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arxiv: 2602.19996 · v1 · submitted 2026-02-23 · 🌌 astro-ph.GA

Simulation of proton radiolysis of H2O and O2 ices with the Nautilus code

Tian-Yu Tu , Valentine Wakelam , Jean-Christophe Loison , Marin Chabot , Emmanuel Dartois , Yang Chen This is my paper

Pith reviewed 2026-05-15 20:29 UTC · model grok-4.3

classification 🌌 astro-ph.GA
keywords radiolysisH2O iceO2 icecosmic raysastrochemistrysuprathermal speciesG-valuesNautilus code
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The pith

By adding radiolysis to the Nautilus code and adjusting a few chemical parameters, the model reproduces the steady-state abundance ratios of H2O2 over H2O and O3 over O2 seen in laboratory proton irradiation experiments on water and oxygen

A machine-rendered reading of the paper's core claim, the machinery that carries it, and where it could break.

This paper incorporates cosmic-ray radiolysis into the Nautilus astrochemical code to simulate proton bombardment of H2O and O2 ices. It tests the effects of removing reaction-diffusion competition, disabling non-diffusive reactions, and changing desorption energies of suprathermal atoms and molecules. With targeted tweaks to G-values and desorption energies, the updated model matches the experimental steady-state abundance ratios across the full range of cosmic-ray fluxes used in the lab. The same changes still overpredict the total fluence required to reach steady state and overestimate the net loss of H2O. The work underscores that better data on ion chemistry inside the ice bulk and on branching ratios would reduce reliance on such parameter adjustments.

Core claim

The model, with a few adjustments of the chemistry, can reproduce the steady-state [H2O2]/[H2O] and [O3]/[O2]_0 abundance ratios in the H2O and O2 radiolysis experiments at any CR flux in the experiments. Reducing the G-values of H2O radiolysis leads to simulated H2O destruction rates closer to the experiments, while the effect of reaction-diffusion competition is significant at low ionization rates and non-diffusive chemistry matters only at 16 K.

What carries the argument

The radiolysis module added to Nautilus, which tracks suprathermal H, O, OH and O3 species together with adjusted G-values for water dissociation yields.

Load-bearing premise

Adjustments to G-values for H2O radiolysis and desorption energies of suprathermal species can compensate for incomplete knowledge of ion chemistry, activation barriers, and branching ratios inside the ice.

What would settle it

A laboratory measurement of the exact fluence at which [H2O2]/[H2O] reaches steady state under proton irradiation that differs from the fluence predicted by the adjusted Nautilus model.

Figures

Figures reproduced from arXiv: 2602.19996 by Emmanuel Dartois, Jean-Christophe Loison, Marin Chabot, Tian-Yu Tu, Valentine Wakelam, Yang Chen.

Figure 1
Figure 1. Figure 1: Simulation results of abundance ratios [H2O2]/[H2O] (black lines), [H2]/[H2O] (orange lines), and [O2]/[H2O] (blue lines) with our model (model A) at 16 K (solid lines) and 77 K (dashed lines). The gray shaded and line filled regions show the experimental results of [H2O2]/[H2O] by Gomis et al. (2004a) at 16 and 77 K, respectively, with an assumed uncertainty of a factor of 3. O2 ice) with an uncertainty o… view at source ↗
Figure 3
Figure 3. Figure 3: Same as [PITH_FULL_IMAGE:figures/full_fig_p007_3.png] view at source ↗
Figure 6
Figure 6. Figure 6: Same as [PITH_FULL_IMAGE:figures/full_fig_p008_6.png] view at source ↗
Figure 5
Figure 5. Figure 5: Simulation results of the steady-state [O3]/[O2]0 abundance ratio in model A as a function of the CR ionization rate. 3.4. Sensitivity to the CR ionization rates Most experiments study the H2O radiolysis effect with a CR flux of ∼ 109–1012 ions s−1 cm−2 (Moore & Hudson 2000; Gomis et al. 2004b,a; Mejía et al. 2022), corresponding to the CR ionization rates of ∼ 10−9–10−6 s −1 , due to the limitation of the… view at source ↗
Figure 7
Figure 7. Figure 7: Same as [PITH_FULL_IMAGE:figures/full_fig_p009_7.png] view at source ↗
Figure 8
Figure 8. Figure 8: Logarithm of the ratio between the simulated [H2O2]/[H2O] after lowering the desorption energy of a specific suprathermal species by an order of magnitude and the simulated [H2O2]/[H2O] in model A. The results at 16 K are shown in blue and those at 77 K are shown in orange. The vertical grey line shows the positions where [H2O2]/[H2O] is not changed after changing the desorption energy. Note that the ratio… view at source ↗
read the original abstract

The radiolysis effect of cosmic rays (CRs) plays an important role in the chemistry in molecular clouds. CRs can dissociate the molecules on dust grains, producing reactive suprathermal species and radicals which facilitate the formation of large molecules. We add the radiolysis process and some relevant reactions into the Nautilus astrochemical code. By adjusting some parameters, we investigate the sensitivity of the simulation results of the H2O ice on the removal of reaction-diffusion competition, the removal of non-diffusive chemistry, and the desorption energies of the suprathermal species. We find the model, with a few adjustments of the chemistry, can reproduce the steady-state [H2O2]/[H2O] and [O3]/[O2]_0 abundance ratios in the H2O and O2 radiolysis experiments at any CR flux in the experiments. These adjustments in the model do not fully reproduce the fluence required to reach the steady state. It tends also to overestimate the destruction of H2O as measured in H2O radiolysis experiments. We show that reducing the G-values of H2O radiolysis, which implies an increase in the efficiency of immediate reformation of water locally after ion impact, leads to simulated H2O destruction rates closer to the experiments. The effect of reaction-diffusion competition on the simulation results of H2O ice is significant at $\zeta \lesssim 10^{-14}\ \rm s^{-1}$. The non-diffusive chemistry affects the simulation results at 16 K but not 77K, while the results are sensitive to the desorption energies of suprathermal H, O, O3 and OH at 77 K. Our results show that the steady-state [H2O2]/[H2O] and [O3]/[O2]_0 in experiments can be reproduced by fine-tuning the chemical model, but still call for more constraints on the intermediate pathways in the radiolysis processes, especially the ion chemistry in the ice bulk, as well as activation barriers and branching ratios of the reactions in the network.

Editorial analysis

A structured set of objections, weighed in public.

Desk editor's note, referee report, simulated authors' rebuttal, and a circularity audit. Tearing a paper down is the easy half of reading it; the pith above is the substance, this is the friction.

Referee Report

3 major / 2 minor

Summary. The manuscript adds proton radiolysis and related reactions to the Nautilus astrochemical code to model H2O and O2 ices. After adjusting G-values for H2O radiolysis and desorption energies of suprathermal species (H, O, O3, OH), the simulations reproduce the steady-state [H2O2]/[H2O] and [O3]/[O2]_0 ratios observed in laboratory experiments across the tested CR fluxes. The same adjustments, however, overestimate H2O destruction and require higher fluence to reach steady state than seen experimentally. Sensitivity tests examine the effects of removing reaction-diffusion competition, non-diffusive chemistry, and varying desorption energies at 16 K and 77 K.

Significance. If the parameter adjustments can be shown to have independent physical justification rather than being tuned solely to the validation data, the work would supply a practical way to include radiolysis-driven chemistry in grain-surface models of molecular clouds. The reported sensitivities to reaction-diffusion competition at low fluxes and to non-diffusive processes at 16 K are useful for guiding future model development, though the fluence mismatch indicates that key ion-chemistry and branching-ratio uncertainties remain unresolved.

major comments (3)
  1. [Abstract] Abstract: the claim that 'a few adjustments of the chemistry' suffice to reproduce the steady-state ratios at any experimental CR flux is load-bearing for the central result, yet the same adjustments are reported to overestimate H2O loss and fail to match the experimental fluence to steady state; this indicates that the tuned effective rates do not correctly capture the net production/destruction kinetics.
  2. [Abstract] Abstract and results: G-values for H2O radiolysis and desorption energies of suprathermal species are adjusted to match the same laboratory abundance ratios used for validation, so the reproduction of steady-state ratios is achieved by construction rather than by independent first-principles prediction; the manuscript should quantify how much of the agreement survives when these parameters are instead taken from independent literature values.
  3. [Results] Results: the statement that reducing G-values brings simulated H2O destruction rates closer to experiment is presented without showing the quantitative change in the full network or demonstrating consistency with known primary radiolysis yields; this adjustment directly affects the reported ratios and must be justified with explicit before/after comparisons.
minor comments (2)
  1. [Abstract] Abstract: the subscript notation [O3]/[O2]_0 should be defined explicitly on first use as the ratio relative to initial O2 abundance.
  2. [Methods] Methods: the implementation of the radiolysis process (how suprathermal species are generated and how their reactions are added to the Nautilus network) is described only at a high level; a table listing the new reactions and their rate coefficients would improve reproducibility.

Simulated Author's Rebuttal

3 responses · 0 unresolved

We thank the referee for the constructive and detailed comments, which have helped us improve the clarity and balance of the manuscript. We address each major comment below and have revised the text, abstract, and added new quantitative material to better reflect the scope and limitations of the parameter adjustments.

read point-by-point responses

  1. Referee: [Abstract] the claim that 'a few adjustments of the chemistry' suffice to reproduce the steady-state ratios at any experimental CR flux is load-bearing for the central result, yet the same adjustments are reported to overestimate H2O loss and fail to match the experimental fluence to steady state; this indicates that the tuned effective rates do not correctly capture the net production/destruction kinetics.

    Authors: We agree that the original abstract phrasing understated the kinetic limitations. The tuned parameters do reproduce the observed steady-state [H2O2]/[H2O] and [O3]/[O2] ratios across the experimental fluxes, but the model still requires higher fluence to reach steady state and overestimates net H2O destruction, showing that the effective rates are approximations rather than a complete kinetic description. We have revised the abstract to explicitly note these discrepancies and their implications for net production/destruction kinetics while preserving the factual statement about the ratios achieved. revision: yes

  2. Referee: [Abstract] G-values for H2O radiolysis and desorption energies of suprathermal species are adjusted to match the same laboratory abundance ratios used for validation, so the reproduction of steady-state ratios is achieved by construction rather than by independent first-principles prediction; the manuscript should quantify how much of the agreement survives when these parameters are instead taken from independent literature values.

    Authors: This observation is correct: the close reproduction of the ratios relies on tuning to the validation data. To address the request for quantification, we have added a new subsection in the Results section that reruns the full network using untuned G-values and desorption energies drawn from independent radiation-chemistry literature. The new material includes a table showing that literature values still recover the ratios to within a factor of 2–3 (order-of-magnitude agreement) but do not achieve the near-exact match obtained after tuning. This demonstrates both the utility of the core network and the remaining need for better constraints on ion chemistry and branching ratios, as already stated in the conclusions. revision: yes

  3. Referee: [Results] the statement that reducing G-values brings simulated H2O destruction rates closer to experiment is presented without showing the quantitative change in the full network or demonstrating consistency with known primary radiolysis yields; this adjustment directly affects the reported ratios and must be justified with explicit before/after comparisons.

    Authors: We accept that the original manuscript lacked explicit before/after quantification. We have added a new figure showing the time-dependent H2O abundance for the original and reduced G-values, together with a table that reports the percentage reduction in destruction rate and the consequent change in the steady-state [H2O2]/[H2O] ratio. The reduction is justified by reference to primary radiolysis yields in the literature, noting that effective net G-values in solid ice are lower than gas-phase or bulk values because of local cage recombination and immediate reformation; this is consistent with experimental radiation-chemistry studies on H2O ice. revision: yes

Circularity Check

1 steps flagged

Steady-state ratios reproduced after fitting G-values and desorption energies to experimental data

specific steps
  1. fitted input called prediction [Abstract]
    "We find the model, with a few adjustments of the chemistry, can reproduce the steady-state [H2O2]/[H2O] and [O3]/[O2]_0 abundance ratios in the H2O and O2 radiolysis experiments at any CR flux in the experiments."

    The adjustments to G-values and suprathermal desorption energies are chosen to fit the same experimental steady-state ratios that are then reported as reproduced. The match is therefore a direct consequence of the parameter tuning rather than an independent test of the underlying kinetics.

full rationale

The paper tunes G-values for H2O radiolysis and desorption energies of suprathermal species specifically to match the laboratory steady-state [H2O2]/[H2O] and [O3]/[O2] ratios across CR fluxes. This match is then presented as model reproduction. The central claim therefore reduces to the fitted inputs by construction (pattern 2). The manuscript is transparent that fluence to steady state and H2O destruction rates remain discrepant, so the circularity is partial rather than total. No self-citation load-bearing or self-definitional steps appear in the provided text.

Axiom & Free-Parameter Ledger

2 free parameters · 2 axioms · 0 invented entities

The central claim rests on several free parameters tuned to experimental data together with standard domain assumptions from grain-surface astrochemistry.

free parameters (2)
  • G-values of H2O radiolysis = reduced
    Reduced from standard values to increase immediate water reformation efficiency after ion impact and better match observed H2O destruction rates.
  • desorption energies of suprathermal H, O, O3, OH
    Tested for sensitivity; values affect results especially at 77 K.
axioms (2)
  • domain assumption Standard Nautilus treatment of grain-surface reaction-diffusion competition and non-diffusive chemistry.
    Base framework to which radiolysis is added; sensitivity tested by removal.
  • domain assumption Laboratory radiolysis experiments supply accurate steady-state abundance ratios as validation benchmarks.
    Used to judge model performance for H2O and O2 ices.

pith-pipeline@v0.9.0 · 5705 in / 1459 out tokens · 50137 ms · 2026-05-15T20:29:11.706735+00:00 · methodology

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