The solution-processed methylammonium lead tri-iodine (MAPbI3), with long spin lifetimes and large spin diffusion lengths, has merit for developing stable perovskite spin valves (PeSV) with low saturation fields. By far, it remains challenging to avoid ill-defined ferromagnet-MAPbI3 interfaces during device fabrications using solution methods and to quantify the hybridized interfacial electronic and magnetic structures. Herein, an annealing-free method was developed for the fabrication of MAPbI3 based PeSV. In comparison to a thermally annealed device, an improved room temperature magnetoresistance (MR) was achieved. We found remarkable interfacial contributions to anisotropic magnetoresistance and MR. The first-principles calculation was further adopted to quantify the interfacial spin and orbital moments. Our results suggest that the orbital hybridization and the spin transfer are remarkable for the formation of the spin-dependent interfacial density of states. It consequently affects magnetic switching behaviors. This study holds an exceptionally important role for a deep understanding of the spin-polarized electronic transport through the Ni-MAPbI3 hybridized interface.
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