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Characterization of the magnetic phase transitions in double perovskite ${Nd}_{2} {NiMnO}_{6}$

John M. Attah-Baah ^1,2, Pascal Manuel³, Dmitry D. Khalyavin³, Nilson S. Ferreira ^1,*, and Roger D. Johnson ^2,4,5,†

¹Department of Physics, Federal University of Sergipe, São Cristovão 49100-000, SE, Brazil
²Department of Physics and Astronomy, University College London, Gower Street, London WC1E 6BT, United Kingdom
³ISIS Pulsed Neutron Source, STFC Rutherford Appleton Laboratory, Didcot, Oxfordshire OX11 0QX, United Kingdom
⁴London Centre for Nanotechnology, University College London, Gordon Street, London WC1H 0AH, United Kingdom
⁵Department of Physics, Durham University, South Road, Durham DH1 3LE, United Kingdom

^*Contact author: nilson@academico.ufs.br
^†Contact author: roger.d.johnson@durham.ac.uk

Phys. Rev. B 112, 184414 – Published 7 November, 2025

DOI: https://doi.org/10.1103/467g-2914

Abstract

Through detailed analysis of neutron powder diffraction data, we confirm that the double perovskite ${Nd}_{2} {NiMnO}_{6}$ adopts a monoclinic $P 2_{1} / n$ structure with nearly complete $B$ -site ordering of ${Ni}^{2 +}$ and ${Mn}^{4 +}$ cations. Below $T_{1} = 198 K$ , magnetic susceptibility measurements and further analysis of neutron diffraction data reveal that the ${Ni}^{2 +}$ and ${Mn}^{4 +}$ sublattices undergo ferromagnetic ordering, as expected of strong $3 d − 3 d$ exchange interactions. Upon cooling through $T_{2} = 22 K$ , a secondary magnetic transition is observed, below which we have discovered an additional noncollinear symmetry-breaking order of ${Nd}^{3 +}$ moments. We argue that the canting of the rare-earth moments naturally arises through the competition of $f − d$ and $f − f$ Heisenberg exchange interactions, which may be finely balanced in the double perovskite framework. Furthermore, the symmetry of the ground state magnetic structure implies significant ${Nd}^{3 +}$ easy plane anisotropy, and an effective decoupling of the antiferromagnetic spin canting from the transition metal sublattice. Between $T_{1}$ and $T_{2}, {Nd}_{2} {NiMnO}_{6}$ shows anomalous behavior in the frequency-dependent ac magnetic susceptibility that is characteristic of reentrant spin-glass-like properties attributed to antisite disorder and competing interactions. Finally, analysis of isothermal magnetization yields magnetic entropy changes that suggest ${Nd}_{2} {NiMnO}_{6}$ and related compounds have potential for magnetic refrigeration, showing a peak in the magnetic entropy change of $2.25 J {kg}^{- 1} K^{- 1}$ at $T_{1}$ under a 7 T field. The scaling behavior of the magnetic entropy, paired with analysis of other critical exponents, shows that the ferromagnetic transition at $T_{1}$ is consistent with a mean-field second-order phase transition. Taken together, our results provide crucial details on the magnetic properties of ${Nd}_{2} {NiMnO}_{6}$ and further consolidate the expectation that double perovskites may serve as model systems for investigating competing magnetic interactions, magnetocaloric effects, and reentrant spin-glass behavior.

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Phys. Rev. B 112, 184414– Published 7 November, 2025

Vol. 112, Iss. 18 — 1 November 2025

Received 27 June 2025
Accepted 22 September 2025

DOI: https://doi.org/10.1103/467g-2914

Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

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Characterization of the magnetic phase transitions in double perovskite ${Nd}_{2} {NiMnO}_{6}$

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Characterization of the magnetic phase transitions in double perovskite Nd2NiMnO6

Abstract

Physics Subject Headings (PhySH)

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References (54)

Characterization of the magnetic phase transitions in double perovskite ${Nd}_{2} {NiMnO}_{6}$