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Abstract Mechanical stacking of two dissimilar materials often has surprising consequences for heterostructure behavior. In particular, a 2D electron gas (2DEG) is formed in the heterostructure of the topological crystalline insulator Pb0.24Sn0.76Te and graphene due to contact of a polar with a nonpolar surface and the resulting changes in electronic structure needed to avoid polar catastrophe. The spintronic properties of this heterostructure with non‐local spin valve devices are studied. This study observes spin‐momentum locking at lower temperatures that transitions to regular spin channel transport only at ≈40 K. Hanle spin precession measurements show a spin relaxation time as high as 2.18 ns. Density functional theory calculations confirm that the spin‐momentum locking is due to a giant Rashba effect in the material and that the phase transition is a Lifshitz transition. The theoretically predicted Lifshitz transition is further evident in the phase transition‐like behavior in the Landé g‐factor and spin relaxation time.
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Abstract Combining topological insulators (TIs) and magnetic materials in heterostructures is crucial for advancing spin‐based electronics. Magnetic insulators (MIs) can be deposited on TIs using the spin‐spray process, which is a unique nonvacuum, low‐temperature growth process. TIs have highly reactive surfaces that oxidize upon exposure to atmosphere, making it challenging to grow spin‐spray ferrites on TIs. In this work, it is demonstrated that a thin titanium capping layer on TI, followed by oxidation in atmosphere to produce a thin TiOxinterfacial layer, protects the TI surface, without significantly compromising spin transport from the magnetic material across the TiOxto the TI surface states. First, it is demonstrated that in Bi2Te3/TiOx/Ni80Fe20heterostructures, TiOxprovides an excellent barrier against diffusion of magnetic species, yet maintains a large spin‐pumping effect. Second, the TiOxis also used as a protective capping layer on Bi2Te3, followed by the spin‐spray growth of the MI, NixZnyFe2O4(NZFO). For the thinnest TiOxbarriers, Bi2Te3/TiOx/NZFO samples have antiferromagnetic (AFM) disordered interfacial layer because of diffusion. With increasing TiOxbarrier thickness, the diffusion is reduced, but still maintains strong interfacial magnetic exchange‐interaction. These experimental results demonstrate a novel method of low‐temperature growth of magnetic insulators on TIs enabled by interface engineering.