Intercalant-mediated Kitaev exchange in Ag3LiIr2O6

Abstract

The recently synthesized Ag3LiIr2O6 has been proposed as a Kitaev magnet in proximity to the quantum spin liquid phase. We explore its microscopic Hamiltonian and magnetic ground state using many-body quantum chemistry methods and exact diagonalization techniques. Our calculations establish a dominant bond dependent ferromagnetic Kitaev exchange between Ir sites and find that the inclusion of Ag 4d orbitals in the configuration interaction calculations strikingly enhances the Kitaev exchange. Furthermore, using exact diagonalization of the nearest-neighbor fully anisotropic J−K−Γ Hamiltonian, we obtain the magnetic phase diagram as a function of further neighbor couplings. We find that the antiferromagnetic off-diagonal coupling stabilizes long range order, but the structure factor calculations suggest that the material is very close to the quantum spin liquid phase and the ordered state can easily collapse into a liquid by small perturbations such as structural distortion or bond disorder.