Spin-Orbit Coupled Insulators and Metals on the Verge of Kitaev Spin Liquids in Ilmenite Heterostructures

Competition and cooperation between electron correlation and relativistic spin-orbit coupling give rise to diverse exotic quantum phenomena in solids. An illustrative example is spin-orbit entangled quantum liquids, which exhibit remarkable features such as topological orders and fractional excitations. The Kitaev honeycomb model realizes such interesting states, called the Kitaev spin liquids, but its experimental feasibility is still challenging. Here we theoretically investigate hexagonal heterostructures including a candidate for the Kitaev magnets, MgIrO₃, to actively manipulate the electronic and magnetic properties toward realizing the Kitaev spin liquids. For three different structure types of ilmenite bilayers MgIrO₃/ATiO₃ with A = Mn, Fe, Co, and Ni, we obtain the optimized lattice structures, the electronic band structures, the stable magnetic orders, and the effective magnetic couplings. We find that the spin-orbital coupled bands characterized by the pseudospin jeff= 1/2 are retained in the MgIrO₃ layer for all the heterostructures, but the magnetic state and the band gap depend on the types of heterostructures as well as the A atoms. In particular, one type becomes metallic irrespective of A, while the other two are mostly insulating. We show that the insulating cases provide spin-orbit coupled Mott insulating states with dominant Kitaev-type interactions, accompanied by different combinations of subdominant interactions depending on the heterostructural type and A, while the metallic cases realize spin-orbit coupled metals with various doping rates. Our results indicate that these hexagonal heterostructures are a good platform for engineering electronic and magnetic properties of the spin-orbital coupled correlated materials, including the possibility of Majorana Fermi surfaces and topological superconductivity.