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Evolution of electronic and magnetic properties in a series of iridate double perovskites Pr$_{2-x}$Sr$_x$MgIrO$_6$ ($x$ = 0, 0.5, 1.0)

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Pith's one-line read In the double perovskites Pr2−xSrxMgIrO6, ordered magnetism comes from iridium while praseodymium stays paramagnetic, so the predicted half-metallic antiferromagnet does not form.

desk verdict Solid experimental refutation of HMAFM in PrSrMgIrO6, with a softer-than-claimed Pr3+ non-ordering conclusion that needs a direct probe. read the letter →

arxiv 1908.05973 v1 pith:PU4W2QKF submitted 2019-08-16 cond-mat.str-el

Abhisek Bandyopadhyay , I. Carlomagno , L. Simonelli , M. Moretti Sala , A. Efimenko , C. Meneghini , Sugata Ray This is my paper · ORCID
classification cond-mat.str-el
keywords iridatedoubleperovskitesspin-orbitcouplinghalf-metallicantiferromagnetismPr3+singletd4iridiummagnetismantiferromagneticorderRIXSMottinsulator
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 sets out to test a theoretical prediction that strontium doping would turn the double perovskite Pr2MgIrO6 into a half-metallic antiferromagnet. Using magnetization, resistivity, X-ray absorption, photoemission, and RIXS on three compositions ($x = 0$, 0.5, 1), the authors conclude that no half-metallicity appears: every composition is an insulator whose gap is set by spin-orbit coupling on iridium. The ordered magnetic response likewise belongs to iridium, with Ir4+ moments ordering at 14 K, the transition weakening to about 6 K with doping, and no order at all for the Ir5+ compound, while Pr3+ contributes only a paramagnetic background. The result matters because it removes a candidate route to half-metallic antiferromagnetic spintronics and sharpens the picture of how 5d electrons and local crystal distortions compete.

What carries the argument

The argument is carried by the spin-orbit-coupled $J$ multiplets of iridium, tuned by strontium doping from the magnetic $d^5$ configuration (Ir4+) to the nominally nonmagnetic $d^4$ configuration (Ir5+). The load-bearing comparison is with barium yttrium iridate, a cubic $d^4$ double perovskite whose low-energy RIXS features and small moments show that the ideal nonmagnetic $J = 0$ state is destabilized by octahedral tilting, noncubic crystal fields, and Ir-Ir hopping; the same mechanism is invoked for PrSrMgIrO6. The other pillar is the non-Kramer Pr3+ ion, whose low-symmetry crystal field leaves a singlet ground state, so it can only contribute a temperature-independent paramagnetic background rather than ordered moments.

What would settle it

Neutron diffraction or muon-spin rotation on Pr2MgIrO6 below 14 K would settle it: an ordered moment on the Pr site, or a second transition below 2 K in PrSrMgIrO6, would contradict the assignment of all ordered magnetism to iridium. Equally decisive would be spin-resolved photoemission showing a finite density of states at the Fermi level in either doped compound.

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Extended reading notes

Core claim

The central experimental finding is that none of the three double perovskites is half-metallic and none shows long-range magnetic order on the praseodymium sublattice. In Pr2MgIrO6 (Ir4+, $d^5$) the authors observe a sharp antiferromagnetic transition near 14 K; substituting strontium oxidizes iridium toward 5+ ($d^4$) and weakens the exchange, shifting the transition to about 6 K in Pr1.5Sr0.5MgIrO6 and suppressing order entirely in PrSrMgIrO6 down to 2 K. Curie-Weiss analysis, using La2MgIrO6 as a reference for the Ir4+ moment, reproduces the measured effective moments when Pr3+ is treated as a nonmagnetic singlet contributing only its paramagnetic susceptibility. The authors therefore conclude that the spin-orbit-coupled $J$ states of iridium control both the insulating gap and the correlated magnetism, and that the atomic $J = 0$ picture for Ir5+ fails because noncubic crystal fields and intersite hopping generate small moments.

Load-bearing premise

The claim that Pr3+ is magnetically inert rests on the assumption that Pr3+ has a nonmagnetic singlet ground state under the low-symmetry A-site crystal field, so it neither orders nor couples to iridium moments.

Editorial extensions

If this is right

  • If the measurements are right, the proposed transition from spin-orbit Mott insulator to half-metallic antiferromagnet does not occur in this series, so this family should be dropped from half-metallic antiferromagnet candidate lists.
  • The insulating behavior of all three compositions, including the $d^4$ end member, supports spin-orbit coupling as the gap-forming interaction even when the atomic $J = 0$ limit is broken.
  • Weakening of the antiferromagnetic order from 14 K to 6 K to no order tracks the dilution of magnetic Ir4+ by nonmagnetic Ir5+, implying exchange rather than single-ion physics sets the ordering temperature.
  • Pr3+ being inert means any future claim of Pr-Ir coupling in this family needs direct evidence such as an ordered moment on the praseodymium site.

Reading between the lines

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

  • Inference: measuring the same series with praseodymium replaced by a nonmagnetic rare earth (for example yttrium or lanthanum) would separate the iridium-only magnetism from any residual 4f contribution and test whether the small Ir5+ moment is intrinsic to the $d^4$ double perovskite.
  • Inference: because Pr3+ is claimed to be a singlet, a low-temperature specific-heat measurement should show only the iridium contribution plus the lattice; an extra Schottky anomaly from a praseodymium crystal-field doublet would indicate the singlet assumption needs revision.
  • Inference: the absence of order down to 2 K with a Curie-Weiss temperature near -39 K makes PrSrMgIrO6 a candidate for a frustrated, possibly spin-liquid-like state of weak Ir moments, but identifying the ground state would need muon spin rotation or neutron scattering.
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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 / 4 minor

Summary. The paper reports a combined structural, spectroscopic, transport, and magnetization study of the double perovskites Pr2-xSrxMgIrO6 (x = 0, 0.5, 1). The authors find all three compounds to be insulating with no density of states at the Fermi level and no spontaneous ferromagnetic moment in the doped samples. XANES and XPS establish the Ir valence progression from 4+ to 5+. Magnetic measurements reveal an AFM transition near 14 K in Pr2MgIrO6, a weakened transition near 6 K in Pr1.5Sr0.5MgIrO6, and no ordering down to 2 K in PrSrMgIrO6. The central conclusions are that the predicted half-metallic antiferromagnetic state is absent, that the magnetic properties are governed by Ir moments, and that Pr3+ contributes only a paramagnetic background without ordering or coupling to Ir.

Significance. If the conclusions hold, the paper provides a convincing experimental refutation of the HMAFM proposal of Ghimire et al. for PrSrMgIrO6, supported by several independent probes: gapped transport, valence-band XPS, absence of spontaneous magnetization, and Arrott analysis. The systematic oxidation-state determination and careful XRD/EXAFS structural characterization are strengths, as is the qualitative high-resolution RIXS comparison with Ba2YIrO6. However, the claim that Pr3+ is magnetically inert is less secure, because it relies on an assumed nonmagnetic crystal-field singlet and an indirect moment balance rather than a direct probe of the Pr sublattice. This weakens the paper's strongly stated conclusion about the exclusive role of Ir moments.

major comments (3)
  1. [Section III F, Eqs. (1)-(5)] The moment balance uses the free-ion Pr3+ effective moment of 3.58 μB and an Ir4+ moment taken from a separately measured LMIO sample, but no uncertainties are propagated through Eqs. (1)-(5). The numerical agreement with the Curie-Weiss effective moments is therefore not an independent quantitative verification of the Pr3+ paramagnetic-only assumption. The conclusion that Pr3+ neither orders nor couples to the Ir sublattice needs direct evidence (e.g., neutron diffraction, muon spin rotation, or Pr-resonant X-ray scattering) or at least an explicit caveat that bulk susceptibility cannot rule out a small ordered Pr moment below the AFM transitions.
  2. [Section III F (PSMIO discussion)] The excess of ~0.3 μB/f.u. over the Pr3+ free-ion value is assigned to a finite Ir5+ moment, but this number is smaller than typical Curie-Weiss fitting uncertainties, and no error bars are supplied for the fit parameters or for the LMIO reference moment. The inference that a correlated moment develops on every Ir site is therefore not quantitatively established; the excess could equally arise from a deviation of the Pr3+ effective moment from the free-ion value in the crystal field. The authors should present error bars and a sensitivity analysis, or temper this conclusion.
  3. [Section III F and Figure 7] The absence of ZFC/FC divergence and the presence of only weak kinks in χ(T) are used to rule out ordering on the Pr sublattice, but bulk dc susceptibility has limited sensitivity to a small ordered Pr moment when a large Pr/Ir paramagnetic background is present. If Pr3+ carries even ~0.2-0.5 μB below 14 K in PMIO or couples to Ir moments in PSMIO1505, the assignment of the transitions purely to Ir moments would need revision. The authors should explicitly state this limitation or provide complementary specific-heat, neutron, or μSR data.
minor comments (4)
  1. [References] Reference 42 contains a corrupted author name: 'Jaworska-Go/suppress l¸ ab' should be corrected to the proper author string.
  2. [Introduction and throughout] There are typographical errors such as 'infact' (Introduction) and 'valance band' (should be 'valence band' in several places); please proofread carefully.
  3. [Section III F and Figure 7 caption] 'Arrot plot' should be 'Arrott plot' in the text and figure caption.
  4. [Section III D] The text refers to the ESRF beamline as 'ID23' when describing the PSMIO RIXS measurement, while the Experimental Section states ID20; please reconcile this discrepancy.

Circularity Check

0 steps flagged · score 0.0 of 10

No circularity: central claims rest on direct measurements and independent cross-compound inputs.

full rationale

The paper's derivation chain is self-contained and does not reduce any predicted quantity to a fitted input. The central experimental claims—insulating transport, absence of density of states at the Fermi level, and absence of spontaneous magnetization (Arrott plot)—are direct measurements independent of any model. The magnetic assignment for PMIO is cross-validated by a genuine external input: the Ir4+ effective moment (1.36 μB) is taken from a separately measured isostructural La2MgIrO6 sample, and the Pr3+ free-ion value (3.58 μB) is taken from literature; their combination (Eq. 2) predicts 5.24 μB/f.u, which is then compared with the measured Curie-Weiss value of ~5.2 μB/f.u. The same independent inputs give 4.49 μB/f.u versus the fitted 4.5 μB/f.u for PSMIO1505 (Eqs. 3–5). For PSMIO, the excess ~0.3 μB/f.u over the Pr3+ value is a residual of the Curie-Weiss fit, and the inference of a small Ir5+ moment is corroborated by high-resolution RIXS showing low-energy magnetic excitations, not by circular reuse of the fit. The 'Pr3+ only paramagnetic background' conclusion is supported by the non-Kramer singlet crystal-field argument cited from external literature (refs 39–42) and by the absence of additional susceptibility anomalies, rather than by the moment-balance calculation itself. No self-citation is load-bearing: refs 10 and 15 from the same group are used as comparative spectroscopy and interpretive support, but the HMAFM refutation and the AFM transition assignments stand on the measured resistivity, XPS valence band, magnetization, XANES, EXAFS, and RIXS data presented in this paper. The paper also explicitly acknowledges that full multiplet calculations would be required for quantitative SOC estimation (Sec. III G), which is a stated limitation, not a circular step. Thus no step satisfies the standard of Eq. X = Eq. Y by construction or a fitted parameter renamed as prediction.

Assumptions & free parameters 4 free parameters · 3 assumptions · 0 invented entities

The paper introduces no new entities. The central interpretive load falls on three external inputs: the single-ion singlet picture for Pr3+, the transferability of the Ir4+ moment from LMIO, and the defect-sensitivity of XANES/XPS. The Curie-Weiss moments are the primary fitted quantities on which the conclusions rest.

free parameters (4)
  • Curie-Weiss effective moment of PMIO = 5.2 muB/f.u (Theta_CW = -36.3 K)
    Fitted to chi(T) in the 100-300 K range; central to the paramagnetic Pr3+ plus Ir4+ moment balance.
  • Curie-Weiss effective moment of PSMIO1505 = 4.5 muB/f.u (Theta_CW = -38.5 K)
    Fitted to chi(T) in the 100-300 K range; used to argue that Pr3+ plus half the Ir4+ moment account for the measured value.
  • Curie-Weiss effective moment of PSMIO = 3.89 muB/f.u (Theta_CW = -38.6 K)
    Fitted to chi(T) in the 150-300 K range; the excess over 3.58 muB per Pr3+ is the basis for the finite Ir5+ moment claim.
  • Curie-Weiss effective moment of LMIO = 1.36 muB/Ir4+
    Obtained from the authors' own Curie-Weiss fit on La2MgIrO6 and used as the Ir4+ moment input for PMIO and PSMIO1505 calculations.
assumptions (3)
  • domain assumption Non-Kramer Pr3+ in a low-symmetry crystal field has a singlet ground state and does not magnetically order or couple to B-site moments.
    Invoked in Section III F to exclude Pr contribution to ordered magnetism; based on references 39-42, not independently measured in this work.
  • domain assumption The Ir4+ magnetic moment measured in La2MgIrO6 can be transferred to Pr2MgIrO6 and Pr1.5Sr0.5MgIrO6 without correction.
    Justified by similar lattice constants and oxidation state; any difference in Ir-O-Ir exchange or crystal field would change the calculated mu_eff.
  • domain assumption Ir L3 XANES and Ir 4f XPS peak fitting can rule out a few percent of magnetic Ir4+ or Ir6+ defects in PrSrMgIrO6.
    Used to rule out an impurity-defect origin of the excess moment; the sensitivity of these probes to few-percent defects is stated, not demonstrated.

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Pith. "Pith review of Evolution of electronic and magnetic properties in a series of iridate double perovskites Pr$_{2-x}$Sr$_x$MgIrO$_6$ ($x$ = 0, 0.5, 1.0)." pith.science (2026). https://pith.science/paper/PU4W2QKF

@misc{pith2026190805973,
  author       = {Pith},
  title        = {Pith review of: Evolution of electronic and magnetic properties in a series of iridate double perovskites Pr$_2-x$Sr$_x$MgIrO$_6$ ($x$ = 0, 0.5, 1.0)},
  year         = {2026},
  howpublished = {\url{https://pith.science/paper/PU4W2QKF}},
  note         = {Machine review of arXiv:1908.05973}
}
abstract

Spin-orbit coupling (SOC) plays a crucial role in magnetic and electronic properties of 5$d$ iridates. In this paper we have experimentally investigated the structural and physical properties of a series of Ir-based double perovskite compounds Pr$_{2-x}$Sr$_x$MgIrO$_6$ ($x$ = 0, 0.5, 1; hereafter abbreviated as PMIO, PSMIO1505, and PSMIO). Interestingly, these compounds have recently been proposed to undergo a transition from the spin-orbit-coupled Mott insulating phase at $x$ = 0 to the elusive half-metallic antiferromagnetic (HMAFM) state with Sr doping at $x$ = 1. However, our detailed magnetic and electrical measurements refute any kind of HMAFM possibility in either of the doped samples. In addition, we establish that within these Pr$_{2-x}$Sr$_x$MgIrO$_6$ double perovskites, changes in Ir-oxidation states (4+ for PMIO to 5+ for PSMIO via mixed 4+/5+ for PSMIO1505) lead to markedly different magnetic behaviors. While SOC on Ir is at the root of the observed insulating behaviors for all three samples, the correlated magnetic properties of these three compounds develop entirely due to the contribution from local Ir moments. Additionally, the magnetic Pr$^{3+}$ (4$f^2$) ions, instead of showing any kind of ordering, only contribute to the total paramagnetic moment. It is seen that the PrSrMgIrO$_6$ sample does not order down to 2 K despite antiferromagnetic interactions. But, the $d^5$ iridate Pr$_2$MgIrO$_6$ shows a sharp antiferromagnetic (AFM) transition at around 14 K, and in the mixed valent Pr$_{1.5}$Sr$_{0.5}$MgIrO$_6$ sample the AFM transition is shifted to a much lower temperature ($\sim$ 6 K) due to weakening of the AFM exchange.

Figures

Figures reproduced from arXiv: 1908.05973 by the authors.

Figure 1
Figure 1. FIG. 1. (color online) Redistribution of [PITH_FULL_IMAGE:figures/full_fig_p019_1.png] view at source ↗
Figure 2
Figure 2. FIG. 2. (color online) (a) Rietveld refined XRD patterns of al [PITH_FULL_IMAGE:figures/full_fig_p021_2.png] view at source ↗
Figure 3
Figure 3. FIG. 3. (colour online) Ir [PITH_FULL_IMAGE:figures/full_fig_p021_3.png] view at source ↗
Figures from the paper (4 more)
Figure 4
Figure 4. Figure 4: FIG. 4. (colour online) (a) Ir [PITH_FULL_IMAGE:figures/full_fig_p021_4.png]
Figure 5
Figure 5. Figure 5: FIG. 5. (colour online) (a)-(c) Low-resolution high-energ [PITH_FULL_IMAGE:figures/full_fig_p021_5.png]
Figure 7
Figure 7. Figure 7: FIG. 7. (colour online) Zero Field cooled (open circles) and [PITH_FULL_IMAGE:figures/full_fig_p022_7.png]
Figure 8
Figure 8. Figure 8: FIG. 8. (colour online) (a) High-resolution RIXS spectra at [PITH_FULL_IMAGE:figures/full_fig_p022_8.png]

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Pith tools

Reviewed August 14, 2026 · model on record in the stance chip above.