Spin Seebeck Effect in Iron Oxide Thin Films: Effects of Phase Transition, Phase Coexistence, And Surface Magnetism.

Understanding the effects 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 the LSSE in biphase iron oxide (BPIO = α-Fe 2 O 3 + Fe 3 O 4 ) thin films grown on Si (100) and Al 2 O 3 (111) substrates. A combination of a temperature-dependent anomalous Nernst effect (ANE) and electrical resistivity measurements show that the contribution of the ANE from the BPIO layer is negligible in comparison to the intrinsic LSSE in the Si/BPIO/Pt heterostructure, even at room temperature. Below the Verwey transition of the Fe 3 O 4 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 Al 2 O 3 /BPIO/Pt heterostructures around the Verwey transition of the Fe 3 O 4 phase and the antiferromagnetic (AFM) Morin transition of the α-Fe 2 O 3 phase are observed. The LSSE signal for Si/BPIO/Pt is found to be almost 2 times greater than that for Al 2 O 3 /BPIO/Pt; however, an opposite trend is observed for the saturation magnetization. Magnetic force microscopy reveals the higher density of surface magnetic moments of the Si/BPIO film in comparison to the Al 2 O 3 /BPIO film, which underscores the dominant role of interfacial magnetism on the LSSE signal and thereby explains the larger LSSE for Si/BPIO/Pt.