Tailoring Neel orders in Layered Topological Antiferromagnets

In the two-dimensional limit, the interplay between Neel order and band topology in van der Waals topological antiferromagnets can give rise to novel quantum phenomena in the quantum anomalous Hall state, including the cascaded quantum phase transition and spin-modulation effect. However, due to the absence of net magnetization in antiferromagnets, probing the energetically degenerate Neel orders has long remained a significant challenge. Inspired by recent advances in realizing the quantum anomalous Hall effect in AlOx-capped layered topological antiferromagnet MnBi2Te4, we demonstrate deterministic control over the Neel order through surface anisotropy engineering enabled by the AlOx capping layer. By tuning the surface anisotropy, we uncover paritydependent symmetry breaking states that manifest as distinct odd-even boundary architectures, including 180 degree domain walls or continuous spin structures. Comparative studies between AlOx-capped and pristine odd-layer MnBi2Te4 flakes using domain-resolved magnetic force microscopy reveal pronounced differences in coercivity and magnetization-reversal dynamics. Notably, an unconventional giant exchange bias, which arises from perpendicular magnetic anisotropy rather than traditional interface pinning mechanisms, is observed for the first time. Our findings establish a pathway for manipulating Neel order through surface modification in A-type antiferromagnets, offering new opportunities for spintronic devices and quantum information technologies.