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arxiv: 2604.12571 · v2 · submitted 2026-04-14 · ❄️ cond-mat.mtrl-sci · cond-mat.mes-hall

Tuning Structure and Magnetism in Large-Scale 2D Ferromagnet Fe₃GeTe₂ through Ni Doping

Kacho Imtiyaz Ali Khan , Tauqir Shinwari , Soheil Ershadrad , Majid Ahmadi , Weiben Li , Hua Lv , Frans Munnik , Adriana I. Figueroa
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Manuel Valvidares Sandra Ruiz-G\'omez Lucia Aballe Jens Herfort Michael Hanke Bart Kooi Biplab Sanyal Jo\~ao Marcelo J. Lopes
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Pith reviewed 2026-05-10 14:52 UTC · model grok-4.3

classification ❄️ cond-mat.mtrl-sci cond-mat.mes-hall
keywords 2D ferromagnetNi dopingFe3GeTe2Curie temperatureperpendicular magnetic anisotropyvan der Waals epitaxymolecular beam epitaxySTEM imaging
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The pith

Nickel doping in Fe3GeTe2 films shrinks both lattice directions and lowers the Curie temperature to 50 K through substitution plus intercalation.

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

The work shows that molecular beam epitaxy grows large-area, high-quality Fe3GeTe2 films with controlled nickel addition. Nickel atoms replace iron inside the layers and also occupy the spaces between layers, which contracts the crystal in both in-plane and out-of-plane directions. These structural shifts remove the preference for magnetization to point perpendicular to the film plane and cut the temperature below which the material stays ferromagnetic down to 50 kelvin. Calculations that model the atomic energies confirm that the doping alters the strength of magnetic interactions between atoms and the energy cost of different magnetization directions. The result supplies a practical route to adjust magnetic behavior in two-dimensional ferromagnets that can be produced at scale.

Core claim

MBE growth produces epitaxial Fe3GeTe2 films on graphene in which nickel both substitutes on iron sites and intercalates into the van der Waals gaps. This incorporation shrinks the in-plane and out-of-plane lattice parameters. The combined substitution and intercalation suppresses perpendicular magnetic anisotropy and reduces the Curie temperature to 50 K. Density functional theory calculations map the resulting changes in magnetic exchange interaction parameters and atom-projected magnetocrystalline anisotropy energies that underlie the experimental observations.

What carries the argument

Nickel substitution on iron sites together with intercalation into the van der Waals gaps, imaged by integrated differential phase contrast STEM, which contracts the lattice and modifies exchange and anisotropy energies.

If this is right

  • Molecular beam epitaxy supplies reproducible thickness and doping control for large-area two-dimensional ferromagnet films.
  • The observed lattice contraction and lowered ordering temperature demonstrate a route to tune magnetic ordering for specific operating conditions.
  • Density functional theory results tie the experimental changes directly to shifts in atom-to-atom exchange strengths and directional anisotropy energies.
  • The van der Waals epitaxial films on graphene are compatible with stacking into heterostructures for device testing.

Where Pith is reading between the lines

These are editorial extensions of the paper, not claims the author makes directly.

  • The same substitution-plus-intercalation approach could be tested on other layered ferromagnets to see whether similar drops in ordering temperature occur.
  • Experiments that deliberately introduce only substitution or only intercalation would separate which process most strongly affects the magnetic properties.
  • Because the lattice shrinks uniformly, the doped films may respond differently to external strain than undoped films.
  • Scalable growth of the doped material makes it feasible to fabricate and test many samples with varying nickel content in the same run.

Load-bearing premise

The measured drops in perpendicular anisotropy and Curie temperature arise specifically from nickel atoms both replacing iron and entering the gaps between layers rather than from defects or thickness differences in the films.

What would settle it

Prepare nickel-containing Fe3GeTe2 films under growth conditions that allow substitution but block intercalation into the gaps, then check whether the Curie temperature still falls to 50 K and whether perpendicular anisotropy is still suppressed.

Figures

Figures reproduced from arXiv: 2604.12571 by Adriana I. Figueroa, Bart Kooi, Biplab Sanyal, Frans Munnik, Hua Lv, Jens Herfort, Jo\~ao Marcelo J. Lopes, Kacho Imtiyaz Ali Khan, Lucia Aballe, Majid Ahmadi, Manuel Valvidares, Michael Hanke, Sandra Ruiz-G\'omez, Soheil Ershadrad, Tauqir Shinwari, Weiben Li.

Figure 1
Figure 1. Figure 1: Schematics and structural properties of Pristine FGT and Ni-doped FGT films. One unit cell of pristine FGT and Ni-doped FGT consists of two quintuple layers (QLs), as displayed along the two orthogonal crystallographic directions (a) [1010] and (b) [1210]. (c,d) Corresponding reflection high-energy electron diffraction (RHEED) patterns for pristine FGT [upper panel] and Ni-doped FGT [bottom panel]. (e) Out… view at source ↗
Figure 2
Figure 2. Figure 2 [PITH_FULL_IMAGE:figures/full_fig_p005_2.png] view at source ↗
Figure 3
Figure 3. Figure 3: f-h], we observed a drastic reduction of TC from 210 K (for pristine FGT) down to 50 K (Ni-doped FGT, x = 0.15). The reduction of TC upon Ni incorporation suggests a weakening of long-range ferromagnetic ordering due to structural deformation of the unit cell. To conclude, from the SQUID measurement, we observed that [PITH_FULL_IMAGE:figures/full_fig_p007_3.png] view at source ↗
Figure 4
Figure 4. Figure 4: XAS and XMCD for pristine FGT and Ni-doped FGT film stacks (a) XMCD hys￾teresis loops measured at 3.5 K for pristine and Ni-doped FGT films. (b) Dependence of XMCD signal amplitude and coercive field (HC) with Ni doping concentration. (c) XAS (open symbols) and XMCD (closed symbols) spectra for Ni-doped (x = 0.06) FGT film, with solid lines showing the integrated signals. (d) Comparison of XMCD spectra (Fe… view at source ↗
Figure 5
Figure 5. Figure 5: DFT results on magnetism. Calculated exchange interaction parameters Jij (truncated between -10 to +10 meV) for (a) Fe-Fe pairs in pristine FGT (x = 0.00), (b) Fe-Fe, Fe-Ni and Ni-Ni pairs in Ni-doped FGT (x = 0.15). Multiple data points for every neighbor interaction shown in (b) correspond to various pair-exchange parameters in the supercell. In both (a) and (b), the insets show all the values of Fe-Fe e… view at source ↗
read the original abstract

Two-dimensional ferromagnets with strong perpendicular magnetic anisotropy exhibit magnetic order down to the monolayer thickness, beneficial for energy-efficient spintronic devices. In this work, molecular beam epitaxy has been employed to realize controlled Ni-doping in Fe$_{3}$GeTe$_{2}$ (FGT) epitaxial films. MBE not only enables a large-scale growth of 2D films, but also allows a precise control over thickness and doping. X-ray diffraction and scanning transmission electron microscopy (STEM) reveal the formation of high-quality epitaxial films of pristine and Ni-doped FGT on graphene via van der Waals (vdW) epitaxy. Integrated differential phase contrast STEM images further provide in-depth information on Ni substitution and intercalation into the vdW gaps. Ni incorporation in doped films results in the shrinking of both in-plane and out-of-plane lattice parameters. Superconducting Quantum Interference Device, Hall, and X-ray magnetic circular dichroism measurements were utilized to probe the ferromagnetic properties of the films. Due to both Ni substitution and intercalation into the vdW gaps for Ni-doped FGT films, we observed a suppression of PMA and a drastic reduction in the Curie temperature down to 50 K. Our density functional theory based calculations of structural and magnetic properties further supports and provide deep insights into the variations of magnetic exchange interaction parameters and atom-projected magnetocrystalline anisotropy energies due to Ni doping to understand the experimental observations.

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 reports MBE growth of Ni-doped Fe3GeTe2 epitaxial films on graphene. XRD and iDPC-STEM indicate high-quality vdW epitaxy with Ni both substituting on Fe sites and intercalating in the vdW gaps, accompanied by contraction of in-plane and out-of-plane lattice parameters. SQUID, Hall, and XMCD measurements show suppression of perpendicular magnetic anisotropy and reduction of Curie temperature to 50 K in the doped films. DFT calculations are used to rationalize changes in exchange parameters and atom-projected magnetocrystalline anisotropy energies.

Significance. If the reported magnetic tuning is robustly attributable to the specific Ni incorporation modes, the work would demonstrate a scalable MBE route to engineer Tc and anisotropy in large-area 2D ferromagnets, which is relevant for spintronic device concepts. The use of multiple orthogonal probes (XRD, STEM, magnetometry, XMCD) plus theory is a methodological strength.

major comments (3)
  1. [Abstract] Abstract and results: the central claim that PMA suppression and Tc reduction to 50 K occur 'due to both Ni substitution and intercalation' rests on qualitative iDPC-STEM interpretation without reported quantitative site-occupancy fractions, intensity-line-profile statistics, or EDX/XPS composition maps correlated to the magnetic data across doping levels.
  2. [Results] Results (magnetic characterization): no error bars, standard deviations, or sample-to-sample statistics are provided for the reported Tc values, anisotropy fields, or Hall data; likewise, no thickness-matched undoped FGT reference series is described to isolate doping effects from possible thickness inhomogeneity or growth-induced disorder.
  3. [DFT calculations] DFT section: the calculated exchange parameters and anisotropy energies depend on the assumed structural models for substitution versus intercalation; the manuscript does not show how these models were validated against the experimental iDPC-STEM images or test the sensitivity of the magnetic trends to small variations in Ni site occupancy.
minor comments (2)
  1. [Abstract] The abstract states 'large-scale growth' but provides no quantitative metrics (e.g., lateral dimensions, uniformity maps, or wafer-scale coverage) to support this description.
  2. [Introduction] Notation for anisotropy (PMA) and Curie temperature (Tc) is introduced without consistent definition on first use in the main text.

Simulated Author's Rebuttal

3 responses · 0 unresolved

We thank the referee for the careful and constructive review of our manuscript. The comments have helped us identify areas where additional detail and analysis can strengthen the presentation. We respond point-by-point below and have revised the manuscript accordingly.

read point-by-point responses

  1. Referee: [Abstract] Abstract and results: the central claim that PMA suppression and Tc reduction to 50 K occur 'due to both Ni substitution and intercalation' rests on qualitative iDPC-STEM interpretation without reported quantitative site-occupancy fractions, intensity-line-profile statistics, or EDX/XPS composition maps correlated to the magnetic data across doping levels.

    Authors: We agree that quantitative support strengthens the attribution of the magnetic changes to the specific Ni incorporation modes. In the revised manuscript we have added (i) intensity line profiles extracted from multiple iDPC-STEM images with statistical error bars, (ii) estimated Ni site-occupancy fractions derived from those profiles, and (iii) EDX composition maps for films at different nominal doping levels, directly correlated with the corresponding SQUID and Hall data. These additions confirm that both substitutional and intercalated Ni are present and that their combined effect accounts for the observed PMA suppression and Tc reduction to 50 K. The abstract has been updated to reflect this quantitative evidence. revision: yes

  2. Referee: [Results] Results (magnetic characterization): no error bars, standard deviations, or sample-to-sample statistics are provided for the reported Tc values, anisotropy fields, or Hall data; likewise, no thickness-matched undoped FGT reference series is described to isolate doping effects from possible thickness inhomogeneity or growth-induced disorder.

    Authors: We acknowledge that the original submission lacked explicit statistical information. The revised manuscript now reports error bars and standard deviations on all Tc, anisotropy-field, and Hall data, obtained from repeated measurements on multiple samples grown under identical conditions. In addition, we have included a dedicated series of thickness-matched undoped FGT reference films grown on the same graphene substrates with the same nominal thicknesses as the doped films. These reference data demonstrate that the suppression of PMA and the drop in Tc are attributable to Ni incorporation rather than thickness variation or growth-induced disorder. revision: yes

  3. Referee: [DFT calculations] DFT section: the calculated exchange parameters and anisotropy energies depend on the assumed structural models for substitution versus intercalation; the manuscript does not show how these models were validated against the experimental iDPC-STEM images or test the sensitivity of the magnetic trends to small variations in Ni site occupancy.

    Authors: The structural models used in the DFT calculations were constructed to reproduce the Ni positions directly observed in the experimental iDPC-STEM images. In the revised manuscript we now include a side-by-side comparison of simulated iDPC-STEM images generated from the DFT-relaxed structures with the corresponding experimental images, confirming that the models accurately capture both substitution and intercalation. We have also performed a sensitivity analysis in which the Ni site occupancies were varied by ±10 % around the experimentally estimated values; the resulting exchange parameters and atom-projected anisotropy energies retain the same qualitative trends (reduced Tc and suppressed PMA) reported in the original submission. revision: yes

Circularity Check

0 steps flagged

No significant circularity; central claims rest on direct experimental measurements

full rationale

The paper's key results on PMA suppression and Tc reduction to 50 K are presented as direct observations from SQUID, Hall, and XMCD measurements on MBE-grown films, with structural confirmation via XRD and iDPC-STEM imaging of Ni sites. DFT is invoked only for post-hoc support on exchange parameters and anisotropy energies, without any equations or fits that define the measured Tc/PMA values by construction. No self-definitional loops, fitted inputs renamed as predictions, load-bearing self-citations, uniqueness theorems, or ansatz smuggling appear in the reported chain. The derivation is self-contained as empirical data collection and interpretation.

Axiom & Free-Parameter Ledger

0 free parameters · 2 axioms · 0 invented entities

The central claim rests on standard assumptions of van der Waals epitaxy and the reliability of DFT for magnetic properties in these compounds; no free parameters are fitted to produce the reported Tc or PMA values, and no new entities are postulated.

axioms (2)
  • domain assumption Van der Waals epitaxy on graphene produces high-quality epitaxial FGT films
    Invoked to explain the formation of high-quality films observed by XRD and STEM.
  • domain assumption DFT calculations reliably predict changes in magnetic exchange and magnetocrystalline anisotropy due to Ni doping
    Used to interpret the experimental suppression of PMA and Tc reduction.

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