Spin Seebeck effect in iron oxide thin films: Effects of phase transition, phase coexistence, and surface magnetism

Understanding impacts of phase transition, phase coexistence, and surface magnetism on the longitudinal spin Seebeck effect (LSSE) in a magnetic system is essential to manipulate the spin to charge current conversion efficiency for spincaloritronic applications. We aim to elucidate these effects by performing a comprehensive study of the temperature dependence of LSSE in biphase iron oxide (BPIO = alpha-Fe2O3 + Fe3O4) thin films grown on Si (100) and Al2O3 (111) substrates. A combination of temperature-dependent anomalous Nernst effect (ANE) and electrical resistivity measurements show that the contribution of ANE from the BPIO layer is negligible compared to the intrinsic LSSE in the Si/BPIO/Pt heterostructure even at room temperature. Below the Verwey transition of the Fe3O4 phase, the total signal across BPIO/Pt is dominated by the LSSE. Noticeable changes in the intrinsic LSSE signal for both Si/BPIO/Pt and Al2O3/BPIO/Pt heterostructures around the Verwey transition of the Fe3O4 phase and the antiferromagnetic (AFM) Morin transition of the alpha-Fe2O3 phase are observed. The LSSE signal for Si/BPIO/Pt is found to be almost two times greater than that for Al2O3/BPIO/Pt, an opposite trend is observed for the saturation magnetization though. Magnetic force microscopy reveals the higher density of surface magnetic moments of the Si/BPIO film compared to the Al2O3/BPIO film, which underscores a dominant role of interfacial magnetism on the LSSE signal and thereby explains the larger LSSE for Si/BPIO/Pt.