Long-range magnetic order with disordered spin orientations in a high-entropy antiferromagnet
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. While atomic disorder normally promotes glassy states, in some rare cases long-range magnetic order can persist. However, the mechanism, and microscopic characters, remain elusive. Here, Shen et al combine neutron diffraction and resonant X-ray scattering to shed light on the formation of long-range magnetic order in a high-entropy honeycomb van der Waals magnet.
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Shen, Y. R., Zhang, G., Zhang, Q., Gui, X., Zhang, Y., Lee, H., Kuo, C.-T., Lee, J.-S., Sutarto, R., Ye, F., Pan, Z. W., Qin, X., Wang, J., Ying, T., & Long, Y. (2026). Long-range magnetic order with disordered spin orientations in a high-entropy antiferromagnet. Nature Communications. https://doi.org/10.1038/s41467-026-70184-x
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