Recently organic–inorganic hybrid perovskite (OIHP) has risen suddenly to become a superstar for spintronic applications. Fundamental understanding of its spin properties is of great importance for future advances of its applications in spin‐optoelectronic devices. In this work, the authors pioneer modulation of the spin Seebeck thermopower (SSTP) in a Pt/MAPbBr3/NiFe nonlocal structure via longitudinal spin Seebeck effect measurements. They unravel the effective magnon injection into the perovskite film from the NiFe layer, and the tunability of SSTP in this structure is easily realized through the optimization of morphology and component engineering of the OIHP film. First, upon biasing samples with a magnetic flux density during the preparation process, a high‐quality OIHP film can be obtained, in which the spin scattering can be reduced leading to the SSTP enhancement. Second, by doping Cr into the OIHP lattice, the increased magnetic moment density and the additional in‐plane inverse Rashba–Edelstein effect synergistically improve spin accumulation in the Pt layer and thus tune its SSTP. Unveiling those phenomena is important to understanding magnon transport in the OIHP interlayer, which is instructive for designing magnonic devices based on OIHP film.
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