Topological Spin Textures in an Insulating van der Waals Ferromagnet

Generation and control of topological spin textures constitutes one of the most exciting challenges of modern spintronics given their potential applications in information storage technologies. Of particular interest are magnetic insulators, which due to low damping, absence of Joule heating and reduced dissipation can provide energy‐efficient spin‐textures platform. Here, it is demonstrated that the interplay between sample thickness, external magnetic fields, and optical excitations can generate a prolific paramount of spin textures, and their coexistence in insulating CrBr3 van der Waals (vdW) ferromagnets. Using high‐resolution magnetic force microscopy and large‐scale micromagnetic simulation methods, the existence of a large region in T‐B phase diagram is demonstrated where different stripe domains, skyrmion crystals, and magnetic domains exist and can be intrinsically selected or transformed to each‐other via a phase‐switch mechanism. Lorentz transmission electron microscopy unveils the mixed chirality of the magnetic textures that are of Bloch‐type at given conditions but can be further manipulated into Néel‐type or hybrid‐type via thickness‐engineering. The topological phase transformation between the different magnetic objects can be further inspected by standard photoluminescence optical probes resolved by circular polarization indicative of an existence of exciton‐skyrmion coupling mechanism. The findings identify vdW magnetic insulators as a promising framework of materials for the manipulation and generation of highly ordered skyrmion lattices relevant for device integration at the atomic level. The formation of a skyrmion lattice in van der Waals ferromagnet CrBr3 opens pathways for exploration of topological spin textures in 2D insulating crystals. These skyrmions manifest in unusual crystalline environment characterized by centrosymmetric crystal structure and are stabilized through dipolar rather than Dzyaloshinskii–Moriya interactions. The construction of B‐T phase diagram enables versatile phase‐switching mechanisms for controlling magnetization textures.