Twist engineering of van der Waals magnets has emerged as an outstanding platform for manipulating exotic magnetic states. However, the complicated form of spin interactions in the large moirésuperlattice obstructs a concrete understanding of such spin systems. To tackle this problem, for the first time, we developed a generic ab initio spin Hamiltonian for twisted bilayer magnets. Our atomistic model reveals that strong AB sublattice symmetry breaking due to the twist introduces a promising route to realize the novel noncentrosymmetric magnetism. Several unprecedented features and phases are uncovered including the peculiar domain structure and skyrmion phase induced by noncentrosymmetricity. The diagram of those distinctive magnetic phases has been constructed, and the detailed nature of their transitions analyzed. Further, we established the topological band theory of moirémagnons relevant to each of these phases. By respecting the full lattice structure, our theory provides the characteristic features that can be detected in experiments.

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Antiferromagnetic topological insulators have attracted great attention in the condensed matter physics owing to the fundamental interest in exotic quantum states and topological antiferromagnetic spintronics. Starting with the typical topological insulator of Bi2Te3, we introduced the magnetic order by substituting Gd at the Bi site and tuned the Fermi level by substituting Se at the Te site. That is, we prepared single crystals of Gd xBi2− xTe3− ySe y with various x (= 0.02 and 0.06) and y (= 0.1, 0.2, 0.5, 0.7, 1.0, and 1.5). The magnetic data revealed an antiferromagnetic order for x = 0.06, and the transport data manifested the charge neutral point at y = 0.7. Combining all these results together, the material with x = 0.06 and y = 0.7 is characterized as an antiferromagnetic topological insulator, where we observed exotic magnetotransport properties such as weak antilocalization and negative longitudinal magnetoresistance that are frequently analyzed as chiral anomalies in Weyl materials.