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Anomalous magnetism in the double perovskite oxide with the Kramers ion
Phys. Rev. B 112, 054429 – Published 12 August, 2025
DOI: https://doi.org/10.1103/c87f-xf83
Abstract
The complex magnetic behavior of double-perovskite oxides () with rare-earth (RE) element A and transition metal (TM) elements B- is determined by the interactions between intra- and interatomic magnetic moments. The peculiar magnetism in these systems stems from the interplay between spin, orbit, and lattice degrees of freedom. This study comprehensively investigates the role of spin-orbit entangled moments of the Kramers ion on the magnetic ground state of a B-site ordered ferrimagnetic (FiM) double-perovskite oxide, . Furthermore, employing microscopic techniques like (muon spin rotation and relaxation) and neutron diffraction, we gained insight into the origin of low-temperature anomalies in the magnetic ground state of the system. The DC magnetization data encompass the first transition at critical temperature K, followed by a negative magnetization below 15 K. The temperature-dependent neutron diffraction shows a commensurate magnetic ordering below 250 K, forming a ferrimagnetic ground state, supported by theoretical calculations. In addition, a sharp drop in initial muon asymmetry confirms the transition from a disordered state to a long-range-ordered state at 250 K. Interestingly, the thermal evolution of the dynamic muon spin-relaxation rate () reveals a transition at two temperatures, at 250 K and K, suggesting a low- ordering at the A site. The heat-capacity data show that hosts the ground-state doublet (pseudospin-1/2) at low temperatures. Our analysis of neutron diffraction, heat capacity, and results suggests that the correlation between the doublet and the complex interaction between Nd-TM moments gives rise to the observed low-temperature anomaly.
Physics Subject Headings (PhySH)
Corrections
23 January, 2026
Correction: A missing statement has been added to the Acknowledgment section.
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References (57)
- A. A. Aczel, Q. Chen, J. P. Clancy, C. dela Cruz, D. Reig-i Plessis, G. J. MacDougall, C. J. Pollock, M. H. Upton, T. J. Williams, N. LaManna, J. P. Carlo, J. Beare, G. M. Luke, and H. D. Zhou, Spin-orbit coupling controlled ground states in the double perovskite iridates (; , Phys. Rev. Mater. 6, 094409 (2022).
- O. Mustonen, S. Vasala, E. Sadrollahi, K. P. Schmidt, C. Baines, H. C. Walker, I. Terasaki, F. J. Litterst, E. Baggio-Saitovitch, and M. Karppinen, Spin-liquid-like state in a spin-1/2 square-lattice antiferromagnet perovskite induced by – cation mixing, Nat. Commun. 9, 1085 (2018).
- S. D. Bader and S. S. P. Parkin, Spintronics, Annu. Rev. Condens. Matter Phys. 1, 71 (2010).
- A. Hirohata, K. Yamada, Y. Nakatani, I.-L. Prejbeanu, B. Diény, P. Pirro, and B. Hillebrands, Review on spintronics: Principles and device applications, J. Magn. Magn. Mater. 509, 166711 (2020).
- S. H. Lee, H. C. Choi, and B.-J. Yang, Odd-parity spin-triplet superconductivity in centrosymmetric antiferromagnetic metals, Phys. Rev. Lett. 126, 067001 (2021).
- M. P. Ghimire, L.-H. Wu, and X. Hu, Possible half-metallic antiferromagnetism in an iridium double-perovskite material, Phys. Rev. B 93, 134421 (2016).
- K.-I. Kobayashi, T. Kimura, H. Sawada, K. Terakura, and Y. Tokura, Room-temperature magnetoresistance in an oxide material with an ordered double-perovskite structure, Nature (London) 395, 677 (1998).
- B. Singh, D. Kumar, V. Kumar, M. Vogl, S. Wurmehl, S. Aswartham, B. Büchner, and P. Kumar, Fractional spin fluctuations and quantum liquid signature in , Phys. Rev. B 104, 134402 (2021).
- A. Harbi, Y. L. E. Godec, H. Moutaabbid, S. Benmokhtar, and M. Moutaabbid, Tailoring the Griffiths-like cluster formation in the insulator ferromagnet spin-glass double perovskite, Phys. Rev. B 104, 054404 (2021).
- P. C. Rout and U. Schwingenschlögl, Strain-attenuated spin frustration in double perovskite , Phys. Rev. B 103, 024426 (2021).
- H. Wang, S. Zhu, X. Ou, and H. Wu, Ferrimagnetism in the double perovskite : A density functional study, Phys. Rev. B 90, 054406 (2014).
- M. Sikora, O. Mathon, P. Van der Linden, J. M. Michalik, J. M. De. Teresa, C. Kapusta, and S. Pascarelli, Field-induced magnetostructural phase transition in double perovskite studied via x-ray magnetic circular dichroism, Phys. Rev. B 79, 220402(R) (2009).
- H. Mutch, O. Mustonen, H. C. Walker, P. J. Baker, G. B. G. Stenning, F. C. Coomer, and E. J. Cussen, Long-and short-range magnetism in the frustrated double perovskite , Phys. Rev. Mater. 4, 014408 (2020).
- G. J. Nilsen, C. M. Thompson, C. Marjerisson, D. I. Badrtdinov, A. A. Tsirlin, and J. E. Greedan, Magnetic order and multipoles in the rhenium double perovskite , Phys. Rev. B 103, 104430 (2021).
- S. Blundell, Magnetism in Condensed Matter (Oxford University Press, Oxford, 2001).
- X. Chen, J. Xu, Y. Xu, F. Luo, and Y. Du, Rare earth double perovskites: A fertile soil in the field of perovskite oxides, Inorg. Chem. Front. 6, 2226 (2019).
- F.-Y. Li, Y.-D. Li, Y. Yu, A. Paramekanti, and G. Chen, Kitaev materials beyond iridates: Order by quantum disorder and Weyl magnons in rare-earth double perovskites, Phys. Rev. B 95, 085132 (2017).
- D. T. Adroja, Shivani Sharma, C. Ritter, A. D. Hillier, Duc Le, C. V. Tomy, R. Singh, R. I. Smith, M. Koza, A. Sundaresan et al., Muon spin rotation and neutron scattering investigations of the -site ordered double perovskite , Phys. Rev. B 101, 094413 (2020).
- A. A. Aczel, D. E. Bugaris, J. Yeon, C. de la Cruz, H.-C. zur Loye, and S. E. Nagler, Coupled Nd and spin ordering in the double perovskites (), Phys. Rev. B 88, 014413 (2013).
- T. Ferreira, S. Calder, D. S. Parker, M. H. Upton, A. S. Sefat, and H.-C. zur Loye, Relationship between A-site cation and magnetic structure in double perovskite iridates (), Phys. Rev. Mater. 5, 064408 (2021).
- J. Sánchez-Benítez, M. J. Martínez-Lope, J. A. Alonso, and J. L. García-Muñoz, Magnetic and structural features of the perovskite series investigated by neutron diffraction, J. Phys.: Condens. Matter 23, 226001 (2011).
- S. Pal, S. Jana, S. Govinda, B. Pal, S. Mukherjee, S. Keshavarz, D. Thonig, Y. Kvashnin, M. Pereiro, R. Mathieu, P. Nordblad, J. W. Freeland, O. Eriksson, O. Karis, and D. D. Sarma, Peculiar magnetic states in the double perovskite , Phys. Rev. B 100, 045122 (2019).
- C. Ritter, S. Sharma, and D. T. Adroja, Magnetic structures of the iridium-based double perovskites and reinvestigated using neutron diffraction, Phys. Rev. Mater. 6, 084405 (2022).
- M. Sun, Y. Xuan, G. Liu, Y. Liu, F. Zhang, J. Ren, and M. Chen, Anomalous magnetic behaviors of double perovskite (R = rare earth elements) predicted by first-principles calculations, J. Magn. Magn. Mater. 504, 166670 (2020).
- J. Rodriguez-Carvajal, Fullprof: a program for Rietveld refinement and pattern matching analysis, in Satellite Meeting on Powder Diffraction of the XV Congress of the IUCr, Toulouse, France (Scientific Research Publishing Inc., 1990), Vol. 127.
- R. Delhez and E. J. Mittemeijer, Winplotr: A windows tool for powder diffraction pattern analysis, Mater. Sci. Forum 378, 118 (2001).
- A. Suter and B. M. Wojek, Musrfit: A free platform-independent framework for data analysis, Phys. Procedia 30, 69 (2012).
- G. Kresse and D. Joubert, From ultrasoft pseudopotentials to the projector augmented-wave method, Phys. Rev. B 59, 1758 (1999).
- P. E. Blöchl, Projector augmented-wave method, Phys. Rev. B 50, 17953 (1994).
- G. Kresse and J. Furthmüller, Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set, Phys. Rev. B 54, 11169 (1996).
- John P. Perdew, K. Burke, and M. Ernzerhof, Generalized gradient approximation made simple, Phys. Rev. Lett. 77, 3865 (1996).
- S. L. Dudarev, G. A. Botton, S. Y. Savrasov, C. J. Humphreys, and A. P. Sutton, Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA + U study, Phys. Rev. B 57, 1505 (1998).
- M. T. Anderson, K. B. Greenwood, G. A. Taylor, and K. R. Poeppelmeier, B-cation arrangements in double perovskites, Prog. Solid State Chem. 22, 197 (1993).
- See Supplemental Material at http://link.aps.org/supplemental/10.1103/c87f-xf83 for anomalous magnetism in the double perovskite oxide with the Kramers ion .
- M. A. Islam, T. Sato, F. Ara, and M. A. Basith, Sol-gel based synthesis to explore structure, magnetic and optical properties of double perovskite nanoparticles, J. Alloys Compd. 944, 169066 (2023).
- S. Sharma, D. T. Adroja, C. Ritter, D. Khalyavin, P. Manuel, G. B. G. Stenning, A. Sundaresan, A. D. Hillier, P. P. Deen, D. I. Khomskii, and S. Langridge, Magnetic ground state of the ordered double-perovskite : Two magnetic transitions, Phys. Rev. B 102, 134412 (2020).
- W. Schnelle, J. Engelhardt, and E. Gmelin, Specific heat capacity of Apiezon N high vacuum grease and of Duran borosilicate glass, Cryogenics 39, 271 (1999).
- Z. Jirák, J. Hejtmánek, K. Knížek, P. Novák, E. Šantavá, and H. Fujishiro, Magnetism of perovskite cobaltites with Kramers rare-earth ions, J. Appl. Phys. 115, 17E118 (2014).
- A. Singh, S. Rajput, P. Balasubramanian, M. Anas, F. Damay, C. M. N. Kumar, G. Eguchi, A. Jain, S. M. Yusuf, T. Maitra, and V. K. Malik, Successive spin reorientations and rare earth ordering in : Experimental and ab initio investigations, Phys. Rev. B 102, 144432 (2020).
- J. Rodríguez-Carvajal, BasIreps: A Program for Calculating Irreducible Representations of Little Groups and Basis Functions of Polar and Axial Vector Properties. Part of the FullProf Suite of Programs (Institut Laue-Langevin, 2010), http://www.ill.eu/sites/fullprof/.
- M. D. I. Bhuyan, R. Hossain, F. Ara, and M. A. Basith, A first-principles study on the phase stability and physical properties of a B-site ordered double perovskite, Phys. Chem. Chem. Phys. 24, 1569 (2022).
- H. M. Rietveld, A profile refinement method for nuclear and magnetic structures, J. Appl. Crystallogr. 2, 65 (1969).
- H. Guo, C. Ritter, Y. Su, A. C. Komarek, and J. S. Gardner, Distinct magnetic ground states of (R = ) determined by neutron powder diffraction, Phys. Rev. B 103, L060402 (2021).
- G. Sala, M. B. Stone, B. K. Rai, A. F. May, C. R. DelaCruz, H. SuriyaArachchige, G. Ehlers, V. R. Fanelli, V. O. Garlea, M. D. Lumsden, D. Mandrus, and A. D. Christianson, Physical properties of the trigonal binary compound , Phys. Rev. Mater. 2, 114407 (2018).
- A. D. Hillier, S. J. Blundell, I. McKenzie, I. Umegaki, L. Shu, J. A. Wright, T. Prokscha, F. Bert, K. Shimomura, A. Berlie, H. Alberto, and I. Watanabe, Muon spin spectroscopy, Nat. Rev. Methods Primers 2, 4 (2022).
- M. G. Flokstra, S. J. Ray, S. J. Lister, J. Aarts, H. Luetkens, T. Prokscha, A. Suter, E. Morenzoni, and S. L. Lee, Measurement of the spatial extent of inverse proximity in a Py/Nb/Py superconducting trilayer using low-energy muon-spin rotation, Phys. Rev. B 89, 054510 (2014).
- S. J. Ray, A. S. Gibbs, S. J. Bending, P. J. Curran, E. Babaev, C. Baines, A. P. Mackenzie, and S. L. Lee, Muon-spin rotation measurements of the vortex state in : Type-1.5 superconductivity, vortex clustering, and a crossover from a triangular to a square vortex lattice, Phys. Rev. B 89, 094504 (2014).
- D. O. G. Heron, S. J. Ray, S. J. Lister, C. M. Aegerter, H. Keller, P. H. Kes, G. I. Menon, and S. L. Lee, Muon-spin rotation measurements of an unusual vortex-glass phase in the layered superconductor , Phys. Rev. Lett. 110, 107004 (2013).
- R. Khasanov, T. Kondo, M. Bendele, Y. Hamaya, A. Kaminski, S. L. Lee, S. J. Ray, and T. Takeuchi, Suppression of the antinodal coherence of superconducting as revealed by muon spin rotation and angle-resolved photoemission, Phys. Rev. B 82, 020511(R) (2010).
- X. Y. Zhu, H. Zhang, D. J. Gawryluk, Z. X. Zhen, B. C. Yu, S. L. Ju, W. Xie, D. M. Jiang, W. J. Cheng, Y. Xu, M. Shi, E. Pomjakushina, Q. F. Zhan, T. Shiroka, and T. Shang, Spin order and fluctuations in the and topological antiferromagnets: A study, Phys. Rev. B 105, 014423 (2022).
- P. D. De Réotier and A. Yaouanc, Muon spin rotation and relaxation in magnetic materials, J. Phys.: Condens. Matter 9, 9113 (1997).
- R. Pelka, P. Konieczny, M. Fitta, M. Czapla, P. M. Zielinski, M. Bałanda, T. Wasiutyński, Y. Miyazaki, A. Inaba, D. Pinkowicz, B. Sieklucka, Magnetic systems at criticality: Different signatures of scaling, Acta Phys. Pol. A 124, 977 (2013).
- J. I. Pankove, Optical Processes in Semiconductors (Courier Corporation, 1975).
- B. Singh, M. Vogl, S. Wurmehl, S. Aswartham, B. Büchner, and P. Kumar, Kramers doublets, phonons, crystal-field excitations, and their coupling in , Phys. Rev. Res. 2, 023162 (2020).
- M. Watahiki, K. Tomiyasu, K. Matsuhira, K. Iwasa, M. Yokoyama, S. Takagi, M. Wakeshima, and Y. Hinatsu, Crystalline electric field study in the pyrochlore with metal-insulator transition, J. Phys.: Conf. Ser. 320, 012080 (2011).
- H. Guo, C. Ritter, and A. C. Komarek, Direct determination of the spin structure of by means of neutron diffraction, Phys. Rev. B 94, 161102(R) (2016).
- H. Guo, K. Matsuhira, I. Kawasaki, M. Wakeshima, Y. Hinatsu, I. Watanabe, and Z.-A. Xu, Magnetic order in the pyrochlore iridate probed by muon spin relaxation, Phys. Rev. B 88, 060411(R) (2013).