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Magnetic phase diagram of as explored by neutron scattering
Phys. Rev. B 112, 224441 – Published 24 December, 2025
DOI: https://doi.org/10.1103/m3wx-4v6k
Abstract
The tetragonal -electron intermetallic is characterized by strong Ising anisotropy along the tetragonal axis. The magnetic moments on the erbium sites can be mapped onto a Shastry-Sutherland lattice, resulting in geometrical frustration. At zero magnetic field exhibits collinear columnar antiferromagnetic (CAFM) order below . In the presence of a magnetic field parallel to the axis, exhibits a plateau at of the saturation magnetization , which arises at a spin-flip transition at 1.9 T. Fractional magnetization plateaus and other exotic spin phases are a well-established characteristic feature of frustrated spin systems. Monte Carlo simulations propose that is an ideal candidate to feature a spin supersolid phase in close vicinity of between the CAFM and plateau (HP) phase. Here, we combine single-crystal neutron diffraction and inelastic neutron scattering to study the magnetic phase diagram and the crystal electric-field (CEF) ground state of . Our measurements as a function of magnetic field find no signature of the spin supersolid phase but allow us to determine the magnetic structure of the HP phase to be of the up-up-up-down (uuud) type consistent with an Ising material. The magnetic moment expected from the CEF configuration determined by our inelastic neutron-scattering measurements is also consistent with the ordered moment observed in neutron diffraction, showing that the moments are fully ordered and close to the free ion moment (9.6 ).
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References (57)
- K. Yoshida, Theory of Magnetism, Springer Series in Solid-State Sciences (Springer, Berlin Heidelberg, 1996).
- H. T. Diep, Frustrated Spin Systems (World Scientific, Singapore, 2013).
- C. Lacroix, Frustrated metallic systems: A review of some peculiar behavior, J. Phys. Soc. Jpn. 79, 011008 (2010).
- A. P. Ramirez, A. Hayashi, R. J. Cava, R. Siddharthan, and B. S. Shastry, Zero-point entropy in ‘spin ice', Nature (London) 399, 333 (1999).
- M. J. Harris, S. T. Bramwell, D. F. McMorrow, T. Zeiske, and K. W. Godfrey, Geometrical frustration in the ferromagnetic pyrochlore , Phys. Rev. Lett. 79, 2554 (1997).
- L. Savary and L. Balents, Quantum spin liquids: A review, Rep. Prog. Phys. 80, 016502 (2017).
- A. Banerjee, C. A. Bridges, J.-Q. Yan, A. A. Aczel, L. Li, M. B. Stone, G. E. Granroth, M. D. Lumsden, Y. Yiu, J. Knolle, S. Bhattacharjee, D. L. Kovrizhin, R. Moessner, D. A. Tennant, D. G. Mandrus, and S. E. Nagler, Proximate Kitaev quantum spin liquid behavior in a honeycomb magnet, Nat. Mater. 15, 733 (2016).
- A. Kitaev, in Exact Methods in Low-dimensional Statistical Physics and Quantum Computing, edited by J. Jacobson, S. Ouphry, V. Pasquier, D. Serban, and L. Cugliandolo (Oxford University Press, Oxford, 2008).
- S. Julian and H.-Y. Kee, Frustrated metallic magnets, La Physique au Canada 68, 95 (2012).
- Q. Si and F. Steglich, Heavy fermions and quantum phase transitions, Science 329, 1161 (2010).
- P. Coleman and A. H. Nevidomskyy, Frustration and the Kondo effect in heavy fermion materials, J. Low Temp. Phys. 161, 182 (2010).
- P. Das, S.-Z. Lin, N.J. Ghimire, K. Huang, F. Ronning, E. D. Bauer, J. D. Thompson, C. D Batista, G. Ehlers, and M. Janoschek, Magnitude of the magnetic exchange interaction in the heavy-fermion antiferromagnet , Phys. Rev. Lett. 113, 246403 (2014).
- D. M. Fobes, E. D. Bauer, J. D. Thompson, A. Sazonov, V. Hutanu, S. Zhang, F. Ronning, and M. Janoschek, Low temperature magnetic structure of by neutron diffraction on absorption-optimized samples, J. Phys.: Condens. Matter 29, 17LT01 (2017).
- S. Nakatsuji, Y. Machida, Y. Maeno, T. Tayama, T. Sakakibara, J. van Duijn, L. Balicas, J. N. Millican, R. T. Macaluso, and J. Y. Chan, Metallic spin-liquid behavior of the geometrically frustrated Kondo lattice , Phys. Rev. Lett. 96, 087204 (2006).
- Y. Tokiwa, J. J. Ishikawa, S. Nakatsuji, and P. Gegenwart, Quantum criticality in a metallic spin liquid, Nat. Mater. 13, 356 (2014).
- T. Kurumaji, T. Nakajima, M. Hirschberger, A. Kikkawa, Y. Yamasaki, H. Sagayama, H. Nakao, Y. Taguchi, T. Arima, and Y. Tokura, Skyrmion lattice with a giant topological Hall effect in a frustrated triangular-lattice magnet, Science 365, 914 (2019).
- M. Hirschberger, T. Nakajima, S. Gao, L. Peng, A. Kikkawa, T. Kurumaji, M. Kriener, Y. Yamasaki, H. Sagayama, H. Nakao, K. Ohishi, K. Kakurai, Y. Taguchi, X. Yu, T. Arima, and Y. Tokura, Skyrmion phase and competing magnetic orders on a breathing kagomé lattice, Nat. Commun. 10, 5831 (2019).
- R. Takagi, N. Matsuyama, V. Ukleev, L. Yu, J. S. White, S. Francoual, J. R. L. Mardegan, S. Hayami, H. Saito, K. Kaneko, K. Ohishi, Y. Ōnuki, T. Arima, Y. Tokura, T. Nakajima, and S. Seki, Square and rhombic lattices of magnetic skyrmions in a centrosymmetric binary compound, Nat. Commun. 13, 1472 (2022).
- H. Nakamura, N. Kim, M. Shiga, R. Kmiec, K. Tomala, E. Ressouche, J. P. Sanchez, and B. Malaman, The partially disordered state of the frustrated face-centred cubic antiferromagnet, J. Phys.: Condens. Matter 11, 1095 (1999).
- O. Stockert, J.-U. Hoffmann, M. Mühlbauer, A. Senyshyn, M. M. Koza, A. A. Tsirlin, F. M. Wolf, S. Bachus, P. Gegenwart, R. Movshovich, S. Bobev, and V. Fritsch, Magnetic frustration in a metallic fcc lattice, Phys. Rev. Res. 2, 013183 (2020).
- R. Okuma, C. Ritter, G. J. Nilsen, and Y. Okada, Magnetic frustration in a van der Waals metal CeSiI, Phys. Rev. Mater. 5, L121401 (2021).
- J. Etourneau and P. Hagenmuller, Structure and physical features of the rare-earth borides, Philos. Mag. B 52, 589 (1985).
- B. Sriram Shastry and B. Sutherland, Exact ground state of a quantum mechanical antiferromagnet, Physica B+C 108, 1069 (1981).
- S. Miyahara and K. Ueda, Theory of the orthogonal dimer Heisenberg spin model for , J. Phys.: Condens. Matter 15, R327 (2003).
- Z. Shi, S. Dissanayake, P. Corboz, W. Steinhardt, D. Graf, D. M. Silevitch, H. A. Dabkowska, T. F. Rosenbaum, F. Mila, and S. Haravifard, Discovery of quantum phases in the Shastry-Sutherland compound under extreme conditions of field and pressure, Nat. Commun. 13, 2301 (2022).
- H. Nojiri, H. Kageyama, K. Oniduka, Y. Ueda, and M. Motokawa, Study of spin gap excitations in by submillimeter wave ESR, Phys. B: Condens. Matter 284-288, 1450 (2000).
- W. Schaefer, G. Will, and K. H. J. Buschow, The magnetic structure of the rare earth tetraborides and , J. Chem. Phys. 64, 1994 (1976).
- F. Pfeiffer, W. Schaefer, G. Will, J. Etourneau, and R. Georges, The magnetic phase diagram of , J. Magn. Magn. Mater. 14, 306 (1979).
- L. Ye, T. Suzuki, and J. G. Checkelsky, Electronic transport on the Shastry-Sutherland lattice in Ising-type rare-earth tetraborides, Phys. Rev. B 95, 174405 (2017).
- D. Okuyama, T. Matsumura, T. Mouri, N. Ishikawa, K. Ohoyama, H. Hiraka, H. Nakao, K. Iwasa, and Y. Murakami, Competition of magnetic and quadrupolar order parameters in , J. Phys. Soc. Jpn. 77, 044709 (2008).
- N. Qureshi, F. Bourdarot, E. Ressouche, W. Knafo, F. Iga, S. Michimura, L.-P. Regnault, and F. Duc, Possible stripe phases in the multiple magnetization plateaus in from single-crystal neutron diffraction under pulsed high magnetic fields, Phys. Rev. B 106, 094427 (2022).
- S. Yoshii, K. Ohoyama, K. Kurosawa, H. Nojiri, M. Matsuda, P. Frings, F. Duc, B. Vignolle, G. L. J. A. Rikken, L.-P. Regnault, S. Michimura, and F. Iga, Neutron diffraction study on the multiple magnetization plateaus in under pulsed high magnetic field, Phys. Rev. Lett. 103, 077203 (2009).
- S. Michimura, A. Shigekawa, F. Iga, T. Takabatake, and K. Ohoyama, Complex magnetic structures of a Shastry–Sutherland lattice studied by powder neutron diffraction analysis, J. Phys. Soc. Jpn. 78, 024707 (2009).
- K. Siemensmeyer, E. Wulf, H.-J. Mikeska, K. Flachbart, S. Gabani, S. Matas, P. Priputen, A. Efdokimova, and N. Shitsevalova, Fractional magnetization plateaus and magnetic order in the Shastry-Sutherland magnet , Phys. Rev. Lett. 101, 177201 (2008).
- W. Schaefer, G. Will, and K. H. J. Buschow, The symmetries of magnetic structures in rare earth tetraborides, J. Magn. Magn. Mater. 3, 61 (1976).
- Y. I. Dublenych, Ground states of an Ising model on an extended Shastry-Sutherland lattice and the 1 / 2 -magnetization plateau in some rare-earth-metal tetraborides, Phys. Rev. E 88, 022111 (2013).
- L. Huo, W. C. Huang, Z. B. Yan, X. T. Jia, X. S. Gao, M. H. Qin, and J.-M. Liu, The competing spin orders and fractional magnetization plateaus of the classical Heisenberg model on Shastry-Sutherland lattice: Consequence of long-range interactions, J. Appl. Phys. 113, 073908 (2013).
- M. Moliner, D. C. Cabra, A. Honecker, P. Pujol, and F. Stauffer, Magnetization process in the classical Heisenberg model on the Shastry-Sutherland lattice, Phys. Rev. B 79, 144401 (2009).
- S. Michimura, A. Shigekawa, F. Iga, M. Sera, T. Takabatake, K. Ohoyama, and Y. Okabe, Magnetic frustrations in the Shastry–Sutherland system , Phys. B: Condens. Matter 378-380, 596 (2006).
- K. Wierschem and P. Sengupta, Columnar antiferromagnetic order and spin supersolid phase on the extended Shastry-Sutherland lattice, Phys. Rev. Lett. 110, 207207 (2013).
- D. Brunt, M. Ciomaga Hatnean, O. A. Petrenko, M. R. Lees, and G. Balakrishnan, Single-crystal growth of metallic rare-earth tetraborides by the floating-zone technique, Crystals 9, 211 (2019).
- See Supplemental Material at http://link.aps.org/supplemental/10.1103/m3wx-4v6k for SC-XRD data, which includes Refs. [43, 44].
- X-Area Software Version 2.1, STOE & Cie GmbH, Darmstadt, Germany, https://www.stoe.com/products/xarea/.
- V. Petříček, L. Palatinus, J. Plášil, and M. Dušek, Jana2020– a new version of the crystallographic computing system Jana, Z. Kristallogr. - Cryst. Mater. 238, 271 (2023).
- P. F. S. Rosa and Z. Fisk, Flux methods for growth of intermetallic single crystals, in Crystal Growth of Intermetallics, edited by P. Gille and Y. Grin (De Gruyter, Berlin/Boston, 2019), pp. 49–60.
- N. Qureshi, mag2pol: A program for the analysis of spherical neutron polarimetry, flipping ratio and integrated intensity data, J. Appl. Crystallogr. 52, 175 (2019).
- J. Lass, H. Jacobsen, K. M. L. Krighaar, D. Graf, F. Groitl, F. Herzog, M. Yamada, C. Kägi, R. A. Müller, R. Bürge, M. Schild, M. S. Lehmann, A. Bollhalder, P. Keller, M. Bartkowiak, U. Filges, U. Greuter, G. Theidel, H. M. Ronnow, C. Niedermayer, et al., Commissioning of the novel continuous angle multi-energy analysis spectrometer at the Paul Scherrer Institut, Rev. Sci. Instrum. 94, 023302 (2023).
- J. Lass, H. Jacobsen, D. G. Mazzone, and K. Lefmann, MJOLNIR: A software package for multiplexing neutron spectrometers, SoftwareX 12, 100600 (2020).
- S. Janßen, J. Mesot, L. Holitzner, A. Furrer, and R. Hempelmann, FOCUS: A hybrid TOF-spectrometer at SINQ, Phys. B: Condens. Matter 234-236, 1174 (1997).
- A. Scheie, PyCrystalField: Software for calculation, analysis and fitting of crystal electric field Hamiltonians, J. Appl. Crystallogr. 54, 356 (2021).
- G. Will and W. Schafer, Neutron diffraction and the magnetic structures of some rare earth diborides and tetraborides, J. Less Common Met. 67, 31 (1979).
- G. Will, W. Schäfer, F. Pfeiffer, F. Elf, and J. Etourneau, Neutron diffraction studies of and , J. Less-Common Met. 82, 349 (1981).
- M. Blume, A. J. Freeman, and R. E. Watson, Theory of spin-orbit coupling in atoms. III, Phys. Rev. 134, A320 (1964).
- K. W. H. Stevens, Matrix elements and operator equivalents connected with the magnetic properties of rare earth ions, Proc. Phys. Soc. A 65, 209 (1952).
- Magnetic form factors, https://www.ill.eu/sites/ccsl/ffacts/.
- L. Yadav, A. Rufino, R. Bag, C. d. Cruz, A. I. Kolesnikov, V. O. Garlea, D. Graf, F. Mila, and S. Haravifard, Observation of unprecedented fractional magnetization plateaus in a new Shastry-Sutherland Ising compound (2024), doi: 10.1103/9ynf-xx1t.
- M. S. Song, K. K. Cho, J. W. Lee, and B. K. Cho, Abnormal field-dependence of magnetocaloric effect in and , AIP Adv. 10, 025219 (2020).