Imaging the short-lived hydroxyl-hydronium pair in ionized liquid water

Lin, M.-F.; Singh, N.; Liang, S.; Mo, M.; Nunes, J. P. F.; Ledbetter, K.; Yang, J.; Kozina, M.; Weathersby, S.; Shen, X.; Cordones, A. A.; Wolf, T. J. A.; Pemmaraju, C. D.; Ihme, M.; Wang, X. J.

doi:10.1126/science.abg3091

Imaging the short-lived hydroxyl-hydronium pair in ionized liquid water

Journal Article · Thu Sep 30 00:00:00 EDT 2021 · Science

DOI:https://doi.org/10.1126/science.abg3091· OSTI ID:1807563

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SLAC National Accelerator Lab., Menlo Park, CA (United States)
Stanford Univ., CA (United States)
Univ. of Nebraska, Lincoln, NE (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)

The radiolysis of water is ubiquitous in nature and plays a critical role in numerous biochemical and technological applications. Although the elementary reaction pathways for the ionized water have been studied, the short-lived intermediate complex and structural dynamic response after the proton transfer reaction remain poorly understood. Here, using liquid-phase ultrafast electron diffraction technique to measure the intermolecular O··O and O··H bonds, we captured the short-lived radical-cation complex OH(H₃O⁺) that was formed within 140 femtoseconds through a direct oxygen-oxygen bond contraction and proton transfer, followed by the radical-cation pair dissociation and the subsequent structural relaxation of water within 250 femtoseconds. These measurements provide direct evidence of capturing this metastable radical-cation complex before separation, thereby improving our fundamental understanding of elementary reaction dynamics in ionized liquid water.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); SLAC National Accelerator Laboratory, Menlo Park, CA (United States). Linac Coherent Light Source (LCLS); Stanford Univ., CA (United States)

Sponsoring Organization:: Deutsche Forschungsgemeinschaft (DFG); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; USDOE Office of Science (SC), Fusion Energy Sciences (FES)

Grant/Contract Number:: AC02-05CH11231; AC03-76SF00515; SC0014170; SC0021129

OSTI ID:: 1807563

Alternate ID(s):: OSTI ID: 1993715

Journal Information:: Science, Journal Name: Science Journal Issue: 6563 Vol. 374; ISSN 0036-8075

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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