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Abstract Magnetocapacitance (MC) effect has been observed in systems where both symmetries of time-reversal and space-inversion are broken, for examples, in multiferroic materials and spintronic devices. The effect has received increasing attention due to its interesting physics and the prospect of applications. Recently, a large tunnel magnetocapacitance (TMC) of 332% at room temperature was reported using MgO-based (001)-textured magnetic tunnel junctions (MTJs). Here, we report further enhancement in TMC beyond 420% at room temperature using epitaxial MTJs with an MgAl₂O₄(001) barrier with a cation-disordered spinel structure. This large TMC is partially caused by the high effective tunneling spin polarization, resulted from the excellent lattice matching between the Fe electrodes and the MgAl₂O₄barrier. The epitaxial nature of this MTJ system sports an enhanced spin-dependent coherent tunneling effect. Among other factors leading to the large TMC are the appearance of the spin capacitance, the large barrier height, and the suppression of spin flipping through the MgAl₂O₄barrier. We explain the observed TMC by the Debye-Fröhlich modelled calculation incorporating Zhang-sigmoid formula, parabolic barrier approximation, and spin-dependent drift diffusion model. Furthermore, we predict a 1000% TMC in MTJs with a spin polarization of 0.8. These experimental and theoretical findings provide a deeper understanding on the intrinsic mechanism of the TMC effect. New applications based on large TMC may become possible in spintronics, such as multi-value memories, spin logic devices, magnetic sensors, and neuromorphic computing. 

Abstract Magnetic tunnel junctions (MTJs) in the field of spintronics have received enormous attention owing to their fascinating spin phenomena for fundamental physics and potential applications. MTJs exhibit a large tunnel magnetoresistance (TMR) at room temperature. However, TMR depends strongly on the bias voltage, which reduces the magnitude of TMR. On the other hand, tunnel magnetocapacitance (TMC), which has also been observed in MTJs, can be increased when subjecting to a biasing voltage, thus exhibiting one of the most interesting spin phenomena. Here we report a large voltage-induced TMC beyond 330% in MgO-based MTJs, which is the largest value ever reported for MTJs. The voltage dependence and frequency characteristics of TMC can be explained by the newly proposed Debye-Fröhlich model using Zhang-sigmoid theory, parabolic barrier approximation, and spin-dependent drift diffusion model. Moreover, we predict that the voltage-induced TMC ratio could reach over 3000% in MTJs. It is a reality now that MTJs can be used as capacitors that are small in size, broadly ranged in frequencies and controllable by a voltage. Our theoretical and experimental findings provide a deeper understanding on the exact mechanism of voltage-induced AC spin transports in spintronic devices. Our research may open new avenues to the development of spintronics applications, such as highly sensitive magnetic sensors, high performance non-volatile memories, multi-functional spin logic devices, voltage controlled electronic components, and energy storage devices.