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电控磁效应调控二维 (2D) 反铁磁 (AFM) 材料的研究结合了电控磁效应与半导体工艺兼容且低能耗的优势, 2D材料范德瓦耳斯界面便于异质集成以及AFM材料无杂散场、抗外磁场干扰、内禀频率高的优势, 成为领域内研究的重点. 载流子浓度调控是电控磁效应的主要机制, 已被证明是调控材料磁性能的有效途径. 层内AFM材料的净磁矩为零, 磁性调控测量存在挑战, 故其电控磁效应研究尚少且潜在的机制尚不清楚. 基于有机阳离子的多样性, 本文利用有机阳离子插层系统地调控了2D 层内AFM材料MPX3 (M = Mn, Fe, Ni; X = S, Se) 的载流子浓度, 并研究了电子掺杂对其磁性能的影响. 笔者在MPX3家族材料中发现了依赖载流子浓度变化的AFM-亚铁磁 (FIM)/铁磁 (FM) 的转变, 并结合理论计算揭示了其调控机制. 本研究为2D磁性材料的载流子调控磁相变提供了新的见解, 并为研究2D磁体的电子结构与磁性之间的强相关性以及设计新型自旋电子器件开辟了一条途径.Electrical control of magnetism of two-dimensional (2D) antiferromagnetic (AFM) materials combines the advantages of controlling magnetism by purely electrical means, compatibility with semiconductor process, low energy consumption, heterogeneous integration of 2D materials with van der Waals (vdW) interface, and AFM materials with no stray field, resistance to external magnetic field interference, and high intrinsic frequency, and thus becomes a research focus in the field. The carrier concentration control is the main mechanism of electrical control of magnetism, and has been proved to be an effective way to control the magnetic properties of materials. The intralayer-antiferromagnetic materials have net-zero magnetic moments, and it is a challenging task to measure their regulated magnetic properties. Therefore, there is limited research on the electrical control of magnetism of intralayer-antiferromagnetic materials, and their potential mechanisms are not yet clear. Based on the diversity of organic cations, the present work systematically modulates the carrier concentrations of 2D intralayer-antiferromagnetic materials MPX3 (M = Mn, Fe, Ni; X = S, Se) by utilizing organic cations intercalation, and investigates the influence of electron doping on their magnetic properties. Phase transitions between AFM-ferrimagnetic (FIM)/ferromagnetic (FM) depending on carrier concentration changes are observed in MPX3 materials, and the corresponding regulation mechanism is revealed through theoretical calculations. This research provides new insights into the carrier-controlled magnetic phase transition of 2D magnetic materials, and opens up a pathway for studying the correlation between the electronic structure and magnetic properties of 2D magnets, and designing novel spintronic devices as well.
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Keywords:
- two-dimensional magnetic material /
- electrical control of magnetism /
- organic cations intercalation /
- magnetic phase transition
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图 1 (a) 电化学有机阳离子插层示意图以及THA+插层NiPS3前后的结构示意图[42]; 剥离后得到的薄层NiPS3 (b) 和THA+插层NiPS3 (c) 的原子力显微镜图像[42]
Fig. 1. Schematic diagram of electrochemical organic cation intercalation and the structure of NiPS3 and THA-NiPS3[42]; atomic force microscope images of exfoliated NiPS3 (b) and exfoliated intercalated THA-NiPS3 (c)[42].
图 2 有机阳离子插层NiPS3的实验结果[42] NiPS3 (a) 和THA-NiPS3 (b) 在H // ab 和H // c* 磁场作用下的M-T曲线, 实线和虚线分别为零场降温、场降温数据, (a)内插图为M与T的一阶微分 (dM/dT vs. T), c* 为垂直于ab平面的轴; (c) T = 5 K时, NiPS3和THA-NiPS3在H // ab磁场作用下M随H的依赖关系; (d) 矫顽场 (黑) 和剩余磁化强度 (红) 随温度的变化关系; (e) T = 10 K时, CTA-NiPS3在 H // ab磁场作用下M随H的依赖关系; (f) Ni(1), Ni(2)的磁矩以及净磁矩 (Ni(1)+Ni(2)) 随掺杂浓度的依赖关系
Fig. 2. Experimental results of organic cations intercalated NiPS3[42]: Temperature dependence of magnetization (M-T) of NiPS3 (a) and THA-NiPS3 (b) under magnetic fields H // ab (red) and H // c* (black), the solid and dashed lines represent zero-field cooled (ZFC) and field cooled (FC) data, respectively, the inset in (a) shows the first-order derivative of magnetization with temperature (dM/dT vs. T), c* represents axis perpendicular to the ab plane; (c) field dependence of magnetization (M-H) of NiPS3 and THA-NiPS3 under magnetic field H // ab at T = 5 K; (d) extracted coercive field Hc (black) and remnant magnetization Mr (red) of intercalated THA-NiPS3 as a function of temperature; (e) field dependence of magnetization (M-H) of CTA-NiPS3 under magnetic field H // ab at T = 10 K; (f) magnetic moments and net magnetic moments of Ni(1) and Ni(2) as a function of doping concentrations.
图 3 有机阳离子插层FePS3的实验结果 FePS3 (黑) 和THA-FePS3 (红) 在H // c* 磁场方向的M-T (a) 和M-H (b) 曲线, 实线和虚线分别为零场降温、场降温数据, (a)内插图为dM/dT vs T; THA-FePS3在H // c* 磁场方向、不同温度下的M-H曲线 (c); CTA-FePS3在H // c* 磁场下的M-T (d) 和M-H (e)曲线, (d)内插图为CTA-FePS3 的dM/dT vs. T; Fe(1), Fe(2)的磁矩以及净磁矩 (Fe(1)+Fe(2)) 随掺杂浓度的依赖关系 (f)
Fig. 3. Experimental results of organic cations intercalated FePS3: (a), (b) M-T (a) and M-H (b) curves of FePS3 (black) and THA-FePS3 (red) under magnetic fields H // c*, the solid and dashed lines represent ZFC and FC data, respectively, the inset in (a) shows the dM/dT vs. T of FePS3; M-H curves of THA-FePS3 under magnetic fields H // c* at different temperatures (c); M-T (d) and M-H (e) curves of intercalated CTA-FePS3 under magnetic fields H // c*, the inset in (d) shows the dM/dT vs. T of CTA-FePS3; magnetic moments and net magnetic moments of Fe(1) and Fe(2) as a function of doping concentrations (f).
图 4 有机阳离子插层FePSe3的实验结果 FePSe3 (黑)、TDA-FePSe3 (蓝) 以及THA-FePSe3 (红) 在H // c* 磁场方向的M-T (a) 和M-H (b) 曲线
Fig. 4. Experimental results of organic cations intercalated FePSe3: The M-T (a) and M-H (b) curves of FePSe3 (black), TDA-FePSe3 (blue) and THA-FePSe3 (red).
图 5 有机阳离子插层MnPS3的实验结果 MnPS3和THA-MnPS3在H // c* 磁场下的M-T (a), M-H (b) 以及H // ab磁场下的M-H (c) 曲线; (d) CTA-MnPS3在H // ab和H // c* 磁场下的M-H曲线. (b)—(d) 中的内插图分别为THA-MnPS3在H // c* (b), H // ab (c) 以及CTA-MnPS3在H // c*, H // ab (c) 小范围磁场下的M-H曲线
Fig. 5. Experimental results of organic cations intercalated MnPS3: M-T (a), M-H (b) curves under magnetic fields H // c* and M-H (c) curves under magnetic fields H // ab of MnPS3 and THA-MnPS3; (d) M-H curves of CTA-MnPS3 under magnetic fields H // ab and H // c*. The insets in (b)–(d) show the zoom-in images of M-H curves of THA-MnPS3 under H // c* (b), H // ab (c) and CTA-MnPS3 under magnetic fields H // ab (d) and H // c*, respectively.
图 6 有机阳离子插层MnPSe3的实验结果 (a) MnPSe3和TBA-MnPSe3在H // ab磁场方向的M-T 曲线; (b) T = 5 K时, TBA-MnPSe3在H // ab和H // c*磁场方向下的M-H曲线; (c) T = 5 K时, THA-MnPSe3在H // ab磁场下的M-H曲线; (d) Néel型AFM序与FM序的相对能量随掺杂浓度的变化
Fig. 6. Experimental results of organic cations intercalated MnPSe3: (a) M-T curves of MnPSe3 and TBA-MnPSe3 under magnetic fields H // ab; (b) M-H curves of TBA-MnPSe3 under magnetic fields H // ab and H // c* at T = 5 K; (c) M-H curve of THA-MnPSe3 under magnetic fields H // ab at T = 5 K; (d) the energy difference between the FM order and Néel AFM order as a function of doping concentration.
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