Abstract

We report on systematic muon-spin rotation and relaxation (μμSR) studies of the magnetic properties of EuAl4_4 and EuGa4_4 single crystals at a microscopic level. Transverse-field μμSR measurements, spanning a wide temperature range (from 1.5 to 50 K), show clear bulk AFM transitions, with an almost 100% magnetic volume fraction in both cases. Zero-field μμSR measurements, covering both the AFM and the paramagnetic (PM) states, reveal internal magnetic fields Bint(0)=0.33B_\mathrm{int}(0) = 0.33 T and 0.89 T in EuAl4_4 and EuGa4_4, respectively. The transverse muon-spin relaxation rate λTλ_\mathrm{T}, a measure of the internal field distribution at the muon-stopping site, shows a contrasting behavior. In EuGa4_4, it decreases with lowering the temperature, reaching its minimum at zero temperature, λT(0)=0.71λ_\mathrm{T}(0) = 0.71 μμs−1^{-1}. In EuAl4_4, it increases significantly below TNT_\mathrm{N}, to reach 58 μμs−1^{-1} at 1.5 K, most likely reflecting the complex magnetic structure and the competing interactions in the AFM state of EuAl4_4. In both compounds, the temperature-dependent longitudinal muon-spin relaxation λL(T)λ_\mathrm{L}(T), an indication of the rate of spin fluctuations, diverges near the onset of AFM order, followed by a significant drop at T<TNT < T_\mathrm{N}. In the AFM state, spin fluctuations are much stronger in EuAl4_4 than in EuGa4_4, while being comparable in the PM state. The evidence of robust spin fluctuations against the external magnetic fields provided by μμSR may offer new insights into the origin of the topological Hall effect and the possible magnetic skyrmions in the EuAl4_4 and EuGa4_4 compounds.

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