Spontaneous reversal of spin chirality and competing phases in the topological magnet EuAl4

Abstract Materials exhibiting a spontaneous reversal of spin chirality have the potential to drive the widespread adoption of chiral magnets in spintronic devices. Unlike the majority of chiral magnets that require the application of an external field to reverse the spin chirality, we observe the spin chirality to spontaneously reverse in the topological magnet EuAl 4 . Using resonant elastic x-ray scattering we demonstrate that all four magnetic phases in EuAl 4 are single-k, where the first two magnetic phases are characterized by spin density wave order and the last two by helical spin order. A single spin chirality was stabilised across the 1mm 2 sample, and the reversal of spin chirality occurred whilst maintaining a helical magnetic structure. At the onset of the helical magnetism, the crystal symmetry lowers to a chiral monoclinic space group, explaining the asymmetry in the chiral spin order, and establishing a mechanism by which the spin chirality could reverse via magnetostructural coupling.