Topological insulators possess strong spin−orbit coupling, which potentially presents efficient charge−spin interconversion. The effective manipulation of this conversion plays a central role in spin-based device applications and is attracting increasing attention nowadays. In this study, by constructing a multifunctional hybrid device Cr-BST/Py/PMN-PT and applying spin-torque ferromagnetic resonance measurement, continuously controllable charge−spin conversion efficiency and even the enhancement of its value up to about 450% are realized via regulation of the ferroelectric polarization in the topological insulator Cr-BST. The band structure of Cr-BST characterized by angle-resolved photoelectron spectroscopy measurement presents an apparent Dirac-like state located at the large band gap of the bulk state near the Fermi level, which indicates a surface statedominated contribution to the charge−spin conversion. Further investigation via density functional theory on the electronic structure of BST verifies that the controllable conversion efficiency dominantly originates from the evolution of the band structure under strain modulation. These findings demonstrate TIs as one of the promising materials for the charge−spin interconversion and its regulation, which are instructive for low-dissipation spintronics devices.

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