Theory of Moiré Magnetism in Twisted Bilayer α-RuCl 3 .

Motivated by the recent developments in moiré superlattices of van der Waals magnets and the desire to control the magnetic interactions of α-RuCl 3 , here we present a comprehensive theory of the long-range ordered magnetic phases of twisted bilayer α-RuCl 3 . Using a combination of first-principles calculations and atomistic simulations, we show that the stacking-dependent interlayer exchange gives rise to an array of magnetic phases that can be realized by controlling the twist angle. In particular, we discover a complex hexagonal domain structure in which multiple zigzag orders coexist. This multidomain order minimizes the interlayer energy while enduring the energy cost due to domain wall formation. Further, we show that quantum fluctuations can be enhanced across the phase transitions. Our results indicate that magnetic frustration due to stacking-dependent interlayer exchange in moiré superlattices can be exploited to tune quantum fluctuations and the magnetic ground state of α-RuCl 3 .