Direct observation of multivalent states and 4 f → 3d charge transfer in Ce-doped yttrium iron garnet thin films

Due to their large magneto-optic responses, rare-earth-doped yttrium iron garnets, Y3Fe5O12 (YIG), are highly regarded for their potential in photonics and magnonics. Here, we consider the case of Ce-doped YIG (Ce-YIG) thin films, in which substitutional Ce3+ ions are magnetic because of their 4f(1) ground state. In order to elucidate the impact of Ce substitution on the magnetization of YIG, we have carried out soft x-ray spectroscopy measurements on Ce-YIG films. In particular, we have used the element specificity of x-ray magnetic circular dichroism to extract the individual magnetization curves linked to Ce and Fe ions. Our results show that Ce doping triggers a selective charge transfer from Ce to the Fe tetrahedral sites in the YIG structure. This, in turn, causes a disruption of the electronic and magnetic properties of the parent compound, reducing the exchange coupling between the Ce and Fe magnetic moments and causing atypical magnetic behavior. Our work is relevant for understanding magnetism in rare-earth-doped YIG and, eventually, may enable a quantitative evaluation of the magneto-optical properties of rare-earth incorporation into YIG.