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Two-dimensional (2D) materials represented by graphene and molybdenum disulfide (MoS2) have attracted much attention in recent years due to their advantages in electrical, thermal, optical and mechanical properties. As a branch of 2D materials, 2D magnetic materials have special properties such as magnetic anisotropy and single-layer magnetic order. Especially, their magnetism can also be controlled by a variety of physical fields, and it possesses various physical properties and potential applications. Therefore, they have received widespread attention of researchers gradually. In this article, we summarize the types, synthesis methods, basic characteristics and characterization methods of 2D magnetic materials in detail, and the magnetism controlling of 2D magnetic materials as well. Finally, a simple outlook on the research directions and future challenges of 2D magnetic materials is given.
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Keywords:
- layered materials /
- magnetic materials /
- two-dimensional materials /
- two-dimensional magnetic materials /
- spintronics
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图 2 (a) Al2O3辅助机械剥离Fe3GeTe2薄片的示意图[32]; (b)在Al2O3薄膜上剥落Fe3GeTe2薄片的光学图片[32]; (c) CVD法合成FeTe纳米片的过程示意图[133]; (d)薄层FeTe纳米片的光学图片[133]; (e)超声液相剥离二维NiPS3的原理图[136]; (f) NiPS3薄片AFM图[136]; (g)分子束外延生长VSe2的原理图[143]; (h)单层VSe2的AFM图[143]
Fig. 2. (a) Schematic of Fe3GeTe2 exfoliated by Al2O3-assisted mechanical method[32]; (b) optical image of typical few-layer Fe3GeTe2 flakes exfoliated on top of an Al2O3 thin film[32]; (c) schematic illustration of FeTe nanosheet growth route by CVD[133]; (d) optical image of few-layer FeTe flakes[133]; (e) schematic illustration of NiPS3 growth route by liquid exfoliation[136]; (f) the AFM image of NiPS3 flakes[136]; (g) schematic illustration of VSe2 growth route by molecular beam epitaxy[143]; (h) the AFM image of monolayer VSe2[143].
图 3 (a)磁圆二色性原理图; (b)和(c)双层和三层CrI3自旋滤波器磁隧道结隧穿电流和反射磁圆二色性(RMCD)随外磁场(μ0H⊥)变化的函数关系曲线, 偏置电压分别为–290 mV和235 mV, 绿色(橙色)曲线表示递减(递增)磁场[59]; (d)不同温度下, 厚度为48 nm的Fe3GeTe2样品RMCD信号随磁场的变化关系[148]; (e)磁光克尔效应原理图; (f)双层Cr2Ge2Te6在不同温度下的克尔旋转信号[30]; (g) CrI3的磁光克尔转角与外加磁场的关系[31]; (h)不同温度下, Ta3FeS6纳米片极向磁光克尔随磁场的变化[151]; (i)在空气环境4个月前后, Ta3FeS6纳米片的MOKE信号随磁场变化[151]
Fig. 3. (a) Schematic diagram of magnetic circular dichroism; (b) and (c) tunneling current and reflective magnetic circular dichroism (RMCD) as a function of out-of-plane magnetic field (μ0H⊥) of double spin-filter magnetic tunnel junctions from bilayer and trilayer CrI3 at a selected bias voltage –290 mV and 235 mV, respectively, green (orange) curve corresponds to decreasing (increasing) magnetic field[59]; (d) comparison of RMCD sweeps for Fe3GeTe2 of thickness 48 nm as a function of the magnetic field, respectively[148]; (e) schematic diagram of magneto-optic Kerr effect; (f) Kerr rotation signals of bilayer Cr2Ge2Te6 vary with temperature[30]; (g) the magneto-optic Kerr signals of different CrI3 layers as a function of the magnetic field[31]; (h) the polar MOKE signal of Ta3FeS6 nanosheet as a function of magnetic field at different temperatures[151]; (i) MOKE signal of Ta3FeS6 nanosheet as a function of magnetic field acquired before and after 4 months aging under atmospheric conditions[151].
图 4 (a)磁力显微镜工作原理图; (b)单层/双层/三层VSe2薄片的MFM相位图像[106]; (c)图(b)中白色虚线对应的MFM图像的地形高度和MFM相位剖面图[106]; (d), (e) Fe3GeTe2分别在204和103 K时MFM图像, (d)的插图为300 K时的MFM图像, 图中白色矩形勾画出了相同的区域[148]; (f) 200 nm厚的CrI3薄片MFM信号作为磁场的函数图[155]; (g) 25 nm厚的CrI3薄片MFM信号作为磁场的函数图[155]; (h)表层和内层的堆叠顺序和自旋方向机理图[155]; (i)扫描隧道显微镜原理图[155]; (j)在热解石墨烯衬底上形成的单层VSe2扫描隧道显微镜图, 单层VSe2优先在阶梯边缘成核[156]; (k)在MoS2衬底上形成的单层VSe2扫描隧道显微镜图, VSe2在MoS2衬底上形成更均匀的单层膜[156]; (l) H型双层CrBr3层间的铁磁性耦合[61]; (m), (n) R型双层CrBr3层间的反铁磁性耦合[61]; (o)八面体的FeCl6单元(顶图)和六边形1T-FeCl2结构的示意图(底图)[157]; (p)具有两种非等边的六边形1T-FeCl2的STM图像[157]
Fig. 4. (a) Schematic diagram of magnetic force microscope (MFM); (b) MFM phase image of monolayer/bilayer/trilayer VSe2 flake[106]; (c) topography height and MFM phase profiles of the MFM image corresponding to the white dashed line in panel (b)[106]; (d), (e) MFM domain images for Fe3GeTe2 at 204 K and 103 K, respectively, inset of (d) is the MFM image at 300 K, and the white rectangles outline the same area[148]; (f) MFM signal as a function of magnetic field for 200 nm CrI3 flake; (g) MFM signal as a function of magnetic field for 25 nm CrI3 flake[155]; (h) illustration of the stacking orders and spin configurations insurface and inner layers[155]; (i) schematic diagram of scanning tunneling microscope[155]; (j) the STM image of VSe2 monolayer on HOPG, VSe2 monolayer islands preferentially nucleate at step edges on HOPG[156]; (k) the STM image of VSe2 monolayer on MoS2, the growth of VSe2 monolayer on MoS2 is more uniform and gives rise to larger monolayer islands[156]; (l) ferromagnetic coupling between H-type bilayer CrBr3 layers[61]; (m), (n) antiferromagnetic coupling between R-type bilayer CrBr3 layers[61]; (o) schematic illustration of an octahedral FeCl6 unit (top) and a hexagonal island of FeCl2 with a 1T structure (bottom)[157]; (p) STM image of 1T-FeCl2 with two non-equallateral hexagons[157].
图 5 (a)少层FePS3拉曼随温度依赖的mapping图[89]; (b)不同厚度下, 少层FePS3的P1a拉曼峰强度随温度的变化[89]; (c)薄层Cr2Ge2Te6样品
$ {\rm{E}}_{\rm{g}}^{1} $ 和$ {\rm{E}}_{\rm{g}}^{2} $ 拉曼峰随温度依赖的mapping图[158]; (d)不同温度下薄层Cr2Ge2Te6样品的原始拉曼图[158]; (e)单层CrI3偏振拉曼光谱随磁场的演化过程[62]; (f)单层CrI3的拉曼强度与磁圆二色的结果比较[62]; (g)双层CrI3偏振拉曼光谱随磁场的演化过程[62]; (h)双层CrI3的拉曼强度与磁圆二色的结果比较[62]; (i)反常霍尔效应的三种机制; (j)四层Fe3GeTe2的剩余霍尔电阻随温度的变化[32]; (k) 2 K温度下, 不同厚度的Fe3GeTe2纳米片的反常霍尔电阻Rxy随磁场的变化关系[111]; (l)不同温度下, 单个Fe3GeTe2的反常霍尔电阻随磁场的变化曲线[142]; (m)不同温度下, Fe3GeTe2/MnTe异质结的反常霍尔电阻随磁场的变化曲线[142]Fig. 5. (a) Temperature dependent Raman mapping of few layers FePS3 temperature dependent[89]; (b) the Raman intensity as a function of temperature for different thickness FePS3 of P1a mode[89]; (c) temperature dependent Raman spectra mapping for Cr2Ge2Te6 of the
$ {\rm{E}}_{\rm{g}}^{1} $ and$ {\rm{E}}_{\rm{g}}^{2} $ modes[158]; (d) the original Raman diagram of few layer Cr2Ge2Te6 at different temperatures[158]; (e) the evolution process of polarization Raman spectra for monolayer CrI3 with magnetic field[62]; (f) comparison of Raman strength and MCD for monolayer CrI3[62]; (g) the evolution process of polarization Raman spectra of bilayer CrI3 with magnetic field[62]; (h) comparison of Raman strength and MCD for bilayer CrI3[62]; (i) the mechanism of anomalous Hall effect; (j) the remanent Hall resistance${R}_{xy}^{\rm r}$ as a function of temperature for four-layer Fe3GeTe2[32]; (k) the Rxy as a function of magnetic field for different thickness Fe3GeTe2 nanosheet at 2 K[111]; (l) the Rxy as a function of magnetic field for Fe3GeTe2 heterojunction at different temperatures[142]; (m) the Rxy as a function of magnetic field for Fe3GeTe2/MnTe heterojunction at different temperatures[142]图 6 (a)顶部: 双栅极双层CrI3场效应器件的示意性侧视图, 其中双分子层CrI3被封装在少层石墨烯中, 石墨烯作为平面外输运测量的源极和漏极; 底部: 单双层样品器件的光学显微图. 左下图, 用于单层CrI3的磁化率测量的电极结构, 比例尺为50 μm; 右下图, 用于双层CrI3的磁化率测量的电极结构, 比例尺为20 μm; 红色虚线为双层样品的边界[51]. (b)单层CrI3的磁性随栅极电压(底轴)和诱导掺杂密度(顶轴)变化的函数[51]. (c)双层CrI3中, 在4 K下掺杂密度-磁场相图[51]. (d)少数层h-BN/Cr2Ge2Te6/h-BN范德瓦耳斯异质结器件[94]. (e) 40 K, 负门电压下磁光克尔角随磁场的变化[94]. (f) 40 K, 正门电压下磁光克尔角随磁场的变化[94]
Fig. 6. (a) Top: A schematic side view of a dual-gate bilayer CrI3 field-effect device. Bilayer CrI3 is encapsulated in few-layer graphene, which also serves as source and drain electrodes for out-of plane transport measurements. Bottom: An optical micrograph for monolayer and bilayer CrI3 sample devices. Scale bars, 50 μm (left panel) and 20 μm (right panel). The metallic ring structure (left panel) is used to create a magnetic field for the susceptibility measurement for monolayer CrI3. The electrode structure (right panel) is used for the susceptibility measurement for bilayer CrI3, the red dashed line marks the boundary of a bilayer sample in the right panel[51]. (b) The magnetic properties of monolayer CrI3 as a function of gate voltage (bottom axis) and induced doping density (top axis)[51]. (c) Doping density-magnetic field phase diagram at 4 K for monolayer CrI3[51]. (d) Schematic diagram of a few-layered h-BN/Cr2Ge2Te6/h-BN heterojunction[94]. (e) Kerr angle as a function of magnetic field at 40 K for negative gate voltages[94]. (f) Kerr angle as a function of magnetic field at 40 K for positive gate voltages[94].
图 7 (a) Fe3GeTe2的磁结构随厚度和温度的变化[32]; (b)在三层Fe3GeTe2样品中获得的电导与门电压的关系, 测试温度为330 K, 插图为Fe3GeTe2离子场晶体管[32]示意图, 其中S, D分别代表源电极和漏电极, Vn表示探测电压, 固态栅极覆盖了样品和周围电极[32]; (c)三层Fe3GeTe2在特定栅压下(T = 10 K和T = 240 K)的反常霍尔电阻随磁场的变化曲线[32]; (d)三层Fe3GeTe2温度和栅压的相图[32]; (e)在栅极电压Vg = 2.1 V时, 四层Fe3GeTe2在室温附近的反常霍尔电阻随磁场的变化[32]
Fig. 7. (a) Phase diagram of Fe3GeTe2 (FGT) as a function of layer number and temperature[32]. (b) conductance as a function of gate voltage Vg measured in a trilayer FGT device. Data are obtained at T = 330 K, the inset shows a schematic of the FGT device structure and measurement setup, S and D label the source and drain electrodes, respectively, and Vn labels the voltage probes. The solid electrolyte covers both the FGT flake and the side gate[32]. (c) Rxy as a function of external magnetic field recorded at representative gate voltages obtained at T = 10 K and T = 240 K[32]; (d) the phase diagram of the trilayer FGT sample as a function of the gate voltage and temperature[32]; (e) Rxy of four-layer FGT as a function of magnetic field under a gate voltage of Vg = 2.1 V at room temperature[32].
图 8 (a) CrI3晶体结构, 分别为单斜相(左)和六方相(右)[164]; (b) CrI3隧道结的光学图片[164]; (c) CrI3隧道结的侧面示意图[164]; (d), (e) 在施加压力前(d)后(e)两个2层(2L)和两个5层(5L)区域, 在3.5 K时, MCD随磁场的变化[164]; (f)双层CrI3隧道结中, 不同压力下, 隧道电流随磁场的变化[165]; (g)双层CrI3隧道结施加压力前后RMCD信号随磁场的变化[165]; (h)高压实验装置示意图[165]; (i), (j), (k)三层CrI3中其中任意三点的RMCD随磁场的变化[165]
Fig. 8. (a) Crystal structure of CrI3, the monoclinic phase (left) and the hexagonal phase (right)[164]; (b) the optical image of CrI3 tunnel junction[164]; (c) the side view of the CrI3 tunnel junction[164]; (d), (e) the MCD for 2L and 5L CrI3 before (d) and after (e) pressured as a function of the magnetic field under the temperature of 3.5 K[164]; (f) the tunnel current for bilayer CrI3 as a function of the magnetic field under different pressures[165]; (g) the RMCD signal for bilayer CrI3 tunnel junction as a function of the magnetic field before and after pressured[165]; (h) schematic of high-pressure experimental set-up[165]; (i), (j), (k) the RMCD signal for any three points of trilayer CrI3 as a function of the magnetic field[165].
图 9 (a) Fe3GeTe2及FePS3/Fe3GeTe2异质结的克尔旋转角随磁场的变化曲线[168]; (b) Fe3GeTe2及FePS3/Fe3GeTe2/FePS3异质结的克尔旋转角随磁场的变化曲线[168]; (c)双层反铁磁/铁磁异质结FePS3/Fe3GeTe2和(d)三层反铁磁/铁磁/反铁磁异质结FePS3/Fe3GeTe2/FePS3表现出的交换偏置现象[168]; (e) Fe3GeTe2及FePS3/Fe3GeTe2异质结的克尔旋转角随温度的变化曲线[168]; (f) Fe3GeTe2及FePS3/Fe3GeTe2/FePS3异质结的克尔旋转角随温度的变化曲线[168]
Fig. 9. (a) The Kerr rotations as a function of magnetic field for Fe3GeTe2 (FGT, yellow curves) and FePS3/Fe3GeTe2 (FPS/FGT, green curves)[168]; (b) the Kerr rotations as a function of magnetic field for FGT (yellow curves) and FePS3/Fe3GeTe2/FePS3 (FPS/FGT/FPS, green curves)[168]; the exchange bias phenomenon for (c) bilayer antiferromagnetic/ferromagnetic heterojunction FPS/FGT and (d) trilayer antiferromagnetic/ferromagnetic/antiferromagnetic heterojunction FPS/FGT/FPS under the different external magnetic fields[168]; (e) the Kerr rotations as a function of the temperature for FGT (red curve) and FPS/FGT (blue curve)[168]; (f) the Kerr rotation as a function of the temperature for FGT (red curve) and FPS/FGT/FPS (blue curve)[168].
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