Making a Hedgehog Spin-Vortex State Possible: Geometric Frustration on a Square Lattice

Magnetic materials with noncollinear spin arrangements are of considerable interest owing to their potential use in emerging computational technologies and memory devices. Competing magnetic interactions, i.e., magnetic frustration, are one of the main origins of noncollinear magnetic structures. While frustrated systems have been mainly studied among magnetic insulators, combining magnetic frustration with electrical conductivity can allow simultaneous charge and spin manipulation, which is crucial for the design of electronic devices. Here, we present a new intermetallic solid solution LaMn2-xAu4+x, whose crystal structure accommodates magnetically frustrated Mn square nets. Powder neutron diffraction and first-principles analysis provide evidence that the metallic LaMn2-xAu4+x phase can host the frustration-driven hedgehog spin-vortex crystal─a rare noncollinear magnetic state, which was previously exclusively observed for iron pnictides.