Direct evidence for the all-in/all-out magnetic structure in the pyrochlore iridates from muon spin relaxation

Abstract

In the pyrochlore iridates R${}_{2}$Ir${}_{2}$O${}_{7}$ (R = lanthanide, Y) determination of the magnetic structure of the iridium moments remains an outstanding problem despite the role this is expected to play in the formation of novel band structures and topologies in these materials. In this work, an analysis of the experimentally measured spontaneous muon spin precession frequency is presented which incorporates both probabilistic and ab initio modeling techniques to determine the ground state magnetic structure. It is shown that the experimentally observed results are consistent only with a magnetically ordered Ir${}^{4+}$ sublattice with the so-called ``all-in/all-out'' magnetic structure, and that the electronic state of the Ir${}^{4+}$ is best described by the ${J}_{\mathrm{eff}}=\frac{1}{2}$ model in several member compounds. Through this approach it is also demonstrated that such a simple structure is not likely to be present on the rare-earth sublattice which contains much larger localized moments.