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 (Mn1/4Fe1/4Co1/4Ni1/4)PS3. 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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Data availability
All data that support the findings of this study have been deposited in the Zenodo database with the access code 1763671649.
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Acknowledgements
We thank Gang Chen for inspiring discussions. This work was supported by the National Key R&D Program of China (Grant No. 2024YFA1408301 (Y.S.), 2023YFA1406500 (J.W.), 2021YFA1400300 (Y.L.)) and the National Natural Science Foundation of China (Grant No. 12574139 (Y.S.), 12425403 (Y.L.), 52272267 (T.Y.), 52522201 (T.Y.), 12261131499(Y.L.)). Neutron diffraction measurements of this research used resources at the Spallation Neutron Source (SNS), a US Department of Energy Office of Science User Facility operated by the Oak Ridge National Laboratory (ORNL). The beam time was allocated to CORELLI on Proposal No. IPTS-30179.1. RSXS measurements were carried out at the Stanford Synchrotron Radiation Lightsource (SSRL), SLAC National Accelerator Laboratory, which is supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences (contract No. DE-AC02-76SF00515), and the Canadian Light Source (CLS), a national research facility of the University of Saskatchewan, which is supported by the Canada Foundation for Innovation (CFI), the Natural Sciences and Engineering Research Council (NSERC), the Canadian Institutes of Health Research (CIHR), the Government of Saskatchewan, and the University of Saskatchewan. Notice: This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (https://www.energy.gov/doe-public-access-plan).
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Y.S., J.W., and T.Y. conceived the project. Q.Z., Y.Z., and T.Y. synthesized and characterized the samples. X.G., F.Y., and J.W. performed the neutron measurements. Y.S., G.Z., H.L., C.T.K., J.S.L., and R.S. performed the X-ray measurements. Y.S., Z.P., X.Q., J.W., T.Y., and Y.L. interpreted the data. The paper was written by Y.S., J.W., and T.Y. with input from all co-authors.
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Shen, Y., Zhang, G., Zhang, Q. et al. Long-range magnetic order with disordered spin orientations in a high-entropy antiferromagnet. Nat Commun (2026). https://doi.org/10.1038/s41467-026-70184-x
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DOI: https://doi.org/10.1038/s41467-026-70184-x
