Tunable symmetry breaking in a hexagonal-stacked moiré magnet
Symmetry plays a central role in defining magnetic phases, making tunable symmetry breaking across magnetic transitions highly desirable for discovering non-trivial magnetism. Magnetic moiré superlattices, formed by twisting two-dimensional magnetic crystals, have been theoretically proposed and experimentally explored as platforms for unconventional magnetic states. However, despite recent advances, the ability to tune symmetry breaking in moiré magnetism remains limited, as twisted two-dimensional magnets predominantly inherit the magnetic properties and symmetries of their constituent layers. Here, in this work, we demonstrate a clear evolution of symmetry in hexagonal-stacked twisted double-bilayer CrI 3 as the twist angle increases from 180° to 190°. Although the net magnetization remains zero across this twist-angle range, the magnetic phase breaks only the threefold rotational symmetry at 180°, but it breaks all the rotational, mirror and time-reversal symmetries at intermediate twist angles between 181° and 185°, and all broken symmetries are recovered at 190°. This pronounced symmetry breaking at intermediate twist angles is accompanied by metamagnetic behaviour, evidenced by symmetric double hysteresis loops around zero magnetic field. Together, these results reveal that hexagonal-stacked twisted double-bilayer CrI3 at intermediate twist angles hosts a distinct moiré magnetic phase, featuring periodic in-plane spin textures with broken rotational, mirror and time-reversal symmetries.