Tunable Itinerant Ferromagnetism in the Two-Dimensional FePd$_2$Te$_2$ Hosting 1D Spin Chains

Alberto M. Ruiz; Andrei Shumilin; Diego L\'opez-Alcal\'a; Jos\'e J.Baldov\'i; Sourav Dey

REVIEW 4 major objections 4 minor 1 cited by

Tunable Itinerant Ferromagnetism in the Two-Dimensional FePd$_2$Te$_2$ Hosting 1D Spin Chains

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

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Pith's one-line read FePd2Te2 is a two-dimensional ferromagnet whose magnetic order is carried almost entirely by 1D Fe chains: intrachain exchange is 32.8 meV while interchain couplings sit near 0.1 meV.

desk verdict A capable DFT follow-up that gives a plausible microscopic 1D-exchange picture for FePd2Te2, with two new predicted compounds and strain/magnon trends; the missing convergence test on small interchain couplings is the main reason to ask for revision, but the paper deserves a serious referee. read the letter →

arxiv 2506.01009 v1 pith:IJCNP4VJ submitted 2025-06-01 cond-mat.mtrl-sci

Alberto M. Ruiz , Andrei Shumilin , Sourav Dey , Diego López-Alcalá , José J.Baldoví This is my paper

classification cond-mat.mtrl-sci

keywords 1Dmagnetism2DferromagnetsFePd2Te2first-principlescalculationsmagneticexchangedopingstraintronicsmagnondispersion

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 tries to establish that FePd2Te2, a metallic two-dimensional ferromagnet with a measured Curie temperature of 183 K, owes its magnetic order to exchange interactions that run almost exclusively along one-dimensional zigzag chains of Fe atoms. First-principles calculations put the dominant intrachain coupling at $J_{12}=32.8$ meV (ferromagnetic), a competing coupling between equivalent Fe sites at $J_{11}=-3.3$ meV (antiferromagnetic), and the nearest interchain couplings at roughly 0.1 meV, which is what it means for a 2D material to host 1D magnetism. A sympathetic reader would take away that CoPd2Te2 is a predicted ferromagnet with a calculated $T_C$ near 140 K, NiPd2Te2 is paramagnetic, and both Co/Ni substitution and uniaxial strain can tune the ordering temperature and magnetic anisotropy. If the picture is right, FePd2Te2 and its analogues become platforms in which unidirectional spin order, directional magnon propagation, and strain or chemical control of magnetism can be engineered in one ultrathin material.

What carries the argument

The load-bearing object is a spin Hamiltonian of the form $H=-\sum_{ij} J_{ij}\,\mathbf{S}_i\cdot\mathbf{S}_j - \sum_i A\,S_{i,z}^2$, with the isotropic exchange couplings $J_{ij}$ extracted from first-principles density-functional calculations through a Wannier-projected tight-binding model and evaluated up to a 14 Å cutoff. The specific identity that carries the argument is the contrast between $J_{12}$ and $J_{11}$: the two inequivalent magnetic sites in the zigzag chain couple ferromagnetically with tens of meV, while equivalent sites couple weakly and, in FePd2Te2, antiferromagnetically. Because the interchain couplings fall to about 0.1 meV, the Hamiltonian is effectively one-dimensional, and this same Hamiltonian is used both to compute the Curie temperatures with classical atomistic spin simulations and to obtain the magnon dispersions that show the unidirectional propagation.

What would settle it

Grow a single crystal of CoPd2Te2 and measure its magnetisation: the paper predicts a ferromagnetic ground state with a Curie temperature near 140 K, so observing no ferromagnetic order, or a very different $T_C$, would undercut the exchange-parameter extraction. Alternatively, inelastic neutron scattering on FePd2Te2 should reveal a magnon branch along the Fe chains with a bandwidth of a few hundred meV, set by $J_{12}=32.8$ meV, and nearly flat branches perpendicular to the chains; a comparable dispersion in both directions would refute the 1D exchange picture.

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Extended reading notes

Core claim

On the paper's own terms, the magnetic interaction picture in FePd2Te2 and CoPd2Te2 is captured by two primary in-plane exchange couplings: $J_{12}$, between the two inequivalent magnetic sites Fe1 and Fe2, and $J_{11}$, between equivalent sites. In FePd2Te2, $J_{12}$ is strongly ferromagnetic at 32.8 meV while $J_{11}$ is antiferromagnetic at $-3.3$ meV; the coexistence of these competing couplings creates a geometrically frustrated spin system that partially suppresses the net ferromagnetism, but the larger $J_{12}$ wins and the material orders ferromagnetically. In CoPd2Te2, $J_{12}=11.6$ meV and $J_{11}$ is ferromagnetic, giving a predicted $T_C$ near 140 K, while NiPd2Te2 is paramagnetic. Interchain couplings are tiny ($J_{12}\approx0.1$ meV, $J_{11}\approx0.07$ meV), and interlayer couplings are ferromagnetic but smaller still, which is the quantitative evidence for the 1D character. Substituting half the Fe with Co gives ferromagnetic $T_C$ estimates of 150 K (alternating arrangement) or 170 K (consecutive arrangement), while Ni substitution suppresses order and can eliminate it entirely in the consecutive arrangement because Ni$-$Ni coupling vanishes. Uniaxial strain along the chain direction changes the balance: compression makes $J_{12}$ more ferromagnetic but also makes $J_{11}$ more antiferromagnetic, and tensile strain strengthens longer-range couplings and raises $T_C$; the computed magnon dispersions are correspondingly much more dispersive along the chains than perpendicular to them.

Load-bearing premise

The central calculation depends on the assumption that magnetic couplings extracted from density-functional theory, truncated at 14 Å, and fed into classical atomic-spin simulations faithfully reproduce the real quantum magnetism and ordering temperature of these transition-metal compounds.

Editorial extensions

If this is right

FePd2Te2 is a metallic 2D ferromagnet whose magnetic order is essentially unidirectional: the dominant exchange acts inside the zigzag chains, and interchain couplings are two orders of magnitude weaker.
CoPd2Te2 is predicted as a new ferromagnetic member of the family with a Curie temperature near 140 K, while NiPd2Te2 is predicted paramagnetic; both retain the layered structure and are predicted dynamically stable.
Replacing half the Fe by Co yields ferromagnetic Fe0.5Co0.5Pd2Te2 with $T_C$ in the 150$-$170 K range depending on atomic ordering; replacing half by Ni suppresses order, and consecutive Ni pairs drive $T_C$ to zero.
Uniaxial strain along the chain direction tunes magnetism: tensile strain raises $T_C$ by strengthening long-range couplings, while compression makes $J_{12}$ more ferromagnetic but $J_{11}$ more antiferromagnetic, lowering $T_C$.
The magnon spectrum of FePd2Te2 and CoPd2Te2 is strongly anisotropic, dispersive along the chains and nearly flat perpendicular to them, which favours unidirectional magnon transport.

Reading between the lines

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

Beyond the paper, a direct experimental check of the 32.8 meV intrachain exchange would be inelastic neutron scattering along the b-axis: a magnon bandwidth of a few hundred meV, with perpendicular branches nearly flat, would confirm the 1D picture.
The identified frustration between ferromagnetic $J_{12}$ and antiferromagnetic $J_{11}$ suggests an untested lever: weakening $J_{11}$ by pressure, intercalation, or substituting the non-magnetic spacer should raise $T_C$ beyond the measured 183 K even without increasing $J_{12}$.
The same two-sublattice zigzag motif could serve as a screening criterion: other compounds with a large $J_{12}/J_{11}$ ratio are plausible 1D magnets in 2D form.
A testable extension is measuring the strain dependence of $T_C$ in few-layer FePd2Te2 along the chain direction: tensile strain should increase $T_C$ and compression should decrease it, following the predicted behaviour of the long-range couplings.

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Editorial analysis

A structured set of objections, weighed in public.

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

Desk Editor's Note

read the letter

Colleague, here's my take. The paper does something useful: it takes the recently synthesized FePd2Te2, which already looked like a 1D-chain magnet, and actually computes the microscopic exchange. The orbital-resolved decomposition is new, the predicted Co and Ni analogs are concrete targets, and the strain and magnon results give experimentalists something to check. The work is honest in the sense that the Hamiltonian is built from DFT/TB2J with no parameters fitted to the measured TC; the 183 K is used only as a comparison. That is reproducible and falsifiable.

The soft spot is exactly where the 1D claim lives. The interchain couplings that separate intrachain J12=32.8 meV from interchain ~0.1 meV are very small numbers, and they are taken from a TB2J calculation truncated at 14 Å. For an itinerant metallic ferromagnet, long-range oscillatory exchange is a real risk, and the paper does not show a cutoff convergence test. The reduced d/p Wannier basis also omits Fe-4s/Pd-5s, which can matter near the Fermi level. So the qualitative picture — strongly dominant intrachain FM — is probably robust, but the quantitative ratio that defines '1D' is less certain.

Two smaller issues. NiPd2Te2 is described as dynamically stable while its phonon spectrum has a small negative branch around Gamma; the text should either call it marginal or temper the claim. And TC=240 K vs 183 K is a 30% overestimate; the authors call it 'not too far'. That is a bit too dismissive, though for a classical-spin simulation of an itinerant system it is not shocking. A short discussion of expected error in VAMPIRE TC would go a long way.

The paper does not fit the experimental TC, so there is no circularity. The citation to the synthesis paper is appropriate. I do not think the stress-test concern sinks the paper; the quantitative uncertainty is real but the central mechanism is supported by the orbital decomposition and the consistency of the easy axis and moment.

Who is this for? People working on 2D magnets, especially the FeGeTe family and FePd2Te2 experiments. It deserves a serious referee. Recommend acceptance after a moderate revision that adds a cutoff convergence test, addresses the Ni phonon, and softens the TC claim.

Referee Report

4 major / 4 minor

Summary. The manuscript reports a first-principles study of the layered ferromagnet FePd2Te2, which contains 1D Fe zigzag chains, and argues that its magnetic exchange is predominantly one-dimensional: intrachain coupling J12 = 32.8 meV (ferromagnetic) and J11 = -3.3 meV (antiferromagnetic), with interchain coupling on the order of 0.1 meV. The authors extend the analysis to isostructural CoPd2Te2 (predicted ferromagnetic) and NiPd2Te2 (predicted paramagnetic), to Co/Ni-substituted FePd2Te2, and to uniaxial strain along the chain direction, and they compute magnon dispersions showing strong anisotropy. The methods combine DFT (VASP), Wannier projection (Wannier90), exchange-coupling extraction (TB2J), and classical atomistic spin dynamics (VAMPIRE) for Curie temperatures.

Significance. If the central exchange picture holds, the paper provides a valuable microscopic explanation of a recently synthesized 2D metallic ferromagnet with 1D spin chains and identifies concrete chemical and mechanical tuning knobs. The study has clear strengths: it reproduces the experimental easy axis and magnetic moment, uses a transparent spin-Hamiltonian framework with no parameters fitted to the experimental TC, and makes falsifiable predictions for two new compounds and for strain dependence. The main risk is that the quantitative conclusions, especially the claimed 1D nature of the exchange and the magnitude of TC, rest on a truncated classical-spin mapping that is not fully validated.

major comments (4)

[Methods (TB2J) and Figure 2] The central claim that the exchange is one-dimensional relies on Jij values obtained with TB2J using a Wannier d/p-only basis and a coupling cutoff at 14 Å, yet no convergence test is shown. The interchain couplings that justify the '1D nature' are 0.1-0.15 meV, precisely the small numbers most sensitive to truncation and to the omitted long-range oscillatory tails expected in itinerant ferromagnets. Please provide a plot of Jij versus distance, the cumulative Jlong as a function of cutoff, and a test showing that increasing the cutoff beyond 14 Å or including s orbitals in the Wannier basis does not change the qualitative conclusion.
[Results (Curie temperature)] The VAMPIRE simulation gives TC = 240 K for FePd2Te2 versus the experimental 183 K, a 31% overestimate that the text describes as 'not too far'. Because the paper's quantitative tuning predictions for Co/Ni substitution and strain are expressed in terms of TC, the origin of this discrepancy needs to be assessed rather than dismissed. Please discuss whether the error is expected from classical spin dynamics, from the truncated exchange model, or from the DFT exchange parameters, and if possible provide a benchmark on a related material or a finite-size/quantum-correction estimate.
[Results (phonon spectra) and Conclusions] The text states that the phonon spectrum of NiPd2Te2 has 'a small negative contribution around G' (Figure 1d), but the abstract and conclusions say that both CoPd2Te2 and NiPd2Te2 are dynamically stable. A negative phonon mode indicates dynamical instability, so the claim of stability for NiPd2Te2 is unsupported as written. Please clarify whether the negative mode is a numerical artifact and, if not, revise the stability claim and any conclusions drawn from it.
[Results (exchange model) and Figure 4] The paper introduces a long-range sum Jlong and uses it to explain strain trends in TC, but the main-text definition of the Hamiltonian and the figure labels are inconsistent (Figure 4 caption lists 'J12 and J11 and J12' instead of Jlong). More substantively, the relative roles of J12, J11, and Jlong under strain should be quantified with a decomposition of the TC change into contributions from each coupling, since the strain dependence of Jlong is claimed to be decisive but no numerical values are given for Jlong at different strains.

minor comments (4)

[Equation (1)] The spin Hamiltonian is rendered with garbled symbols in the manuscript text; please reformat it so that the sums over Jij and the single-ion anisotropy term A are unambiguous.
[Figure 4 caption] The caption lists 'exchange couplings J12, J11 and J12'; the third quantity should presumably be Jlong, which is defined in the text.
[Table 1] The table uses dashes in inconsistent ways and would benefit from explicit 'not applicable' entries and a note on the sign convention for MAE.
[Results (substitution)] The statement that 'the system does not retain long-range magnetic ordering (TC = 0K)' for the CON configuration of Fe0.5Ni0.5Pd2Te2 is surprising given the large Fe1-Fe2 coupling reported in the same paragraph; please clarify whether this is a finite-size effect of the VAMPIRE supercell or a real frustration effect.

Circularity Check

0 steps flagged · score 0.0 of 10

No significant circularity: exchange couplings, TC, and magnons are computed from DFT with no parameter fitted to the experimental ordering temperature.

full rationale

The derivation chain is self-contained. Magnetic exchange couplings J12 and J11 are obtained from DFT via the Wannier90/TB2J pipeline using a spin Hamiltonian with no adjustable parameters, and the experimental TC = 183 K is used only as a post-hoc comparison ('The calculated TC for FePd2Te2 is 240K, which is not too far from the experimental value of 183K'), not as a constraint. The TC = 240 K and CoPd2Te2 TC = 140 K values follow from VAMPIRE classical spin dynamics using the computed couplings and moments; the magnon dispersion is likewise evaluated from the same computed spin Hamiltonian, which is internal consistency rather than a fitted prediction. Co/Ni substitution and strain trends are obtained by re-running the same first-principles workflow on distinct structures, so they are not encoded in the input. The self-citations to prior work by the authors (e.g., refs 13, 27, and 38) are motivational analogies with Fe3GeTe2 and Fe5GeTe2 and are not load-bearing for the central 1D-ferromagnetism claim. The 14 Å truncation of exchange couplings and the classical-spin approximation are convergence and validity risks for the quantitative Jij and TC values, but they do not make the derivation circular because the target conclusion is not an input to the calculation.

Assumptions & free parameters 2 free parameters · 4 assumptions · 0 invented entities

The DFT calculations contain no data-fitted parameters; the central predictions come from computed exchange couplings. The main assumptions are the GGA approximation for correlated d electrons, the TB2J mapping from a Wannier Hamiltonian, the truncation of exchange at 14 Å, and the use of classical spin dynamics to estimate TC. These assumptions are standard but can bias quantitative predictions.

free parameters (2)

Exchange coupling truncation radius = 14 Å
Spin Hamiltonian includes couplings up to 14 Å and neglects beyond; this cutoff affects Jij sums, TC, and magnon dispersions.
VAMPIRE simulation supercell size = 15 nm
Finite-size spin simulation supercell used for TC; finite-size effects could bias TC values.

assumptions (4)

domain assumption DFT-GGA without Hubbard U gives reliable electronic structure and exchange couplings for these itinerant metallic magnets.
VASP/GGA used; no U or hybrid functional; correlated d electrons may be poorly described.
domain assumption TB2J mapping from Wannier Hamiltonian to Heisenberg Jij is valid.
A tight-binding Hamiltonian with reduced basis (d orbitals of Fe/Co/Ni and Pd, p of Te) is used as input to TB2J; accuracy depends on Wannier projection.
domain assumption Classical-spin VAMPIRE simulations reproduce magnetic ordering temperatures.
TC estimated with 10000 steps and 15 nm supercells; quantum fluctuations and 1D long-range order are not treated quantum mechanically.
domain assumption Phonon stability and formation energy predict synthesizability.
Stable phonons and negative Eform are taken as indicators that CoPd2Te2 and NiPd2Te2 can be made.

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Cite this review

Pith. "Pith review of Tunable Itinerant Ferromagnetism in the Two-Dimensional FePd$_2$Te$_2$ Hosting 1D Spin Chains." pith.science (2026). https://pith.science/paper/IJCNP4VJ

@misc{pith2026250601009,
  author       = {Pith},
  title        = {Pith review of: Tunable Itinerant Ferromagnetism in the Two-Dimensional FePd$_2$Te$_2$ Hosting 1D Spin Chains},
  year         = {2026},
  howpublished = {\url{https://pith.science/paper/IJCNP4VJ}},
  note         = {Machine review of arXiv:2506.01009}
}

abstract

One-dimensional (1D) magnetism offers unidirectional spin interactions that allow unique tunable properties and unconventional spin phenomena. However, it often suffers from poor stability, limiting practical applications. In this regard, integrating 1D magnetism into two-dimensional (2D) materials enables a promising route to stabilize these systems while preserving their anisotropic magnetic characteristics. Here, we focus on the 2D ferromagnet FePd$_2$Te$_2$ (T$_C$ = 183K), which hosts 1D spin chains and strong in-plane anisotropy. Our first-principles calculations reveal highly anisotropic magnetic exchange interactions, confirming its 1D ferromagnetic nature. We modulate this behavior by Co and Ni substitution and introduce two new members of this family, CoPd$_2$Te$_2$ -- a ferromagnet -- and NiPd$_2$Te$_2$. Our results unveil the microscopic mechanisms governing the behaviour of FePd$_2$Te$_2$ and CoPd$_2$Te$_2$. Furthermore, we also demonstrate that the variation of the chain length is key to modulate magnetism. Finally, we determine the magnon dispersion, showcasing a pronounced anisotropy that enables unidirectional magnon propagation.

Figures

Figures reproduced from arXiv: 2506.01009 by the authors.

**Figure 1.** (a) Top view of bulk FePd2Te2. Color code: Fe (red), Pd (grey) and Te (green). (b) 3D Brillouin zone (BZ) of FePd2Te2 and illustration of 1D chain of the material. (c) Band structure and (d) phonon spectra for FePd2Te2, CoPd2Te2 and NiPd2Te2 (from left to right, respectively) [PITH_FULL_IMAGE:figures/full_fig_p015_1.png] view at source ↗

**Figure 2.** Top view of 1D chains of (a) FePd2Te2 and (b) CoPd2Te2. For simplicity, we only depict the magnetic centres Fe and Co atoms. (c) Exchange interactions J12 and J11 for FePd2Te2 (red) and CoPd2Te2 (blue). (d) Orbital-resolved J12 exchange coupling for FePd2Te2 (left), CoPd2Te2 (middle) and subtracted contribution, DJ12 (right). (e) Same as (d), but for J11 [PITH_FULL_IMAGE:figures/full_fig_p016_2.png] view at source ↗

**Figure 3.** Top view of 1D chains in the ALT configuration for (a) Fe0.5Co0.5Pd2Te2 and (a) Fe0.5Ni0.5Pd2Te2 along with their corresponding (c) magnetic couplings for each material. Top view of 1D chains in the CON configuration for (d) Fe0.5Co0.5Pd2Te2 and (e) Fe0.5Ni0.5Pd2Te2 along with their corresponding (f) magnetic couplings for each material [PITH_FULL_IMAGE:figures/full_fig_p017_3.png] view at source ↗

Figures from the paper (2 more)

**Figure 4.** Figure 4: Evolution of (a) MAE, (b) exchange couplings J [PITH_FULL_IMAGE:figures/full_fig_p018_4.png]

**Figure 5.** Figure 5: Magnon dispersion for (a) FePd2Te2 and (b) CoPd2Te2 as a function of strain applied along the [010] direction [PITH_FULL_IMAGE:figures/full_fig_p018_5.png]

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Cited by 1 Pith paper

Reviewed papers in the Pith corpus that reference this work. Sorted by Pith novelty score. Full citation record

Atomic to mesoscale hierarchical structures and magnetic states in an anisotropic layered ferromagnet FePd2Te2
cond-mat.mtrl-sci 2025-06 conditional novelty 6.0 of 10

Microscope images show that twinning domains in FePd2Te2 create compressed and stretched regions with different magnetic responses, including a polarized paramagnetic state above the ordering temperature.

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Works this paper leans on

5 extracted references · 5 canonical work pages · cited by 1 Pith paper

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María de Maeztu

consistent with the previously discussed exchange interactions. In both compounds, strongly dispersive branches are observed along the Γ−Z direction, corresponding to magnons propagating along the 1D spin chains. In contrast, dispersion is notably weaker along directions perpendicular to them (e.g., Γ−B or Γ−Y2), indicating suppressed interchain magnon tr...

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Pith tools

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

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(35) Qiao, L.; Li, M.; Cui, Y.; Xu, S.; Reimers, J

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María de Maeztu

consistent with the previously discussed exchange interactions. In both compounds, strongly dispersive branches are observed along the Γ−Z direction, corresponding to magnons propagating along the 1D spin chains. In contrast, dispersion is notably weaker along directions perpendicular to them (e.g., Γ−B or Γ−Y2), indicating suppressed interchain magnon tr...

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(13) Esteras, D. L.; Baldoví, J. J. Strain Engineering of Magnetic Exchange and Topological Magnons in Chromium Trihalides from First-Principles. Materials Today Electronics 2023, 6, 100072. (14) Olsen, T. Magnetic Anisotropy and Exchange Interactions of Two-Dimensional FePS 3 , NiPS 3 and MnPS3 from First Principles Calculations. J Phys D Appl Phys 2021,...

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