DOE OSTI · 3030486
Long-range magnetic order with disordered spin orientations in a high-entropy antiferromagnet
Abstract
Disorder in magnetic systems typically suppresses long-range order, promoting short-range states such as spin glasses and magnetic clusters. This is particularly prominent in high-entropy materials, characterized by the random distributions of local magnetic entities and exchange interactions. However, in rare exceptions, long-range magnetic order can persist in high-entropy systems, while the microscopic characters and underlying mechanisms remain elusive, especially the magnetic behaviors of individual elements. Here, combining neutron diffraction and resonant soft x-ray scattering, we have conducted an element-specific investigation into the magnetic order of a high-entropy honeycomb-lattice van der Waals material (Mn 1/4 Fe 1/4 Co 1/4 Ni 1/4 )PS 3 . Despite significant atomic disorder, long-range zigzag antiferromagnetic order is observed below 72 K, with all four transition-metal elements participating in a unified phase transition. However, the spin orientations of various elements are distinct, attributed to the competition between single-ion anisotropies and exchange interactions. Our findings showcase a novel form of long-range magnetic order with disordered spin orientations, which is synergically stabilized by distinct magnetic elements in a high entropy magnet, offering a new paradigm for understanding complex magnetic systems.
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Shen, Yao [Chinese Academy of Sciences (CAS), Beijing (China); University of Chinese Academy of Sciences, Beijing (China)] (ORCID:0000000346974719), Zhang, Guangkai [Chinese Academy of Sciences (CAS), Beijing (China); Shanghai Normal University (China)], Zhang, Qinghua [Chinese Academy of Sciences (CAS), Beijing (China)] (ORCID:0000000190867000), Gui, Xuejuan [Renmin University of China, Beijing (China)], Zhang, Yu [Chinese Academy of Sciences (CAS), Beijing (China)], Lee, Heemin [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)], Kuo, Cheng-Tai [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)] (ORCID:0000000177216481), Lee, Jun-Sik [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)] (ORCID:0000000301819352), Sutarto, Ronny [University of Saskatchewan, Saskatoon, SK (Canada). Canadian Light Source, Inc.] (ORCID:0000000219693690), Ye, Feng [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000174774648), Pan, Zhao [Chinese Academy of Sciences (CAS), Beijing (China)], Qin, Xiaomei [Shanghai Normal University (China)], Wang, Jinchen [Renmin University of China, Beijing (China); Paul Scherrer Inst. (PSI), Villigen (Switzerland); Ecole Polytechnique Federale Lausanne (EPFL) (Switzerland)] (ORCID:0000000226919002), Ying, Tianping [Chinese Academy of Sciences (CAS), Beijing (China)] (ORCID:0000000176651270), Long, Youwen [Chinese Academy of Sciences (CAS), Beijing (China); University of Chinese Academy of Sciences, Beijing (China)] (ORCID:0000000285877818). 2026-03-06. Long-range magnetic order with disordered spin orientations in a high-entropy antiferromagnet. https://doi.org/10.1038/s41467-026-70184-x
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