- Open Access
Three-Dimensional XY Universality and Nonlinear Magnetic Susceptibility in a Kagome Ice Compound
Phys. Rev. X 16, 021043 – Published 26 May, 2026
DOI: https://doi.org/10.1103/xl5f-zj9p
Abstract
Kagome spin ice is an intriguing class of spin systems constituted by in-plane Ising spins with ferromagnetic interaction residing on the kagome lattice, theoretically predicted to host a plethora of magnetic transitions and excitations. In particular, different variants of kagome spin ice models can exhibit different sequences of symmetry breaking upon cooling from the paramagnetic to the fully ordered ground state. Recently, it has been demonstrated that the frustrated intermetallic HoAgGe stands as a faithful solid-state realization of kagome spin ice. However, whether any of the established symmetry-breaking pathways apply to this material remains unaddressed. Here, we use single-crystal neutron diffuse scattering to map the spin ordering of HoAgGe at various temperatures more accurately; surprisingly, we find that the ordering sequence appears to be different from previously known scenarios: From the paramagnetic state, the system first enters a partially ordered state with fluctuating magnetic charges, in contrast to a charge-ordered paramagnetic phase, before reaching the fully ordered state. Through Monte Carlo simulations and scaling analyses using an extended three-dimensional (3D) spin model for the distorted kagome spin ice in HoAgGe, we elucidate a single 3D XY phase transition into the ground state with broken time-reversal symmetry (TRS). However, the 3D XY transition has a long crossover tail before the fluctuating magnetic charges fully order. More interestingly, we find, both experimentally and theoretically, that the TRS-breaking phase of HoAgGe features an unusual, hysteretic response: Despite their vanishing magnetization, the two time-reversal partners are distinguished and selected by a nonlinear magnetic susceptibility tied to the kagome ice rule. Our discovery not only unveils a new symmetry-breaking hierarchy of kagome spin ice but also demonstrates the potential of TRS-breaking frustrated spin systems for information technology applications.
Physics Subject Headings (PhySH)
- Critical phenomena
- Magnetic phase transitions
- Quantum phase transitions
- Spin dynamics
- Thermal expansion
- Chiral magnets
- Noncollinear magnets
- Rare-earth magnetic materials
- Strongly correlated systems
- Ising model
- Monte Carlo methods
- Quasi elastic neutron scattering
- Specific heat measurements
- Susceptibility measurements
- XY model
Popular Summary
Identifying the nature of symmetry breaking in frustrated magnets is a significant challenge because unconventional states, such as those governed by local ice rules, often lack a net magnetization. We addressed this by investigating the kagome spin-ice compound HoAgGe and demonstrating that nonlinear magnetic susceptibility can detect time-reversal-symmetry breaking even in the absence of a macroscopic magnetic moment. Our study, which combined neutron scattering, thermodynamic measurements, and large-scale Monte Carlo simulations, revealed that the transition into the ordered phase belongs to the three-dimensional XY universality class. We found that this represents a previously unexplored ordering pathway for quasi-two-dimensional systems realized in actual solids. These results provide an experimental probe for hidden magnetic order and establish a framework for understanding critical behavior in a wide range of kagome spin-ice materials. Our work advances the general understanding of spin-ice physics and offers a versatile method for probing frustrated magnetic systems.
Article Text
References (92)
- L. Balents, Spin liquids in frustrated magnets, Nature (London) 464, 199 (2010).
- C. Broholm, R. J. Cava, S. A. Kivelson, D. G. Nocera, M. R. Norman, and T. Senthil, Quantum spin liquids, Science 367, eaay0668 (2020).
- 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).
- A. P. Ramirez et al., Zero-point entropy in ‘spin ice’, Nature (London) 399, 333 (1999).
- S. T. Bramwell and M. J. P. Gingras, Spin ice state in frustrated magnetic pyrochlore materials, Science 294, 1495 (2001).
- C. Castelnovo, R. Moessner, and S. L. Sondhi, Magnetic monopoles in spin ice, Nature (London) 451, 42 (2008).
- L. Pauling, The structure and entropy of ice and of other crystals with some randomness of atomic arrangement, J. Am. Chem. Soc. 57, 2680 (1935).
- D. J. P. Morris et al., Dirac strings and magnetic monopoles in the spin ice , Science 326, 411 (2009).
- T. Fennell et al., Magnetic Coulomb phase in the spin ice , Science 326, 415 (2009).
- M. Wolf and K. D. Schotte, Ising model with competing next-nearest-neighbour interactions on the Kagome lattice, J. Phys. A 21, 2195 (1988).
- T. Takagi and M. Mekata, Magnetic ordering of Ising spins on kagomé lattice with the 1st and the 2nd neighbor interactions, J. Phys. Soc. Jpn. 62, 3943 (1993).
- A. S. Wills, R. Ballou, and C. Lacroix, Model of localized highly frustrated ferromagnetism: The kagomé spin ice, Phys. Rev. B 66, 144407 (2002).
- G. Möller and R. Moessner, Magnetic multipole analysis of kagome and artificial spin-ice dipolar arrays, Phys. Rev. B 80, 140409(R) (2009).
- G.-W. Chern, P. Mellado, and O. Tchernyshyov, Two-stage ordering of spins in dipolar spin ice on the kagome lattice, Phys. Rev. Lett. 106, 207202 (2011).
- G.-W. Chern and O. Tchernyshyov, Magnetic charge and ordering in kagome spin ice, Phil. Trans. R. Soc. A 370, 5718 (2012).
- K. Zhao et al., Realization of the kagome spin ice state in a frustrated intermetallic compound, Science 367, 1218 (2020).
- K. Zhao et al., Discrete degeneracies distinguished by the anomalous Hall effect in a metallic kagome ice compound, Nat. Phys. 20, 442 (2024).
- L. Anghinolfi et al., Thermodynamic phase transitions in a frustrated magnetic metamaterial, Nat. Commun. 6, 8278 (2015).
- Benjamin Canals et al., Fragmentation of magnetism in artificial kagome dipolar spin ice, Nat. Commun. 7, 11446 (2016).
- M. E. Brooks-Bartlett, S. T. Banks, L. D. C. Jaubert, A. Harman Clarke, and P. C. W. Holdsworth, Magnetic-moment fragmentation and monopole crystallization, Phys. Rev. X 4, 011007 (2014).
- Yao Wang, Stephan Humeniuk, and Yuan Wan, Tuning the two-step melting of magnetic order in a dipolar kagome spin ice by quantum fluctuations, Phys. Rev. B 101, 134414 (2020).
- Wen-Yu Su, Feng Hu, Chen Cheng, and Nvsen Ma, Berezinskii-Kosterlitz-Thouless phase transitions in a kagome spin ice by a quantifying Monte Carlo process: Distribution of Hamming distances, Phys. Rev. B 108, 134422 (2023).
- Eric C. Andrade and Matthias Vojta, Partial magnetic order in kagome spin ice, Phys. Rev. B 109, L241102 (2024).
- N. Li et al., Low-temperature transport properties of the intermetallic compound HoAgGe with a kagome spin-ice state, Phys. Rev. B 106, 014416 (2022).
- S. Roychowdhury et al., Enhancement of the anomalous Hall effect by distorting the Kagome lattice in an antiferromagnetic material, Proc. Natl. Acad. Sci. U.S.A. 121, 01970 (2024).
- H. B. Deng et al., Local excitation of kagome spin ice magnetism seen by scanning tunneling microscopy, Phys. Rev. Lett. 133, 046503 (2024).
- Hari Bhandari et al., Tunable topological transitions in the frustrated magnet , Commun. Mater. 6, 52 (2025).
- S. Wu, L. Zhao, W. Song, M. Tan, F. Jin, T. Ying, J. X. Yin, and Q. Zhang, Lattice dynamics and spin-phonon coupling in the kagome spin ice HoAgGe, Phys. Rev. B 111, 125116 (2025).
- F. Schilberth et al., Large magnetoreflectance and optical anisotropy due to flat bands in the frustrated kagome magnet HoAgGe, arXiv:2504.10274.
- G. F. Schwertfeger, P. H. Chang, P. Nikolic, and I. I. Mazin, Modeling of a twisted kagome spin ice using reduced configuration space search and density functional theory, Phys. Rev. B 112, 214411 (2025).
- Jiyuan Li et al., Complex magnetic phase diagram of the metallic kagome ice , Phys. Rev. B 112, 224426 (2025).
- Y. Tabata, H. Kadowaki, K. Matsuhira, Z. Hiroi, N. Aso, E. Ressouche, and B. Fak, kagomé ice state in the dipolar spin ice , Phys. Rev. Lett. 97, 257205 (2006).
- T. Fennell et al., Pinch points and Kasteleyn transitions in kagome ice, Nat. Phys. 3, 566 (2007).
- A. A. Turrini, A. Harman Clarke, G. Haeseler, T. Fennell, I. G. Wood, P. Henelius, S. T. Bramwell, and P. C. W. Holdsworth, Tunable critical correlations in kagome ice, Phys. Rev. B 105, 094403 (2022).
- Y. Qi, T. Brintlinger, and J. Cumings, Direct observation of the ice rule in an artificial kagome spin ice, Phys. Rev. B 77, 094418 (2008).
- E. Mengotti et al., Real-space observation of emergent magnetic monopoles and associated Dirac strings in artificial kagome spin ice, Nat. Phys. 7, 68 (2011).
- C. Nisoli, R. Moessner, and P. Schiffer, Colloquium: Artificial spin ice: Designing and imaging magnetic frustration, Rev. Mod. Phys. 85, 1473 (2013).
- R. Shindou and N. Nagaosa, Orbital ferromagnetism and anomalous Hall effect in antiferromagnets on the distorted fcc lattice, Phys. Rev. Lett. 87, 116801 (2001).
- Y. Taguchi et al., Spin chirality, Berry phase, and anomalous hall effect in a frustrated ferromagnet, Science 291, 2573 (2001).
- Y. Machida et al., Time-reversal symmetry breaking and spontaneous Hall effect without magnetic dipole orderm, Nature (London) 463, 210 (2010).
- H. Chen, Q. Niu, and A. H. MacDonald, Anomalous Hall effect arising from noncollinear antiferromagnetism, Phys. Rev. Lett. 112, 017205 (2014).
- S. Nakatsuji et al., Large anomalous Hall effect in a non-collinear antiferromagnet at room temperature, Nature (London) 527, 212 (2015).
- Z. Q. Liu et al., Electrical switching of the topological anomalous Hall effect in a non-collinear antiferromagnet above room temperature, Natl. Electron. Rev. 1, 172 (2018).
- K. Zhao, T. Hajiri, H. Chen, R. Miki, H. Asano, and P. Gegenwart, Anomalous Hall effect in the noncollinear antiferromagnetic antiperovskite , Phys. Rev. B 100, 045109 (2019).
- H. Chen, Electronic chiralization as an indicator of the anomalous Hall effect in unconventional magnetic systems, Phys. Rev. B 106, 024421 (2022).
- R. R. Birss and J. C. Anderson, Linear magnetostriction in antiferromagnetics, Proc. Phys. Soc. London 81, 1139 (1963).
- G. Gorodetsky, B. Sharon, and S. Shtrikman, Linear effect of the magnetic field on the magnetic susceptibility in antiferromagnetic , Solid State Commun. 5, 739 (1967).
- M. Blume, L. M. Corliss, J. M. Hastings, and E. Schiller, Observation of an antiferromagnet in an induced staggered magnetic field: Dysprosium aluminum garnet near the tricritical point, Phys. Rev. Lett. 32, 544 (1974).
- J. F. Dillon, E. Y. Chen, N. Giordano, and W. P. Wolf, Time-reversed antiferromagnetic states in dysprosium aluminum garnet, Phys. Rev. Lett. 33, 98 (1974).
- R. Alben, M. Blume, L. M. Corliss, and J. M. Hastings, Induced staggered magnetic fields in antiferromagnets, Phys. Rev. B 11, 295 (1975).
- N. Giordano and W. P. Wolf, Induced staggered magnetic fields in antiferromagnets: Microscopic mechanisms, Phys. Rev. B 21, 2008 (1980).
- W. Wolf, Induced staggered field effects in antiferromagnets, J. Magn. Magn. Mater. 90–91, 197 (1990).
- T. C. Fujita, Y. Kozuka, M. Uchida, A. Tsukazaki, T. Arima, and M. Kawasaki, Odd-parity magnetoresistance in pyrochlore iridate thin films with broken time-reversal symmetry, Sci. Rep. 5, 9711 (2015).
- Tian Liang, Timothy H. Hsieh, Jun J. Ishikawa, Satoru Nakatsuji, Liang Fu, and N. P. Ong, Orthogonal magnetization and symmetry breaking in pyrochlore iridate , Nat. Phys. 13, 599 (2017).
- Yilin Wang, Hongming Weng, Liang Fu, and Xi Dai, Noncollinear magnetic structure, and multipolar order in , Phys. Rev. Lett. 119, 187203 (2017).
- E. Lhotel et al., Evidence for dynamic kagome ice. Nat. Commun. 9, 3786 (2018).
- J. Xu et al., Anisotropic exchange Hamiltonian, magnetic phase diagram, and domain inversion of , Phys. Rev. B 99, 144420 (2019).
- Aloysius P. Gottlob and Martin Hasenbusch, Critical behaviour of the 3D XY-model: A Monte Carlo study, Physica (Amsterdam) 201A, 593 (1993).
- Seiji Miyashita, Nature of the ordered phase, and the critical properties of the three dimensional six-state clock model, J. Phys. Soc. Jpn. 66, 3411 (1997).
- J. Lou, A. W. Sandvik, and L. Balents, Emergence of U(1) symmetry in the 3D model with anisotropy, Phys. Rev. Lett. 99, 207203 (2007).
- M. E. Fisher, Renormalization Group in Critical Phenomena, and Quantum Field Theory, edited by J. Gunton and M. S. Green (Temple University, Philadelphia, 1975).
- D. R. Nelson, Coexistence-curve singularities in isotropic ferromagnets, Phys. Rev. B 13, 2222 (1976).
- D. J. Amit and L. Peliti, On dangerously irrelevant operators, Ann. Phys. (N.Y.) 140, 207 (1982).
- H. Shao, W. Guo, and A. W. Sandvik, Monte Carlo renormalization flows in the space of relevant and irrelevant operators: Application to three-dimensional clock models, Phys. Rev. Lett. 124, 080602 (2020).
- Samuel V. Gallego, Jesus Etxebarria, Luis Elcoro, Emre S. Tasci, and J. Manuel Perez-Mato, Automatic calculation of symmetry-adapted tensors in magnetic and non-magnetic materials: A new tool of the bilbao crystallographic server, Acta Crystallogr. Sect. A 75, 438 (2019).
- Mois Ilia Aroyo, Juan Manuel Perez-Mato, Cesar Capillas, Eli Kroumova, Svetoslav Ivantchev, Gotzon Madariaga, Asen Kirov, and Hans Wondratschek, Bilbao crystallographic server: I. databases, and crystallographic computing programs, Z. Kristallogr.-Cryst. Mater. 221, 15 (2006).
- Mois I. Aroyo, Asen Kirov, Cesar Capillas, J. M. Perez-Mato, and Hans Wondratschek, Bilbao crystallographic server. ii. representations of crystallographic point groups and space groups, Acta Crystallogr. Sect. A 62, 115 (2006).
- S. Lucas et al., Entropy evolution in the magnetic phases of partially frustrated , Phys. Rev. Lett. 118, 107204 (2017).
- G. M. Schmiedeshoff et al., Multiple regions of quantum criticality in , Phys. Rev. B 83, 180408(R) (2011).
- J. F. Allen and A. D. Misener, Flow of liquid helium II, Nature (London) 141, 75 (1938).
- P. Kapitza, Viscosity of liquid helium below the λ-point, Nature (London) 141, 74 (1938).
- J. A. Lipa, D. R. Swanson, J. A. Nissen, T. C. P. Chui, and U. E. Israelsson, Heat capacity and thermal relaxation of bulk helium very near the lambda point, Phys. Rev. Lett. 76, 944 (1996).
- J. A. Lipa, J. A. Nissen, D. A. Stricker, D. R. Swanson, and T. C. P. Chui, Specific heat of liquid helium in zero gravity very near the lambda point, Phys. Rev. B 68, 174518 (2003).
- M. Campostrini, M. Hasenbusch, A. Pelissetto, and E. Vicari, Theoretical estimates of the critical exponents of the superfluid transition in by lattice methods, Phys. Rev. B 74, 144506 (2006).
- Ti-Yen Lan, Yun-Da Hsieh, and Ying-Jer Kao, High-precision Monte Carlo study of the three-dimensional XY model on GPU, arXiv:1211.0780.
- E. Morosan, S. L. Bud’ko, P. C. Canfield, M. S. Torikachvili, and A. H. Lacerda, Thermodynamic and transport properties of RAgGe () single crystals, J. Magn. Magn. Mater. 277, 298 (2004).
- R. Kuchler, T. Bauer, M. Brando, and F. Steglich, A compact and miniaturized high resolution capacitance dilatometer for measuring thermal expansion and magnetostriction, Rev. Sci. Instrum. 83, 095102 (2012).
- R. Kuchler, A. Worl, P. Gegenwart, M. Berben, B. Bryant, and S. Wiedmann, The world’s smallest capacitive dilatometer, for high-resolution thermal expansion and magnetostriction in high magnetic fields, Rev. Sci. Instrum. 88, 083903 (2017).
- R. Prozorov and V. G. Kogan, Effective demagnetizing factors of diamagnetic samples of various shapes, Phys. Rev. Appl. 10, 014030 (2018).
- V. Hutanu, POLI: Polarised hot neutron diffractometer, J. Large-Scale Res. Facil. 1, A16 (2015).
- H. Thoma, W. Luberstetter, J. Peters, and V. Hutanu, Polarised neutron diffraction using novel high-Tc superconducting magnet on single crystal diffractometer POLI at MLZ, J. Appl. Crystallogr. 51, 17 (2018).
- V. Petříček, M. Dušek, and L. Palatinus, Crystallographic computing system JANA2006: General features, Z. Kristallogr. 229, 345 (2014).
- S. V. Gallego, E. S. Tasci, G. de la Flor, J. M. Perez-Mato, and M. I. Aroyo, Magnetic symmetry in the Bilbao Crystallographic Server: A computer program to provide systematic absences of magnetic neutron diffraction, J. Appl. Crystallogr. 45, 1236 (2012).
- H. T. Stokes and D. M. Hatch, FINDSYM: Program for identifying the space-group symmetry of a crystal, J. Appl. Crystallogr. 38, 237 (2005).
- Yixi Su, DNS: Diffuse scattering neutron time-of-flight spectrometer, J. Large-Scale Res. Facil. 1, A27 (2015).
- D. A. Keen, M. J. Gutmann, and C. C. Wilson, SXD – the single-crystal diffractometer at the ISIS spallation neutron source, J. Appl. Crystallogr. 39, 714 (2006).
- Nicholas Metropolis, Arianna W. Rosenbluth, Marshall N. Rosenbluth, Augusta H. Teller, and Edward Teller, Equation of state calculations by fast computing machines, J. Chem. Phys. 21, 1087 (1953).
- A. W. Sandvik, Computational studies of quantum spin systems, AIP Conf. Proc. 1297, 135 (2010).
- M. Kang et al., Dirac fermions and flat bands in the ideal kagome metal , Nat. Mater. 19, 163 (2020).
- Nirmal J. Ghimire and Igor I. Mazin, Topology and correlations on the kagome lattice, Nat. Mater. 19, 137 (2020).
- D. J. Lockwood and M. G. Cottam, The spin-phonon interaction in and studied by Raman spectroscopy, J. Appl. Phys. 64, 5876 (1988).
- Ch. Kant, J. Deisenhofer, T. Rudolf, F. Mayr, F. Schrettle, A. Loidl, V. Gnezdilov, D. Wulferding, P. Lemmens, and V. Tsurkan, Optical phonons, spin correlations, and spin-phonon coupling in the frustrated pyrochlore magnets and , Phys. Rev. B 80, 214417 (2009).
