Inducing magnetism in a topological insulator (TI) by exchange coupling with a ferromagnetic insulator (FMI) will break the time-reversal symmetry of topological surface states, offering possibilities to realize several predicted novel magneto-electric effects. Seeking suitable FMI materials is crucial for the coupling of heterojunctions, and yet is challenging as well and only a few kinds have been explored. In this report, we introduce epitaxial LaCoO3 thin films on a SrTiO3 substrate, which is an insulating ferromagnet with a Curie temperature of TC ∼ 85 K, to be combined with TIs for proximity coupling. Thin films of the prototype topological insulator, Bi2Se3, are successfully grown onto the (001) surface of LaCoO3/SrTiO3, forming a high-quality TI/FMI heterostructure with a sharp interface. The magnetic and transport measurements manifest the emergence of a ferromagnetic phase in Bi2Se3 films, with additional induced moments and a suppressed weak antilocalization effect, while preserving the carrier mobility of the intrinsic Bi2Se3 films at the same time. Moreover, a signal of an anomalous Hall effect is observed and persists up to temperatures above 100 K, paving the way towards spintronic device applications.
The enigma of the emergent ferromagnetic state in tensile-strained LaCoO3 thin films remains to be explored because of the lack of a well agreed explanation. The direct magnetic imaging technique using a low-temperature magnetic force microscope (MFM) is critical to reveal new aspects of the ferromagnetism by investigating the lateral magnetic phase distribution. Here we show the experimental demonstration of the rare halved occupation of the ferromagnetic state in tensilestrained LaCoO3 thin films on SrTiO3 substrates using the MFM. The films have uniformly strained lattice structure and minimal oxygen vacancies (less than 2%) beyond the measurement limit. It is found that percolated ferromagnetic regions with typical sizes between 100 nm and 200 nm occupy about 50% of the entire film, even down to the lowest achievable temperature of 4.5 K and up to the largest magnetic field of 13.4 T. Preformed ferromagnetic droplets were still observed when the temperature is 20 K above the Curie temperature indicating the existence of possible Griffiths phase. Our study demonstrated a sub-micron level phase separation in high quality LaCoO3 thin films, which has substantial implications in revealing the intrinsic nature of the emergent ferromagnetism.
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