We show that the solvation dynamics are governed by the magnitude of the random structural fluctuations present in water. As a consequence, the solvation time is highly sensitive to temperature and to the specific way the electron is injected into water.
AB - We present time-resolved X-ray absorption spectra of ionized liquid water and demonstrate that OH radicals, H3O+ ions, and solvated electrons all leave distinct X-ray-spectroscopic signatures. Particularly, this allows us to characterize the electron solvation process through a tool that focuses on the electronic response of oxygen atoms in the immediate vicinity of a solvated electron. Our experimental results, supported by ab initio calculations, confirm the formation of a cavity in which the solvated electron is trapped. We show that the solvation dynamics are governed by the magnitude of the random structural fluctuations present in water. As a consequence, the solvation time is highly sensitive to temperature and to the specific way the electron is injected into water.
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U2 - 10.1021/jacs.3c11857
DO - 10.1021/jacs.3c11857
M3 - Article
C2 - 38270463
AN - SCOPUS:85184523068
SN - 0002-7863
VL - 146
SP - 3262
EP - 3269
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 5
ER -