Temperature dependence of the Fricke dosimeter and spur expansion time in the low-LET high-temperature radiolysis of water up to 350 °C: a Monte-Carlo simulation study
Bibliographic record
Abstract
Monte-Carlo simulations of the radiolysis of the ferrous sulfate (Fricke) dosimeter with low-linear energy transfer (LET) radiation (such as (60)Co γ-rays or fast electrons) have been performed as a function of temperature from 25 to 350 °C. The predicted yields of Fe(2+) oxidation are found to increase with increasing temperature up to ∼100-150 °C, and then tend to remain essentially constant at higher temperatures, in very good agreement with experiment. By using a simple method based on the direct application of the stoichiometric relationship that exists between the ferric ion yields so obtained G(Fe(3+)) and the sum {3 [g(e(-)(aq) + H˙) + g(HO(2)˙)] + g(˙OH) + 2 g(H(2)O(2))}, where g(e(-)(aq) + H˙), g(HO(2)˙), g(˙OH), and g(H(2)O(2)) are the primary radical and molecular yields of the radiolysis of deaerated 0.4 M H(2)SO(4) aqueous solutions, the lifetime (τ(s)) of the spur and its temperature dependence have been determined. In the spirit of the spur model, τ(s) is an important indicator for overlapping spurs, giving the time required for the changeover from nonhomogeneous spur kinetics to homogeneous kinetics in the bulk solution. The calculations show that τ(s) decreases by about an order of magnitude over the 25-350 °C temperature range, going from ∼4.2 × 10(-7) s at 25 °C to ∼5.7 × 10(-8) s at 350 °C. This decrease in τ(s) with increasing temperature mainly originates from the quicker diffusion of the individual species involved. Moreover, the observed dependence of G(Fe(3+)) on temperature largely reflects the influence of temperature upon the primary free-radical product yields of the radiolysis, especially the yield of H˙ atoms. Above ∼200-250 °C, the more and more pronounced intervention of the reaction of H˙ atoms with water also contributes to the variation of G(Fe(3+)), which may decrease or increase slightly, depending on the choice made for the rate constant of this reaction. All calculations reported herein use the radiolysis database of Elliot (Atomic Energy of Canada Limited) and Bartels (University of Notre Dame) that contains all the best currently available information on the rate constants, reaction mechanisms, and g-values in the range 20 to 350 °C.
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How this classification was reachedexpand
Full frame distilled prediction
Teacher imitationNot calibrated prevalence, not ground truth. Human validation pending. Learned from the 10,348 direct Codex labels and 10,348 direct Gemma labels. Candidate is the union of thresholded teacher heads; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels or direct frontier model labels.
Codex and Gemma teacher scores by category
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.000 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.000 | 0.000 |
Machine scores (provisional)
The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.
Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from itClassification
machine, unvalidatedMachine predicted; a candidate call from one teacher head, not a consensus.
How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".