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Physical Sciences › Chemistry › Inorganic Chemistry
Observation of the fastest chemical processes in the radiolysis of water
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Conflicts of Interest
Identified Weaknesses
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Paper Summary
Paperzilla title
Zapping Water with X-rays: Catching H2O+ in the Act!
This study reveals the ultrafast dynamics of the H2O+ radical cation and OH radical formation in ionized liquid water using femtosecond x-ray pulses. The H2O+ cation is found to decay within 46 fs via proton transfer, leading to the formation of OH radical, which undergoes subsequent vibrational cooling and geminate recombination with a hydrated electron on longer timescales.
Possible Conflicts of Interest
None identified
Identified Weaknesses
Limited QM cluster size
The limited QM cluster size in the theoretical calculations introduces an artifact of linear drift in the spectrum peak position, which needs to be addressed for accurate interpretation of the dynamics.
Strong-field ionization
The study relies on strong-field ionization, which may introduce complexities in the interpretation of the data due to potential plasma dynamics.
Limited time resolution
The experimental time resolution of ~110 fs limits the ability to capture the fastest dynamics with high precision.
Low ionization fraction
The relatively low ionization fraction (~0.8%) makes it challenging to isolate spectral signatures of H2O+ and hot OH radicals.
Unclear origin of pre-edge absorption increase
The origin of the observed absorption increase at the pre-edge region requires further investigation with a thinner liquid microjet target.
Rating Explanation
This study provides valuable insights into the ultrafast dynamics of ionized liquid water using a novel experimental approach. The combination of ultrafast x-ray spectroscopy with strong-field ionization enables the detection of short-lived species like H2O+ and OH radical. Despite some limitations in time resolution and the complexity introduced by strong-field ionization, the findings are supported by theoretical calculations and significantly advance the understanding of water radiolysis. The limitations are acknowledged and addressed, and suggestions for future research are provided.
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Original Title:
Observation of the fastest chemical processes in the radiolysis of water
File Name:
LCLS_Water_paper_combined_revised3.pdf
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File Size:
1.97 MB
Uploaded:
July 14, 2025 at 10:41 AM
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