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$\mathrm{^{117m}Sn}$ and $\mathrm{^{119m}Te}$ Production via Proton Bombardment on Natural Antimony and Implications for Modeling Charged Particle Reactions

T0 review · 5 major / 4 minor · reviewed 2026-08-07 · deepseek-v4-flash

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Pith's one-line read Proton data on antimony sharpen predictions for two medical isotopes

desk verdict New cross sections for medically relevant Sn/Te isotopes up to 200 MeV, but the TALYS spin-cutoff and pre-equilibrium claims lean on BNL points that may carry unquantified secondary-particle contamination. read the letter →

arxiv 2506.13948 v1 pith:HRITU5AN submitted 2025-06-16 nucl-ex

Catherine E. Apgar , Andrew S. Voyles , Jon C. Batchelder , Cathy S. Cutler , Morgan B. Fox , Yun-Hsuan Lee , Dmitri G. Medvedev , Jonathan T. Morrell
show 4 more authors
Ellen M. O'Brien Michael Skulski C. Etienne Vermeulen Lee A. Bernstein
This is my paper · ORCID
classification nucl-ex PACS 25.40.-h25.40.Sc27.60.+j
keywords crosssectionproton-inducedreactionstin-117mtellurium-119mstackedtargetactivationTALYSisomericratioAugertherapy
verification ladder T0 review T1 audit T2 compute T3 formal

The pith

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

The reading

This paper reports new measured cross sections for producing the Auger-therapy isotopes $\mathrm{^{117m}Sn}$ and $\mathrm{^{119m}Te}$ by proton bombardment of natural antimony, covering incident energies up to 200 MeV, together with 22 co-produced reaction channels. It then uses these data to test and adjust the reaction-model code TALYS 1.95, finding that a set of physically motivated parameter changes greatly improves the modeled excitation functions, especially for tellurium isomers. The measurements matter because $\mathrm{^{117m}Sn}$ and the $\mathrm{^{119}Sb}$ daughter of $\mathrm{^{119m}Te}$ are promising for targeted radiotherapy, and better reaction modeling helps plan isotope production and assess radionuclidic impurities.

What carries the argument

The central object is the spin cut-off parameter $\sigma^2$, the width of the angular-momentum distribution in TALYS's phenomenological level-density models, together with the weighted $\chi^2$ goodness-of-fit metric that lets the largest independent channels drive the optimization. The spin cut-off controls how much population flows to high-spin isomers, and reducing it to 0.4 is what repairs the measured $^{119g/m}$Te and $^{121g/m}$Te ground-state-to-isomer ratios. Supporting machinery includes the stacked-target activation method with monitor-foil current and energy characterization by variance minimization, and two channel-weighting schemes (cumulative cross-section and maximum cross-section) that balance the fit between the many low-energy points and the few high-energy points.

What would settle it

Measure the $\mathrm{^{nat}Sb}(p,x)^{119m}\mathrm{Te}$ and $\mathrm{^{nat}Sb}(p,x)^{121m}\mathrm{Te}$ excitation functions using a target arrangement that suppresses secondary neutrons (for example, thin degraders of low-Z material or an active neutron veto), and compare the results with the stacked-target data presented here. If the tellurium cross sections or isomer ratios shift significantly when the neutron fluence is reduced, the fitted TALYS parameters are biased by neutron-induced contributions and the claimed physical adjustments would need to be revisited.

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Extended reading notes

Core claim

The paper establishes that default TALYS 1.95 systematically overpopulates high-spin isomeric states and underpopulates low-spin ground states in proton-induced reactions on antimony near A = 119-123. A parameter set with reduced spin cut-off ($\texttt{rspincut}=0.4$), a shell-effect-aware spin-cut-off model ($\texttt{spincutmodel}=2$), a deeper and narrower imaginary neutron volume potential ($\texttt{w1adjust}(n)=2.5$, $\texttt{w2adjust}(n)=0.6$), analytical pre-equilibrium transition rates ($\texttt{preeqmode}=1$), and adjusted exciton matrix-element parameters ($\texttt{m2constant}=2$, $\texttt{m2limit}=0.8$, $\texttt{m2shift}=1.8$, $\texttt{rpinu}=\texttt{rnupi}=\texttt{rnunu}=1.5$) reduces the reduced-$\chi^2$ for the tellurium channels by factors between 2.16 and 56.78 relative to defaults. The same parameters improve the overall fit to cumulative validation channels, while some antimony and indium channels fit worse, which the paper attributes to co-production of neutron-deficient products by secondary neutrons in the target stacks.

Load-bearing premise

The optimized model parameters are trustworthy only if the tellurium reaction channels that drive the fit are produced purely by protons and are not also fed by secondary neutrons created in the target stack.

Editorial extensions

If this is right

  • The measured $\mathrm{^{nat}Sb}(p,x)$ cross sections provide new experimental benchmarks for $\mathrm{^{117m}Sn}$ and $\mathrm{^{119m}Te}$ production, including contaminant channels such as $\mathrm{^{113}Sn}$, $\mathrm{^{121g,m}Te}$, and $\mathrm{^{123m}Te}$ that affect radionuclidic purity for medical use.
  • If the optimized TALYS parameters are adopted for proton-induced reactions near $A \approx 120$-$130$, predicted isomer-to-ground-state ratios for other tellurium and nearby isotopes should improve substantially.
  • The persistent misfit of neutron-deficient antimony channels is evidence that secondary neutrons generated inside high-energy target stacks measurably contribute to isotope production, so future stacked-target experiments should account for or suppress this neutron field.
  • The finding that stacked-target activation alone cannot unambiguously determine pre-equilibrium parameters implies that outgoing neutron spectral measurements are needed to fix the underlying physics of the model.
  • The cross-section dataset, once submitted to the EXFOR database, will serve as a benchmark for future nuclear reaction model evaluations and for isotope-production simulation codes.

Reading between the lines

Editorial extensions of the paper, not claims the author makes directly.

  • A natural extension of the spin-cut-off result is to test whether $\texttt{rspincut}=0.4$ also improves isomer-ratio predictions for proton-induced reactions on neighboring target elements such as tin and iodine, which would indicate a generic deficiency in default spin distributions rather than a quirk of antimony.
  • Because the optimized parameters were chosen to fit tellurium channels specifically, applying them to other targets may overcorrect for spin effects; a cross-validation against independent isomer-ratio data outside the fitted mass region would test the generality of the adjustment.
  • The paper's secondary-neutron hypothesis could be tested directly by comparing measurements taken with and without high-Z degraders, or by placing neutron detectors around the stack and correlating neutron yield with the excess antimony production.
  • If the decrease in spin cut-off reflects the prolate deformation neglected by the default model, then independent nuclear-structure calculations of level densities for deformed $^{119,121}$Te could corroborate or refute the physical interpretation of the fitted parameter.
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Editorial analysis

A structured set of objections, weighed in public.

Desk editor's note, referee report, and a circularity audit.

Referee Report

5 major / 4 minor

Summary. This paper reports new stacked-target activation measurements of natSb(p,x)117mSn and natSb(p,x)119mTe, together with 22 co-produced residual-product cross sections and monitor-foil cross sections, for proton energies up to 200 MeV from LBNL, LANL, and BNL. The analysis uses a variance-minimization procedure to determine beam current and energy, and the data are compared with TALYS 1.95 calculations. A set of physics-motivated parameter adjustments (rspincut=0.4, spincutmodel=2, w1adjust(n)=2.5, w2adjust(n)=0.6, preeqmode=1, m2constant=2, m2limit=0.8, m2shift=1.8, rpinu=rnupi=rnunu=1.5) is reported to improve reduced chi2 for the dominant Te channels by factors between 2.16 and 56.78, with validation on cumulative and smaller independent channels.

Significance. The experimental dataset is the strongest part of the paper: the activation analysis is detailed, the decay-gamma assignments are documented, monitor foils and variance minimization are used carefully, and the data will be a useful EXFOR entry for medical-isotope production and for testing reaction models. If the modeling improvements were independently confirmed, the spin cut-off and optical-model adjustments would be a valuable step toward better proton-reaction modeling. The modeling conclusions are not yet established at the same level: the parameters are fit to the same data used for the improvement claim, the paper itself acknowledges that pre-equilibrium parameters cannot be uniquely assigned, and the high-energy Te data have not been shown to be free of secondary-particle contamination.

major comments (5)
  1. [Section IV; Table XV] The parameter optimization is driven by the seven Te channels, and the BNL data points at 102-188 MeV are the only high-energy constraints on the pre-equilibrium region. The paper excludes Sb residual data above 100 MeV because of secondary-neutron production (Section IV), but it does not apply an equivalent exclusion or correction to the Te channels. The BNL stack contains thick aluminum degraders (e.g., 4668.98 mg/cm2 in Table XV), which can generate secondary protons; unlike secondary neutrons, secondary protons can produce Te (Z=52) from Sb (Z=51) in downstream foils. No transport calculation, measured secondary fluence, or sensitivity estimate is provided to bound this contribution. If secondary-proton production of Te is not negligible, the fitted rspincut, optical-model, and pre-equilibrium parameters would be biased and the Table VII improvement ratios would not be transferable. Please quantify this contribution or explicitly restrict the high-energy modeling conclusions.
  2. [Section IV D, Eqs. (11)-(13)] There is an inconsistency in the goodness-of-fit definition. Equation (11) includes a factor 1/Nc multiplying the sum over channels, but the weights wc defined in Eqs. (12) and (13) are already normalized so that they sum to unity over channels. With the stated definitions, chi2_tot = (1/Nc) * sum_c chi2_c * wc is not the weighted average implied by the text, and the absolute values in Table V depend on this choice. Although the improvement ratios may be robust to an overall factor, this normalization must be corrected and the quoted values recalculated.
  3. [Section IV D-F; Table VII] The reported improvement factors in Table VII are in-sample: the same 12 independent channels were used both to select the TALYS parameters and to evaluate the fit. The validation channels (Table VIII) are a genuine out-of-sample check within the same dataset, but they were selected after the optimization and are not independent of the experimental conditions. Please present the Table VII ratios as fit diagnostics, add a sensitivity analysis that removes one channel or one energy region at a time, and state explicitly that the parameter set has not been tested on an independent dataset.
  4. [Section III C; Table II] The BNL points above 100 MeV carry the high-energy part of the modeling claim, but the BNL beam-energy and current determination relies on a single monitor reaction, natCu(p,x)58Co, and the paper notes this gives a relatively shallow reduced-chi2 minimum. The Table II energy uncertainties (e.g., +/-2.1 to +/-3.1 MeV) are propagated, but the normalization of these points is weakly constrained. A sensitivity study showing how the fitted parameters and improvement ratios change under alternative stopping-power adjustments, or with the natCu(p,x)56Co data included as a consistency check, would substantially strengthen the high-energy conclusions.
  5. [Section V] The paper's own conclusion that stacked-target measurements 'cannot unambiguously assign the correct pre-equilibrium parameters independently' and that outgoing neutron spectra are needed is an important caveat that is not reflected in the abstract or in the presentation of Table X as the optimized parameter set. The abstract and Section IV F should be revised to present the parameter adjustments as illustrative constraints on TALYS parameters, not as a uniquely determined or globally validated parameter recommendation.
minor comments (4)
  1. [Section V] The sentence 'The decay gamma spectroscopy used in this research is avalable for access' contains a typo; 'avalable' should be 'available'.
  2. [Figure 13] In Figure 13, panel (c) is captioned '123mTe' but the plotted curve and the surrounding text concern natSb(p,x)121(m)Te; relabel the panel.
  3. [Table II] Table II is very dense and some entries, such as the 117Te rows, have large relative uncertainties; a machine-readable supplement with pointwise cross sections and covariance information would improve usability and reproducibility.
  4. [Section III C] The sentence 'The existing experimental data for natCu(p,x)56Co was leveraged as a validation check for the BNL results, but these data were not incorporated into the final calculations' would benefit from a brief description of what the validation check showed, since it is the only consistency check for the BNL normalization.

Circularity Check

0 steps flagged · score 2.0 of 10

No significant circularity: the measured cross sections are independent data and the TALYS parameter optimization is transparently in-sample, with genuine held-out validation.

full rationale

The derivation chain is self-contained. The measured natSb(p,x) cross sections are obtained from activation data via Eqs. (1)-(5), with beam current and energy anchored to external IAEA monitor evaluations and a variance-minimization procedure taken from prior work; the data are not functions of the paper's conclusions. The TALYS modeling section is presented as an explicit optimization rather than as prediction: Section IV D states 'Twelve of the largest measured reaction channels were used to optimize TALYS 1.95 parameters,' and the Table VII improvement ratios (2.16-56.78) are in-sample chi-square values on those same channels, labeled as fit improvements. The abstract itself limits the modeling claim to a 'goodness-of-fit metric established by the largest independent cross section channels and cross-validated with remaining channels.' That cross-validation (Table VIII, improvement ratios 12.39 and 12.04 on nine cumulative channels and three independent channels not used in the fit) is genuine out-of-sample content, so the central modeling result does not reduce by construction to its inputs. The self-citations (Fox et al. [9,10], Morrell et al. [11,14,23], Voyles et al. [13,15]) supply methodology and prior context only; the reported chi-square values and the adopted parameter values (rspincut=0.4, spincutmodel=2, w1adjust=2.5, w2adjust=0.6, preeqmode=1, m2constant=2, m2limit=0.8, m2shift=1.8, rpinu=rnupi=rnunu=1.5) are computed in this paper from its own data, and the spin cut-off finding is independently supported by the external compilation of Rodrigo et al. [29]. Section V's admission that a stacked-target measurement 'cannot unambiguously assign the correct pre-equilibrium parameters independently' is an honest caveat about parameter degeneracy, not circular reasoning. The possible secondary-neutron contamination of the BNL Te points (Sb data excluded above 100 MeV while Te data are retained) is a systematic-uncertainty and correctness risk rather than an input-output circularity, so it does not raise this score.

Assumptions & free parameters 10 free parameters · 5 assumptions · 0 invented entities

The paper fits many TALYS model parameters to the measured data, which are free parameters for the modeling claim, and relies on standard nuclear data and model assumptions for the experimental claim. No new particles or entities are introduced.

free parameters (10)
  • rspincut = 0.4
    Adjusted to improve the 119Te and 121Te isomer-to-ground-state ratios; value chosen by reduced chi2 minimization.
  • spincutmodel = 2
    Selected to improve m/g ratios for Te isotopes by neglecting shell closure due to prolate deformation.
  • w1adjust (n) = 2.5
    Imaginary neutron optical potential volume term adjusted for better fit to Te channels.
  • w2adjust (n) = 0.6
    Imaginary neutron optical potential volume term adjusted together with w1adjust.
  • preeqmode = 1
    Chosen analytical transition rates instead of default numerical rates for best fit.
  • m2constant = 2
    Pre-equilibrium matrix element constant adjusted to improve magnitude of compound peak.
  • m2limit = 0.8
    Pre-equilibrium matrix element asymptotic value adjusted.
  • m2shift = 1.8
    Pre-equilibrium matrix element energy shift adjusted.
  • rpinu, rnupi, rpipi, rnunu = 1.5, 1.5, 1, 1.5
    Residual nucleon-nucleon interaction multipliers in the exciton model, adjusted to improve Te fits; different values needed for Sb/In channels.
  • Areal density adjustment factors per experiment = 102.6%, 101.4%, 104.9%, 98.2%, 103.0%
    Global density multipliers found by variance minimization of monitor reaction currents; up to 4.9% deviation from nominal.
assumptions (5)
  • domain assumption TALYS 1.95 provides an adequate framework for proton-induced reactions (optical model, Hauser-Feshbach, exciton model).
    The entire modeling section relies on TALYS 1.95 as the reaction code; its validity is assumed.
  • domain assumption IAEA 2017 monitor reaction cross sections are accurate.
    Beam current and energy are derived from monitor reactions natCu(p,x), natTi(p,x), natNb(p,x) using IAEA recommended data.
  • domain assumption Anderson-Ziegler stopping powers with a global areal density multiplier within +/-10% describe energy loss in the stacks.
    The variance minimization technique adjusts areal density by a global factor to reduce chi2; this assumes the stopping-power model is correct up to that scaling.
  • domain assumption Natural antimony composition and decay data (half-lives, gamma intensities) from Nuclear Data Sheets are correct.
    Cross sections are computed from gamma intensities and half-lives taken from NDS evaluations.
  • domain assumption TALYS level density models assume a Gaussian spin distribution with adjustable spin cutoff.
    The rspincut parameter modifies this assumed distribution; the Gaussian form is a model assumption.

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Cite this review

Pith. "Pith review of $\mathrm{^{117m}Sn}$ and $\mathrm{^{119m}Te}$ Production via Proton Bombardment on Natural Antimony and Implications for Modeling Charged Particle Reactions." pith.science (2026). https://pith.science/paper/HRITU5AN

@misc{pith2026250613948,
  author       = {Pith},
  title        = {Pith review of: $\mathrm^117mSn$ and $\mathrm^119mTe$ Production via Proton Bombardment on Natural Antimony and Implications for Modeling Charged Particle Reactions},
  year         = {2026},
  howpublished = {\url{https://pith.science/paper/HRITU5AN}},
  note         = {Machine review of arXiv:2506.13948}
}
abstract

$\mathrm{^{117m}Sn}$ and $\mathrm{^{119}Sb}$, the latter of which is produced via a $\mathrm{^{119m}Te}$ generator, are promising radionuclides for the targeted treatment of both osteoarthritis and small mass tumors via Auger therapy. Experiments were conducted at Lawrence Berkeley National Laboratory, Los Alamos National Laboratory, and Brookhaven National Laboratory to measure the $\mathrm{^{nat}Sb}$(p,x)$\mathrm{^{117m}Sn}$ and $\mathrm{^{nat}Sb}$(p,x)$\mathrm{^{119m}Te}$ cross sections for incident proton energies up to 200 MeV. Additional measurements for co-produced isotopes are included as well. In addition to this dataset, this paper investigates improvements for proton-induced reaction modeling capabilities through comparison of these experimental dataset against theoretical models in TALYS 1.95. Parameter adjustments affecting level density, optical model potential, and pre-equilibrium emission were explored, with a goodness-of-fit metric established by the largest independent cross section channels and cross-validated with remaining channels.

Figures

Figures reproduced from arXiv: 2506.13948 by the authors.

Figure 1
Figure 1. FIG. 1. Representative mounted foils prior to irradiation. [PITH_FULL_IMAGE:figures/full_fig_p002_1.png] view at source ↗
Figure 2
Figure 2. FIG. 2. Target boxes for the irradiations. Red arrows indicate [PITH_FULL_IMAGE:figures/full_fig_p003_2.png] view at source ↗
Figure 3
Figure 3. FIG. 3 [PITH_FULL_IMAGE:figures/full_fig_p005_3.png] view at source ↗
Figures from the paper (10 more)
Figure 4
Figure 4. Figure 4: FIG. 4 [PITH_FULL_IMAGE:figures/full_fig_p005_4.png]
Figure 6
Figure 6. Figure 6: FIG. 6. Local minima in [PITH_FULL_IMAGE:figures/full_fig_p006_6.png]
Figure 7
Figure 7. Figure 7: FIG. 7. Energy and current distribution across the stack for [PITH_FULL_IMAGE:figures/full_fig_p006_7.png]
Figure 10
Figure 10. Figure 10: The phenomenological level density models [PITH_FULL_IMAGE:figures/full_fig_p009_10.png]
Figure 9
Figure 9. Figure 9: FIG. 9. Decay schema for [PITH_FULL_IMAGE:figures/full_fig_p010_9.png]
Figure 11
Figure 11. Figure 11: FIG. 11. Reduced [PITH_FULL_IMAGE:figures/full_fig_p010_11.png]
Figure 10
Figure 10. Figure 10: FIG. 10. Default (1.0 - green-dashed curves) vs adjusted (0.4 [PITH_FULL_IMAGE:figures/full_fig_p010_10.png]
Figure 12
Figure 12. Figure 12: FIG. 12. Default vs adjusted TALYS value for [PITH_FULL_IMAGE:figures/full_fig_p011_12.png]
Figure 13
Figure 13. Figure 13: FIG. 13. Experimental datapoints, along with baseline TALYS 1.95 values, TENDL 2019 results, and optimized TALYS 1.95 [PITH_FULL_IMAGE:figures/full_fig_p015_13.png]
Figure 14
Figure 14. Figure 14: FIG. 14. Experimental datapoints, along with baseline TALYS 1.95 values, TENDL 2019 results, and optimized TALYS 1.95 [PITH_FULL_IMAGE:figures/full_fig_p016_14.png]

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    180. (32) 118Te(i) 55.7 (27) 78.4 (18) 107.9 (21) 121.7 (32) 132.6 (16) 126.3 (40) 125.8 (16) 119gTe(i) 26.8 (25) 32.9 (28) 38.2 (41) 49.4 (53) 74.2 (73) 88.3 (84) 99. (11) 119mTe(i) 36.74 (87) 45.41 (76) 59.94 (80) 80.1 (10) 114.6 (13) 140.1 (16) 161.1 (21) 121gTe(i) 12.53 (5...

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