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Interplay of spin-tetramer cluster magnetism and magnetodielectric effect in polar
Phys. Rev. Materials 9, 114407 – Published 12 November, 2025
DOI: https://doi.org/10.1103/rqpb-qwkp
Abstract
We explore the interrelation between crystal structure, magnetism, and magnetodielectric behavior in the spin-cluster compound . Magnetization measurements indicate the emergence of long-range antiferromagnetic order at , supported by corresponding anomalies in the specific heat. Magnetic isotherms display a field-induced spin-flop transition at critical fields and . Field-dependent neutron diffraction uncovers an antiferromagnetic ground state characterized by the propagation vector for fields , which transitions to a ferrimagnetic state with for . In the intermediate field range (), both magnetic vectors exist. Dielectric measurements exhibit a distinct anomaly near , alongside a robust magnetodielectric response that persists well above the transition, indicating strong coupling between the Fe tetramer spin clusters and dipolar degrees of freedom. The resulting phase diagram delineates three magnetic regimes, distinguished by shifts in propagation vectors and corresponding variations in magnetization, thermal, and dielectric properties. Furthermore, temperature-dependent synchrotron x-ray diffraction suggests a subtle magnetostrictive effect near the ordering temperature. These findings highlight the intricate magnetodielectric effect in and position it as a promising candidate for magnetodielectric applications.