Please use this identifier to cite or link to this item: https://hdl.handle.net/10356/163520
Title: Observation of a transient intermediate in the ultrafast relaxation dynamics of the excess electron in strong-field-ionized liquid water
Authors: Low, Pei Jiang
Chu, Weibin
Nie, Zhaogang
Muhammad Shafiq Mohd Yusof
Prezhdo, Oleg V.
Loh, Zhi-Heng
Keywords: Science::Chemistry
Issue Date: 2022
Source: Low, P. J., Chu, W., Nie, Z., Muhammad Shafiq Mohd Yusof, Prezhdo, O. V. & Loh, Z. (2022). Observation of a transient intermediate in the ultrafast relaxation dynamics of the excess electron in strong-field-ionized liquid water. Nature Communications, 13(1), 7300-. https://dx.doi.org/10.1038/s41467-022-34981-4
Project: MOE-T2EP50221-0004
RG1/20
RG105/17
MOE2014-T2- 2-052
Journal: Nature Communications
Abstract: A unified picture of the electronic relaxation dynamics of ionized liquid water has remained elusive despite decades of study. Here, we employ sub-two-cycle visible to short-wave infrared pump-probe spectroscopy and ab initio nonadiabatic molecular dynamics simulations to reveal that the excess electron injected into the conduction band (CB) of ionized liquid water undergoes sequential relaxation to the hydrated electron s ground state via an intermediate state, identified as the elusive p excited state. The measured CB and p-electron lifetimes are 0.26 ± 0.02 ps and 62 ± 10 fs, respectively. Ab initio quantum dynamics yield similar lifetimes and furthermore reveal vibrational modes that participate in the different stages of electronic relaxation, with initial relaxation within the dense CB manifold coupled to hindered translational motions whereas subsequent p-to-s relaxation facilitated by librational and even intramolecular bending modes of water. Finally, energetic considerations suggest that a hitherto unobserved trap state resides ~0.3-eV below the CB edge of liquid water. Our results provide a detailed atomistic picture of the electronic relaxation dynamics of ionized liquid water with unprecedented time resolution.
URI: https://hdl.handle.net/10356/163520
ISSN: 2041-1723
DOI: 10.1038/s41467-022-34981-4
DOI (Related Dataset): 10.21979/N9/FVLTAJ
Schools: School of Physical and Mathematical Sciences 
School of Chemistry, Chemical Engineering and Biotechnology 
Rights: © 2022 The Author(s). This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/ licenses/by/4.0/.
Fulltext Permission: open
Fulltext Availability: With Fulltext
Appears in Collections:CCEB Journal Articles
SPMS Journal Articles

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