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Crystal electric field excitations and spin dynamics in the spin-orbit coupled distorted honeycomb magnet
Phys. Rev. B 113, 214452 – Published 23 June, 2026
DOI: https://doi.org/10.1103/z66x-362w
Abstract
The magnetic properties and crystal electric field (CEF) scheme of are investigated via magnetization, heat capacity, inelastic neutron scattering (INS) and muon spin relaxation () experiments on a polycrystalline sample. The ions form a quasi-two-dimensional distorted honeycomb network with a Kramers doublet ground state. Magnetic susceptibility and heat capacity reveal short-range antiferromagnetic correlations, manifested as a broad maximum around 1.4 K and 1.1 K, respectively. Heat-capacity data further confirm the onset of a magnetic long-range order at . The INS spectra exhibit eight CEF excitations, and the CEF analysis yields the -factor anisotropy with and exchange anisotropy with and . The experimental temperature and field-dependent magnetization and heat capacity are also reproduced by the simulation using the CEF energy scheme. Zero-field measurements down to 30 mK do not exhibit coherent oscillations or a static tail. The spectra are well described by two exponential relaxation components, indicating two magnetically inequivalent muon environments. The relaxation rates display a nearly temperature-independent plateau below and follow an Orbach-type activated behavior at higher temperatures involving excited CEF levels, consistent with the INS results. Longitudinal-field measurements reveal only weak decoupling up to 1.5 T, indicating the presence of slow spin fluctuations that persist well below . Overall, emerges as an anisotropic spin-orbit-coupled honeycomb magnet in which strong CEF-driven anisotropy and reduced dimensionality give rise to unconventional low-temperature magnetic behavior distinct from its Yb counterpart .