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中国物理学会期刊

FeCl2/GaSe范德华异质结中二维磁性的滑移铁电调控:第一性原理研究

Sliding Ferroelectric-induced Manipulation of Two-Dimensional Magnetism in the FeCl2/GaSe Heterostructures: A First-Principles Study

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  • 与传统范德华铁电材料不同,二维滑移铁电体可通过原子层间的相对滑移实现面外铁电极化翻转,兼具翻转势垒低、响应速度快与室温稳定优异等特性,目前已成为自旋电子学领域的研究热点。由反铁磁层与滑移铁电层构建的二维范德华异质结,为研制新型二维多铁薄膜提供了理想的研究平台。本文基于第一性原理计算,系统研究了FeCl2/GaSe异质结中滑移铁电性对磁性的调控规律及其微观作用机制。结果表明,层间滑移诱导的铁电极化翻转可驱动体系的磁基态在AFM4与AFM1两种反铁磁序之间可逆转变,同步伴随金属-半导体相变过程;与此同时,体系内Fe-Cl-Fe超交换作用强度与磁交换耦合系数也得到有效调控。磁性调控的根源为:层间滑移引发体系产生反演对称性破缺与铁电极化翻转,进而诱导FeCl2双层内局域电荷重新分布。滑移铁电极化通过界面相互作用与二维磁性产生耦合,使体系展现出显著的磁电耦合效应。本研究揭示了滑移铁电调控二维磁性的物理机制,可为后摩尔时代低功耗、超高密度二维自旋电子器件的设计提供理论支撑。

     

    Two-dimensional (2D) van der Waals (vdW) sliding ferroelectric materials can reverse their out-of-plane ferroelectric polarization through interlayer sliding, a process characterized by low energy barriers, fast response kinetics, and robust stability at room temperature. These materials are promising candidates for low-power and ultra-high-density spintronic devices in the post-Moore era. Assembling sliding ferroelectrics and magnetic materials into 2D vdW heterostructures is an ideal route to realizing strong magnetoelectric coupling. Nevertheless, the underlying physical mechanism for manipulating 2D magnetism via sliding ferroelectricity still lacks a comprehensive theoretical explanation. In this work, we perform first-principles calculations on FeCl2/GaSe multiferroic heterostructures to systematically investigate how ferroelectric polarization reversal, triggered by interlayer sliding, governs the 2D magnetism and electronic structures, and to elucidate the underlying physical origins. The calculated results show that interlayer sliding can achieve ferroelectric polarization reversal, with the polarization Pz varying from -2.17 pC/m (Structure_1) to 2.25 pC/m (Structure_7). The sliding process has minimal effects on the vdW spacing, bond lengths, and the magnetic moments of Fe ions; however, it can drive a metal-semiconductor transition in our FeCl2/GaSe heterostructures. Moreover, interlayer sliding can induce the magnetic ground state of our 2D system to switch between two different antiferromagnetic orders, AFM4 and AFM1, and effectively manipulate the strengths of the Fe-Cl-Fe superexchange interactions and exchange couplings. The intralayer antiferromagnetic interaction remains dominant, while the interlayer exchange coupling parameter Jc also show antiferromagnetic behaviors. This is mainly attributable to reinforced charge redistribution and enhanced orbital hybridization at the vdW interface. Furthermore, the magnetic easy axis remains perpendicular to the surface of the 2D heterostructure. The magnetic anisotropy energy increases from -0.20 meV to -0.92 meV, which significantly enhances the thermal stability of magnetic domains and effectively suppresses thermal fluctuations. This work confirms that the interlayer sliding can efficiently and reversibly manipulate the 2D magnetism in FeCl2/GaSe heterostructure. We also revealed the microscopic mechanism underlying this manipulation, which provides a solid theoretical foundation for the design of high-performance spintronic devices with strong magnetoelectric coupling and low-power multistate memory devices for the post-Moore era.

     

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