Rare-earth Zintl compound EuIn₂As₂ has been theoretically recognized as a candidate for realizing an intrinsic antiferromagnetic (AFM) bulk axion insulator and a higher-order topological state, which provides a fertile platform to explore novel topological transport phenomena. However, the axion state has yet to be realized because EuIn₂As₂ is highly hole-doped. Here, we synthesized a series of high-quality Ca-doped EuIn2As2 (CaₓEu₁₋ₓIn₂As₂, x = 0 ~ 0.25) single crystals to tune the Fermi energy above the hole pocket. Our Hall measurements reveal that the isovalent Ca substitution decreases the hole carrier density by shrinking the lattice spacing, which is also confirmed by our first-principles calculations. We further find that both the temperature dependence of the magnetic susceptibility with a local maximum at the N\'eel temperature and the topological Hall effect originating from the finite real-space spin chirality persist in the Ca-doped samples as observed in the pristine EuIn₂As₂, despite that the nonmagnetic Ca substitution decreases the effective moment and the N\'eel temperature. These results show that the Ca substitution tunes the Fermi energy while keeping the AFM magnetic structure, suggesting that the axion insulating state may be realized by further Ca substitution.
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Jian et al. (2024) studied this question.
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