Novel magnetic state in $d^4$ Mott insulators

We show that the interplay of strong Hubbard interaction $U$ and spin-orbit coupling $\lambda$ in systems with the $d^4$ electronic configuration leads to several unusual magnetic phases. While in the atomic limit the system is in a non-magnetic $J=0$ singlet state, we find that the competition between superexchange and atomic spin-orbit coupling dramatically changes the local moment, which challenges the conventional wisdom that local moments are well-defined in a Mott insulator. Most notably, we find that in the Mott limit at strong $U$ there is a phase transition from a non-magnetic insulator of uncoupled $J=0$ singlets to an orbitally entangled ferromagnetic insulator. We identify candidate materials and present predictions for Resonant X-ray Scattering (RXS) signatures for the unusual magnetism in $d^4$ Mott insulators and contrast them with the well-studied $d^5$ case.