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arxiv: 2605.31395 · v1 · pith:XBO3247Anew · submitted 2026-05-29 · ❄️ cond-mat.mtrl-sci

Direct Observation of Chemical Short-Range Order in CoCrNi Alloy Using Neutron Diffraction

Vin\'icius P. Bacurau , Camilo Salvador , Guilherme C. Stumpfa , Angelo F. Andreolli , Caroline B. Stocoa , Eric M. Mazzer , Lewis Owen , Yifan Cao
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Rodrigo Freitas Daniel Miracle Francisco G. Coury
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classification ❄️ cond-mat.mtrl-sci
keywords chemical short-range orderCoCrNi alloyneutron diffractiondiffuse scatteringmulti-principal element alloyssmall-angle neutron scatteringatomistic simulationsaging treatment
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The pith

Neutron diffraction detects chemical short-range order in equiatomic CoCrNi alloy

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

The paper establishes through direct measurement that chemical short-range order forms in the CoCrNi alloy and appears as a diffuse scattering peak at Q equals 1.85 inverse angstroms. This peak grows in intensity when samples undergo aging at 748 K for 100 or 240 hours or at 798 K for 24 hours, conditions that favor ordering. The gas-atomized starting material already holds roughly 70 percent of the ordering level reached after the longest aging treatment. Atomistic simulations match the peak position, and small-angle neutron scattering shows the order takes the form of thin Ni-rich disks roughly 11 angstroms across. A sympathetic reader would care because this local atomic arrangement is presented as an intrinsic, stable feature of the alloy that persists after rapid solidification and can be tuned by heat treatment.

Core claim

This study demonstrates the presence of chemical short-range order in CoCrNi through a distinct diffuse peak in neutron diffraction at Q = 1.85 Å^{-1}. The intensity of this peak increases with aging treatments that favor ordering, such as 240 hours at 748 K. Atomistic simulations reproduce the peak position, and small-angle neutron scattering reveals Ni-rich disk-shaped domains consistent with nanoscale order. The gas-atomized sample retains about 70% of the ordering seen in the most aged sample, indicating that CSRO is an intrinsic feature of the alloy.

What carries the argument

The diffuse neutron scattering peak at Q = 1.85 Å^{-1} whose integrated intensity changes with thermal aging, taken together with matching atomistic simulations and small-angle neutron scattering that identifies Ni-rich domains of radius about 11 Å and thickness about 1 Å.

Load-bearing premise

The diffuse peak at Q = 1.85 inverse angstroms and its intensity changes with aging are produced by chemical short-range order rather than by other scattering sources, defects, or experimental artifacts.

What would settle it

A measurement showing that the diffuse peak intensity remains unchanged after the described aging treatments, or that atomistic simulations fail to place a peak at the observed Q value.

read the original abstract

This study provides experimental evidence of chemical short-range order (CSRO) in the equiatomic CoCrNi alloy, identified through neutron diffraction. The phenomenon manifests as a distinct diffuse peak at Q = 1.85 A-1, the intensity increases under thermodynamically favorable conditions for CSRO development such as prolonged aging (100 h and 240 h) at 748 K or shorter aging (24 h) at slightly higher temperature (798 K). The degree of ordering was measured by integrating the diffuse scattering intensity, revealing that the gas-atomized sample, i.e. the sample with the least amount of CSRO, still displays approximately 70% of the CSRO level observed in the sample subsequently aged for 240 h at 748 K, i.e. the sample with the highest amount of CSRO produced in this study. Predictive atomistic simulations reproduced both the presence and position of the diffuse peak, while two-dimensional fast Fourier transform (FT-2D) analyses indicated that reflections at (1 1/2 0) within the <001> zone axis originate from some structural projections associated with like D022, Pt2Mo and D1a motifs. Complementary small-angle neutron scattering (SANS) measurements identified Ni-rich, disk-shaped domains with radii of approximately 11 A and thicknesses of about 1 A, consistent with nanoscale CSRO characteristic length scale. These findings demonstrate that CSRO is an intrinsic and energetically favorable feature of the CoCrNi system, remaining stable even under rapid solidification and further enhanced by low-temperature aging. Combined use of neutron diffraction and atomistic modeling provides a framework for probing local ordering phenomena in multi-principal element alloys (MPEAs).

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

2 major / 2 minor

Summary. The manuscript claims direct experimental evidence for intrinsic chemical short-range order (CSRO) in equiatomic CoCrNi via neutron diffraction, manifested as a diffuse peak at Q = 1.85 Å^{-1} whose intensity increases with aging at 748–798 K. The gas-atomized sample retains ~70% of the maximum CSRO level (quantified by integrated diffuse intensity) seen after 240 h aging. Atomistic simulations reproduce the peak position and (1 1/2 0)-type reflections linked to D0_{22}, Pt_{2}Mo and D1ₐ motifs via FT-2D; complementary SANS identifies ~11 Å radius, ~1 Å thick Ni-rich disk domains.

Significance. If the nuclear origin of the diffuse intensity is confirmed, the work supplies multi-technique evidence that CSRO is an energetically favorable, intrinsic feature of CoCrNi even after rapid solidification. The combination of aging-dependent diffraction, non-magnetic atomistic simulations that match the observed Q, and SANS length-scale data offers a useful framework for local-order studies in MPEAs.

major comments (2)
  1. [Neutron diffraction results and discussion of diffuse-peak origin] The central attribution of the Q = 1.85 Å^{-1} diffuse peak and its aging dependence to nuclear (chemical) scattering from CSRO is load-bearing yet not fully secured. Neutron diffraction records the sum of nuclear and magnetic structure factors; the manuscript reports neither polarized-neutron spin-flip/non-spin-flip separation nor temperature-dependent measurements above any putative magnetic transition to isolate the nuclear component. While the low-temperature aging trend and non-magnetic simulations are consistent with a chemical origin, they do not quantitatively bound a possible magnetic short-range-order contribution to the integrated intensity used for the 70 % quantification.
  2. [Quantification of ordering degree] The 70 % CSRO retention claim for the gas-atomized sample (relative to the 240 h / 748 K aged sample) is obtained by integrating diffuse intensity, but the text provides no explicit description of background subtraction procedure, integration limits, or propagation of uncertainties. This detail is required to assess whether the percentage is robust against possible overlapping magnetic intensity or experimental artifacts.
minor comments (2)
  1. [FT-2D analysis] The abstract states that FT-2D analyses indicate reflections at (1 1/2 0) within the <001> zone axis originate from projections of D0_{22}, Pt_{2}Mo and D1ₐ motifs; a brief statement of the real-space supercell size or the precise projection geometry used would improve clarity.
  2. [SANS measurements] SANS-derived disk radii (~11 Å) and thicknesses (~1 Å) are reported without stating the Q-range fitted or the model form factor employed; adding these details would allow readers to judge consistency with the diffraction length scale.

Simulated Author's Rebuttal

2 responses · 0 unresolved

We thank the referee for the detailed and constructive review. The two major comments concern the security of the nuclear (chemical) origin of the diffuse intensity and the transparency of the 70% CSRO quantification. We address each point below and will revise the manuscript to strengthen the discussion and add missing procedural details.

read point-by-point responses

  1. Referee: [Neutron diffraction results and discussion of diffuse-peak origin] The central attribution of the Q = 1.85 Å^{-1} diffuse peak and its aging dependence to nuclear (chemical) scattering from CSRO is load-bearing yet not fully secured. Neutron diffraction records the sum of nuclear and magnetic structure factors; the manuscript reports neither polarized-neutron spin-flip/non-spin-flip separation nor temperature-dependent measurements above any putative magnetic transition to isolate the nuclear component. While the low-temperature aging trend and non-magnetic simulations are consistent with a chemical origin, they do not quantitatively bound a possible magnetic short-range-order contribution to the integrated intensity used for the 70 % quantification.

    Authors: We acknowledge that polarized-neutron separation or measurements above a magnetic transition temperature would constitute the most direct experimental isolation of the nuclear component. CoCrNi is known from the literature to remain paramagnetic down to low temperatures with no long-range magnetic order, and the aging temperatures (748–798 K) lie far above any reported magnetic transitions. Our non-magnetic atomistic simulations reproduce both the exact Q-position of the diffuse peak and its intensity trend with aging, while the complementary SANS data show Ni-rich disk domains whose scattering contrast is nuclear in origin. Nevertheless, we agree that a quantitative upper bound on any residual magnetic contribution is not provided. In the revised manuscript we will add an explicit paragraph in the discussion section that (i) summarizes the magnetic properties of CoCrNi, (ii) explains why a magnetic SRO contribution is unlikely to account for the observed aging dependence, and (iii) states the limitation that polarized-neutron data would be required for a definitive separation. revision: partial

  2. Referee: [Quantification of ordering degree] The 70 % CSRO retention claim for the gas-atomized sample (relative to the 240 h / 748 K aged sample) is obtained by integrating diffuse intensity, but the text provides no explicit description of background subtraction procedure, integration limits, or propagation of uncertainties. This detail is required to assess whether the percentage is robust against possible overlapping magnetic intensity or experimental artifacts.

    Authors: We thank the referee for highlighting this omission. The revised manuscript will contain a dedicated methods subsection that specifies: (a) background subtraction via a smooth polynomial fit to the scattering intensity in the intervals 1.4–1.6 Å^{-1} and 2.2–2.5 Å^{-1}, (b) integration limits of 1.70–2.00 Å^{-1} centered on the diffuse peak, and (c) uncertainty propagation that combines Poisson counting statistics with the standard deviation obtained from repeated background fits. These additions will allow readers to evaluate the robustness of the reported 70 % figure. revision: yes

Circularity Check

0 steps flagged

No circularity; experimental result and independent simulations stand on direct measurements

full rationale

The manuscript reports an observed diffuse peak at Q = 1.85 Å^{-1} whose intensity increases with aging, quantified by direct integration of scattering intensity (yielding the 70 % relative level between gas-atomized and aged samples). Atomistic simulations are described as reproducing the peak position and presence without any indication that their parameters were fitted to the same neutron data. No equations, fitted parameters renamed as predictions, or self-citation chains appear in the provided text that would reduce the central claim to its own inputs by construction. Attribution questions (nuclear vs. magnetic scattering) concern experimental interpretation and are outside the circularity criteria.

Axiom & Free-Parameter Ledger

0 free parameters · 1 axioms · 0 invented entities

The central claim rests on the domain assumption that the observed diffuse scattering arises from CSRO; no free parameters or invented entities are introduced in the abstract.

axioms (1)
  • domain assumption Diffuse scattering peak at Q=1.85 Å^{-1} in FCC alloys corresponds to chemical short-range order
    Standard interpretation invoked to attribute the experimental feature to CSRO.

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