Bragg-Peak Luminescence of Liquid Water under High-LET Carbon-Ion Irradiation: Constraints from Nitrate and Dissolved-Gas Perturbations

Abstract The origin of the faint luminescence emitted by liquid water below the Cherenkov threshold─whether it is mediated by chemically evolving radiolytic intermediates or originates from a prompt physical excitation of the medium─has remained unresolved since its first observation by Belcher in 1953. We examine the Bragg-peak luminescence of pure water under 290 MeV u–1 12C-ion irradiation using two independent perturbations: NaNO3 addition (0–1000 mM) and replacement of dissolved air with N2. At the Bragg peak, where the carbon-ion velocity is far below the Cherenkov threshold and even the most energetic δ-rays cannot produce Cherenkov radiation, neither perturbation produces a large suppression of the observed luminescence; the concentration-dependent Bragg-peak position shift is quantitatively accounted for by the increased solution density. At 1 M NaNO3, the mean nitrate spacing is comparable to the characteristic track-core dimension, so nitrate scavenging can compete directly with precursor relaxation and intratrack reactions on subpicosecond time scales rather than being excluded spatially. The weak nitrate dependence therefore constrains a dominant contribution from longer-lived, readily scavenged radiolytic intermediates but does not exclude an ultrafast chemical pathway. Independently, the observations are compatible with a dielectric energy-loss framework in which Im[−1/ε(ω)] governs electronic excitation of the medium. The ∼8 eV feature provides a plausible, but nonunique, microscopic doorway to the emitting manifold, while contributions from higher-energy excitations followed by relaxation cascades cannot be excluded.

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Publication Details

Journal
The Journal of Physical Chemistry B
Published
2026-10-26
DOI
https://doi.org/10.1021/acs.jpcb.6c05234
Primary Topic
Radiation Effects and Dosimetry
Type
article
Field-Weighted Citation Impact
0.00

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article

Bragg-Peak Luminescence of Liquid Water under High-LET Carbon-Ion Irradiation: Constraints from Nitrate and Dissolved-Gas Perturbations

Naoki Kawachi, Makoto Sakai, Takuya Yabe, Kazuyuki Enomoto et al.
The Journal of Physical Chemistry B
Radiation Effects and Dosimetry
article

Bragg-Peak Luminescence of Liquid Water under High-LET Carbon-Ion Irradiation: Constraints from Nitrate and Dissolved-Gas Perturbations

Naoki Kawachi, Makoto Sakai, Takuya Yabe, Kazuyuki Enomoto, Mutsumi Tashiro, Yuto Nagao, Mitsutaka Yamaguchi, Michiko Tsuda
article en

Abstract

Abstract The origin of the faint luminescence emitted by liquid water below the Cherenkov threshold─whether it is mediated by chemically evolving radiolytic intermediates or originates from a prompt physical excitation of the medium─has remained unresolved since its first observation by Belcher in 1953. We examine the Bragg-peak luminescence of pure water under 290 MeV u–1 12C-ion irradiation using two independent perturbations: NaNO3 addition (0–1000 mM) and replacement of dissolved air with N2. At the Bragg peak, where the carbon-ion velocity is far below the Cherenkov threshold and even the most energetic δ-rays cannot produce Cherenkov radiation, neither perturbation produces a large suppression of the observed luminescence; the concentration-dependent Bragg-peak position shift is quantitatively accounted for by the increased solution density. At 1 M NaNO3, the mean nitrate spacing is comparable to the characteristic track-core dimension, so nitrate scavenging can compete directly with precursor relaxation and intratrack reactions on subpicosecond time scales rather than being excluded spatially. The weak nitrate dependence therefore constrains a dominant contribution from longer-lived, readily scavenged radiolytic intermediates but does not exclude an ultrafast chemical pathway. Independently, the observations are compatible with a dielectric energy-loss framework in which Im[−1/ε(ω)] governs electronic excitation of the medium. The ∼8 eV feature provides a plausible, but nonunique, microscopic doorway to the emitting manifold, while contributions from higher-energy excitations followed by relaxation cascades cannot be excluded.

The Journal of Physical Chemistry B
Japan Society for the Promotion of Science (JP), National Institutes for Quantum Science and Technology (JP), Gunma University Hospital (JP), Gunma University Heavy Ion Medical Center (JP)
Terumo Life Science Foundation, Heavy Ion Medical Center, Gunma University, Japan Society for the Promotion of Science, Japan Science and Technology Agency
Openalex Percentile: Top 16%
Radiation Effects and Dosimetry
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