Long-range magnetic order with disordered spin orientations in a high-entropy antiferromagnet.

Shen, Yao; Zhang, Guangkai; Zhang, Qinghua; Gui, Xuejuan; Zhang, Yu; Lee, Heemin; Kuo, Cheng-Tai; Lee, Jun-Sik et al. · Nat Commun · 2026

basic_science · Level V

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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<sub>1/4</sub>Fe<sub>1/4</sub>Co<sub>1/4</sub>Ni<sub>1/4</sub>)PS<sub>3</sub>. 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.