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REVIEW 3 major objections 5 minor 34 references

Polarized Neutrons at ISIS: Recent Developments And Highlights

T0 review · 3 major / 5 minor · reviewed 2026-08-07 · deepseek-v4-flash

Pith's one-line read A compact 380 mm 'Magic Box' magnetostatic cavity gives 3He spin filters a field-gradient relaxation time of at least 421 hours, while X-ray reflectometry shows caesium reacts chemically with a silicon oxide surface at 150°C.

desk verdict The Magic Box section is a solid instrument paper; the caesium chemistry claim is a preliminary observation that needs a better model or more data before it becomes a result. read the letter →

arxiv 2506.05148 v2 pith:5C7VDNCB submitted 2025-06-05 physics.ins-det

classification physics.ins-det
keywords polarizedneutrons3HespinfiltermagnetostaticcavityadiabaticfastpassageelectromagneticsimulationssinglecrystallinesiliconalkalimetalsX-rayreflectometry
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 two engineering results that improve the performance of polarized-neutron experiments that use hyperpolarized $^{3}$He spin filters. First, a redesigned compact magnetostatic cavity, the 'Magic Box,' is only 380 mm long — 43% shorter than the previous design — yet provides a field-gradient relaxation time of at least 421 hours for a $^{3}$He cell, with an optimized simulated value of 615 hours; it also contains a radiofrequency coil for adiabatic fast passage flipping of the $^{3}$He polarization. Second, to understand why alkali-metal coatings improve $^{3}$He wall relaxation times, the authors built a sealed chamber in which caesium is deposited on a single-crystal silicon wafer and then baked, mimicking cell preparation, and read out by X-ray reflectometry through transparent windows. The first results indicate that baking at 150°C produces signs that caesium interacts chemically with the native silicon oxide layer rather than remaining a simple metallic film. If these findings hold, instrument space constraints become much less severe and the long-standing mechanism of alkali-metal coatings becomes experimentally addressable.

What carries the argument

The paper rests on two central devices. The first is the magnetostatic cavity, a mu-metal rectangular box whose static-field homogeneity is tuned by main coils and end-compensation coils; its performance is quantified by the normalized transverse field gradient averaged over the cell volume, $|\nabla_\perp B|/B$, which determines the field-gradient relaxation time $T_1^{\mathrm{grad}}$ through Eq. (3). The optimization used electromagnetic simulations with a parameter sweep over box length, gap width and position, and the current ratio $I_{\mathrm{comp}}/I_{\mathrm{main}}$ between compensation and main coils. The second device is the model-surface chamber: an air-tight aluminium assembly holding a silicon wafer above a caesium reservoir, with windows that allow X-ray or neutron reflectometry of the surface; the reflectometry curves are interpreted with a slab model (substrate, SiO$2$ layer, optional caesium layer). The connecting identity is the relaxation-time sum $1/T_1 = 1/T_1^{\mathrm{dd}} + 1/T_1^{\mathrm{w}} + 1/T_1^{\mathrm{grad}}$, which ties the two projects together — the Magic Box minimizes the field-gradient term, and the surface study targets the wall term.

What would settle it

Map the magnetic field inside the built 380 mm Magic Box and integrate the gradient over the cell volume; if the resulting field-gradient relaxation time falls far below 421 h in the same ambient conditions, the optimization claim fails. For the caesium result, repeat the deposition and baking on fused silica or on an actual cell inner surface: if no reacted layer appears there, the silicon-wafer model does not emulate real $^{3}$He cells.

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Extended reading notes

Core claim

The paper's central claim is that a 380 mm 'Magic Box' magnetostatic cavity can house a $^{3}$He spin filter with a field-gradient contribution to the longitudinal relaxation time of at least 421 h in ambient conditions, derived from a measured total relaxation time of 130 h and a wall relaxation time of 238 h at 0.9 bar; simulations predicted 615 h for the optimized geometry, and even with a 2.1 T high-temperature superconducting magnet at the sample position the field-gradient relaxation time remains 124 h. The second central claim concerns cell-wall chemistry: caesium deposited on a (111) single-crystal silicon wafer and baked at 150°C for one week does not sit as a simple metallic overlayer but interacts chemically with the wafer's silicon dioxide surface, as evidenced by X-ray reflectometry features that the simple slab model (silicon substrate, SiO$2$ layer, caesium layer) fits only poorly, with a $\chi^2$ of 157. The authors present this as the first step of a systematic study of how alkali-metal coatings form and evolve under heat treatment, with the eventual aim of controlling the wall relaxation term in the $^{3}$He polarization decay.

Load-bearing premise

The study assumes that the surface chemistry observed on a single-crystal silicon wafer in the model chamber reproduces what happens inside a real $^{3}$He cell, which is usually made of glass or quartz and coated by distillation; if the wafer does not emulate the real cell surface, the chemical-interaction conclusion does not carry over.

Editorial extensions

If this is right

  • The 380 mm cavity fits instruments where the previous 690 mm cavity was too long, extending polarized-$^{3}$He analysis to small-angle and spin-echo beamlines without sacrificing field homogeneity.
  • With a field-gradient relaxation time of 421 h (and 615 h predicted in the optimized ideal), the magnetic-field contribution to polarization decay becomes small relative to wall relaxation, so further gains in cell lifetime must come from controlling the wall term.
  • The X-ray evidence that caesium reacts with the silicon oxide layer at 150°C implies that the standard baking step may routinely produce a reacted layer rather than a pure alkali-metal film, which changes how the effectiveness of coatings should be assessed.
  • The chamber-and-reflectometry method provides a way to screen substrate materials and alkali metals for their effect on $^{3}$He wall relaxation without cutting open real cells.
  • If the chemical interaction is confirmed, deliberate tuning of baking temperature and time could be used to maximize wall relaxation times and thereby extend the usable lifetime of cells polarized by metastable exchange optical pumping.

Reading between the lines

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

  • The gap between the simulated 615 h and the measured 421 h field-gradient relaxation time suggests the coil winding or the operating current ratio is not yet at its optimum; rewinding the coils and re-tuning currents could close part of that gap, a direction the paper itself hints at.
  • A plausible reading of the 150°C data is that the alkali metal scavenges or chemically transforms the oxide surface, which could be the very mechanism that suppresses $^{3}$He wall relaxation — a hypothesis the authors are working toward but have not yet asserted.
  • If the same chemistry occurs on fused-silica cells, then the baking protocol could be optimized to complete the reaction, and the planned neutron reflectometry could identify the reaction product and any incorporated impurities that X-rays cannot see.
  • A direct test would compare the wall relaxation times of real cells prepared with and without the high-temperature bake against the X-ray-observed layer structure on companion wafers; a correlation would strongly support the model-system approach.
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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

3 major / 5 minor

Summary. The paper reports two R&D projects at ISIS for improving polarized neutron scattering with hyperpolarized 3He spin filters. The first is a compact magnetostatic cavity ("Magic Box") designed via CST simulations, with a chosen length of 380 mm; a preliminary test yields a field-gradient relaxation time of 421 h at a 3He pressure of 0.9 bar, compared to a simulated prediction of 615 h. The second project is a model study of caesium deposition on single-crystal silicon wafers using X-ray reflectometry, aimed at understanding the wall-relaxation contribution in 3He cells. The XRR data, fitted to a Si/SiO2/Cs slab model, suggest that caesium may interact chemically with the silicon oxide layer at 150°C, although the fit quality at that temperature is poor.

Significance. If the Magic Box performance is reproduced in routine use, it offers a practical, compact solution for instruments with tight space constraints, which is a genuine instrumentation advance. The XRR study is among the first systematic attempts to characterize alkali-metal coatings with reflectometry, and even a tentative result could help guide future work on the long-standing problem of wall relaxation in 3He cells. However, the paper's central quantitative and qualitative claims need to be better supported before they can be fully credited.

major comments (3)
  1. [Section 2, Eq. (3) and Section 4] The numbers reported for the transverse field gradient and the corresponding T1_grad are not mutually consistent with the formula as printed. Using Eq. (3) with 1/T1_grad = (3400/p)|∇B⊥/B|^2 and p = 0.9 bar, the simulated gradient of 4.67×10⁻⁴ cm⁻¹ gives T1_grad ≈ 1210 h, not 615 h; similarly, a measured T1_grad of 421 h corresponds to |∇B⊥/B| ≈ 7.9×10⁻⁴ cm⁻¹, not the stated 5.65×10⁻⁴ cm⁻¹. The constant in Eq. (3) appears to be off by about a factor of two (a value near 6700 would reconcile all the numbers). This inconsistency affects the central comparison between the CST prediction and the measured relaxation time and must be corrected.
  2. [Section 3, Table I, and Section 4] The claim that caesium "interacts chemically with the oxide layer" at 150°C is not supported by the presented XRR analysis. The fit at 150°C has χ² = 157, roughly two orders of magnitude larger than at lower temperatures, and the authors themselves state that the slab model becomes inadequate. The extra peak at Q ≈ 0.55 Å⁻¹ is suggestive, but it is not accounted for by a model, so the data could also be explained by surface roughening, island formation, or a changed SiO2 stoichiometry rather than a specific chemical reaction. The 100°C datum (SiO2 thickness 8.3 Å) is an outlier. Unless an alternative model including a reacted layer is provided, or complementary chemical/spectroscopic evidence is presented, the claim should be presented as tentative (e.g., "possibly indicates").
  3. [Section 4, Eq. (2)] The paper states that the field-gradient contribution is "at least 421 h" but does not show how this number is derived from the measured total relaxation time of 130 h and wall relaxation time of 238 h. Reproducing the derivation from Eq. (2) as printed (1/T1_dd = p/80.4) yields a dipole-dipole relaxation time of about 89 h at 0.9 bar, which is shorter than the total measured T1 and makes the calculation impossible. The formula appears to contain a typo (presumably p/804 rather than p/80.4). Please present the explicit calculation with the correct formula and, ideally, with uncertainties.
minor comments (5)
  1. [General] Equations (2) and (3) contain garbled characters in the provided text; please ensure the typeset version is legible and the constants are correct.
  2. [Section 2] The NMR measurement yielding T1 = 130 h and the wall relaxation time of 238 h is reported without experimental details (cell geometry, filling pressure, NMR technique, error bars). This is important for assessing the derived T1_grad value.
  3. [Section 3] The model system uses a single-crystal silicon wafer, whereas real 3He cells are typically made of GE180 glass or quartz. The transferability of the chemical-interaction result to actual cell preparation should be discussed more explicitly, as the authors only note that the chamber "attempt[s] to emulate" the cell conditions.
  4. [Section 3, Fig. 4] The interference peak at Q ≈ 0.25 Å⁻¹ after baking at 100°C and the peak at Q ≈ 0.55 Å⁻¹ after 150°C are mentioned in the text but not interpreted; a more detailed discussion or an annotated figure would help the reader understand their significance.
  5. [References] Reference [24] (D. Jullien, private communication) is the basis for the starting design of the Magic Box; if a citable public reference exists, it would strengthen the reproducibility of the work.

Circularity Check

0 steps flagged · score 1.0 of 10

No significant circularity: the Magic Box field-gradient prediction is a genuine CST-simulation prediction tested against an independent lab measurement (615 h predicted vs 421 h inferred, discrepancy reported), and the Cs-SiO2 interaction claim is a hedged data interpretation rather than a constructed fit.

full rationale

The paper's central quantitative claim is a genuine, falsifiable prediction: the transverse field gradient for the 380 mm Magic Box is obtained from a CST parameter sweep minimizing |grad B_perp/B| (Eq. 3, attributed to Schearer & Walters [16], an external source), which yields T1gr = 615 h at 0.9 bar. This prediction is then compared with laboratory data: total T1 = 130 h with a wall relaxation of 238 h gives an inferred field-gradient component of 421 h, and the paper explicitly reports the shortfall ('the deviation from the predicted 615 h leaves certain room for further improvements'). Reporting a prediction/measurement discrepancy is the opposite of a circular reduction; the simulation inputs (coil geometry, currents, HTS magnet field) contain no information from the measured 130 h value. The caesium-deposition project makes no prediction: a three-slab model (Si substrate / SiO2 / Cs) is fitted to XRR data and the fitted parameters are interpreted. The claim that caesium 'interacts chemically with the oxide layer' (Sec. 4) rests on fitted SiO2-layer changes, an observed extra peak at Q = 0.55 A-1, and the deterioration of fit quality at 150 C (chi2 = 157 in Table I). The text's reasoning loop (the fit degrades 'due to the interaction' and the interaction is then asserted) is explicitly hedged: the authors write the reduced fit quality 'may reflect' the model becoming inadequate and list 'surface inhomogeneities and temperature- and time-dependent chemical transformations' as alternatives. That is an evidence-robustness/correctness concern (the skeptic critique), not a definitional equivalence; no fitted parameter is renamed as a prediction, and no quantity is defined in terms of the quantity it is said to explain. Self-citations [1]-[6] and [9] establish the prior LET polarized-neutron context and are not load-bearing for either new result; the Magic Box starting design is credited to ILL via D. Jullien (private communication) and the end-compensation coils to external work [17] (McIver et al.). No uniqueness theorem is imported from the authors' prior work, no ansatz is smuggled in via citation, and no known empirical result is renamed. Verdict: no significant circularity; the derivation chain for the Magic Box is self-contained and independently tested, and the chemistry claim is a tentative, data-anchored interpretation whose limitations the paper itself discloses.

Assumptions & free parameters 4 free parameters · 4 assumptions · 0 invented entities

The paper relies on standard relaxation formulas and on a model-system assumption that a silicon wafer plus caesium deposition reproduces the cell wall environment. The XRR layer parameters are fitted to data, and the fit quality degrades at high temperatures, so the inferred chemistry at 150°C rests on a less reliable model. No new physical entities are introduced.

free parameters (4)
  • Cs layer thickness = 15.8 to 21.9 Å depending on baking
    Fitted in GenX to XRR data; used to infer layer structure and chemical interaction.
  • Cs layer density = 42 to 57 x 10^4 F.U./Å3
    Fitted to XRR data; deviation from solid Cs density supports non-crystalline or inhomogeneous layer.
  • SiO2 layer thickness = 8.3 to 19.8 Å depending on baking
    Fitted to XRR data; decrease at higher temperatures indicates reaction with Cs.
  • SiO2 layer roughness = 1.6 to 3.5 Å
    Fitted to XRR data; trends inform surface changes during baking.
assumptions (4)
  • domain assumption Formula (3) for field-gradient relaxation time from Schearer and Walters (ref [16]) is valid.
    Used to convert measured field gradients to relaxation times; standard in the field.
  • domain assumption Formula (2) for dipole-dipole relaxation applies with the stated constant.
    Used to subtract the dipole-dipole contribution from the total relaxation rate.
  • domain assumption The silicon wafer chamber faithfully emulates the inner surface of real 3He cells.
    The chamber uses a silicon wafer and caesium reservoir to mimic cell walls; the paper acknowledges this is an attempt to emulate conditions (§3).
  • domain assumption The slab model (Si/SiO2/Cs) adequately describes the XRR data.
    Used to extract layer parameters; the authors note the model becomes inadequate at 150°C (Table I, chi2=157).

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Cite this review

Pith. "Pith review of Polarized Neutrons at ISIS: Recent Developments And Highlights." pith.science (2026). https://pith.science/paper/5C7VDNCB

@misc{pith2026250605148,
  author       = {Pith},
  title        = {Pith review of: Polarized Neutrons at ISIS: Recent Developments And Highlights},
  year         = {2026},
  howpublished = {\url{https://pith.science/paper/5C7VDNCB}},
  note         = {Machine review of arXiv:2506.05148}
}
abstract

We present two recent projects which aim to improve the performance of polarized neutron scattering experiments using hyperpolarized $^{3}He$ spin filters at ISIS. The first is the optimization of a new compact magnetostatic cavity ("Magic Box") to house the $^{3}He$ spin filters based on an existing design. With a length of only 380 mm, it provides a field gradient relaxation time for the $^{3}He$ cell of 421 h in ambient conditions. It also contains a radiofrequency coil for adiabatic fast passage flipping. The second project is dedicated to the improvement of the $^{3}He$ relaxation time inside the spin filter cell. We have developed a chamber which allows for the deposition of alkali metal coatings on the surface of substrates. This emulates the spin filter cell walls, as well as subsequent heat treatment, thus mimicking the preparation of a new spin filter cell. The chamber is air-tight and has transparent windows, so that the structure resulting from the deposition of alkali metal on the surface of the wafer can be studied by X-ray or neutron reflectometry. We plan to continue this work by performing a systematic study at various conditions, which should help to shed light on the long-standing mystery of how alkali metal coatings help to improve relaxation time of $^{3}He$ cells. The first results are discussed in the text.

Figures

Figures reproduced from arXiv: 2506.05148 by the authors.

Figure 1
Figure 1. a) General view of the Magic Box with an Si-windowed 3He spin filter cell inside. White arrows show the direction of the magnetic field. b) Side view showing sections for main coils (middle) and compensation coils (ends) which run at a higher current. All dimensions are shown for the final optimized configuration (see text) [PITH_FULL_IMAGE:figures/full_fig_p004_1.png] view at source ↗
Figure 2
Figure 2. Results of the CST simulations. a) Pink dotted diamonds (right axis) - optimal current ratio Icomp/Imain in the static coils as a function of the box length (gap width and position are set to their optimized numbers for each particular length value). Blue up-triangles (left axis) - normalized volume￾averaged transverse magnetic field gradient taken within a volume of 140 × 140 × 100 mm3 (width × height × length) at … view at source ↗
Figure 3
Figure 3. The chamber for the reflectometry studies of caesium deposition on the silicon wafer. a) Basement with mounted Si wafer. b) Cut view of the assembly with top section for caesium deposition and baking procedure. c) Cut view of the assembly with top section for X-ray reflectometry measurements. d) Photo of the assembly with top part for X-ray reflectometry measurements. Caps screwed on the top and the left side cover … view at source ↗
Figures from the paper (1 more)
Figure 4
Figure 4. Figure 4: XRR profiles measured on wafer without caesium, coated by caesium without additional baking, and with heating at 50⁰C during 12h, 100⁰C during one week and 150⁰C for one week. Symbols – experiment, lines – fitting (see text). Table I. Fitting results for XRR profiles. …

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Reviewed August 7, 2026 · model on record in the stance chip above.