二维材料/铁电异质结构的研究进展

王慧; 徐萌; 郑仁奎

doi:10.7498/aps.69.20191486

摘要

二维材料是一类具有原子层厚度的层状材料, 拥有独特的电学、磁学、光学和力学性能. 以石墨烯和过渡金属硫族化合物为代表的二维材料展现出迁移率高、能带可调、可见光透过率高等特点, 是近年来微纳科学领域的前沿热点. 将二维材料与各种功能材料, 如SiO₂绝缘体、半导体、金属、有机化合物等结合, 可以深化和拓宽二维材料的基础研究和应用. 其中, 铁电材料因具有自发极化、高介电常数、高压电系数等优点吸引了众多研究者的目光. 二维/铁电复合材料很好地兼顾了二者的优点, 不仅包含了磁电耦合效应、铁电场效应、晶格应变效应、隧穿效应、光电效应、光致发光效应等丰富的物理现象, 而且在多态存储器、隧穿晶体管、光电二极管、太阳能电池、超级电容器、热释电红外探测器等器件中有广阔的应用前景, 引起了学术界的广泛关注. 本文选取典型的二维/铁电复合材料, 重点介绍了这类材料界面处的物理机制、材料的性能以及应用前景, 并对二维/铁电复合材料的研究进行了展望.

关键词:

Abstract

With the rapid development of microelectronic integration technology, the miniaturization, integration and multifunction of electronic devices are becoming a general trend. Two-dimensional materials are a class of layered material with atomic layer thickness, and have unique electrical, magnetic, optical and mechanical properties. The co-existence of the weak van der Waals force between layers and the strong covalent bonding within layers makes the two-dimensional material very suitable for the miniature design of new-generation multifunctional electronic devices. Two-dimensional materials, represented by graphene and transition metal chalcogenides, exhibit high mobility, adjustable energy band and high visible light transmittance, and thus having become the frontier hotspots in the field of micro-nanoscience in recent years. Synergy between two-dimensional materials and various functional materials such as SiO₂ insulator, semiconductor, metal and organic compound may lead to new properties and device applications, thus can deepen and expand the basic research and application of two-dimensional materials. Among them, ferroelectric materials have received much attention because of their spontaneous polarizations, high dielectric constants, and high piezoelectric coefficients. The two-dimensional ferroelectric composites well have the advantages of the two, i.e. they not only contain a variety of rich phenomena such as the magnetoelectric coupling effect, ferroelectric field effect and lattice strain effect, tunneling effect, photoelectric effect, and photoluminescence effect, but also have broad applications in devices such as multi-state memories, tunneling transistors, photoelectric diodes, solar cells, super capacitors, and pyroelectric infrared detectors, which have attracted wide concern from academia and industry. To better understand the combination of two-dimensional thin films with ferroelectric substrates and provide a holistic view, we review the researches of several typical two-dimensional film/ferroelectrics heterostructures in this article. First, two-dimensional materials and ferroelectric materials are introduced. Then, the physical mechanism at the interface is briefly illustrated. After that, several typical two-dimensional film/ferroelectrics heterostructures are mainly introduced. The ferroelectric materials including Pb(Zr_1–xTi_x)O₃, (1–x)PbMg_1/3Nb_2/3O₃–xPbTiO₃, P(VDF-TrFE), are mainly summarized, and other ferroelectric materials such as P(VDF-TrFE-CFE), BaTiO₃, BiFeO₃, PbTiO₃, CuInP₂S₆, HfO₂ are briefly involved. The future research emphasis of the two-dimensional materials/ferroelectrics composites is also suggested at the end of the article. This review will present a significant reference to the future design of miniature and multifunctional devices.

Keywords:

作者及机构信息

1.
南昌大学, 材料科学与工程学院, 南昌　330031

2.
中国科学院上海硅酸盐研究所, 高性能陶瓷和超微结构国家重点实验室, 上海　200050

通信作者: 郑仁奎, zrk@ustc.edu

基金项目: 国家自然科学基金(批准号: 51572278, 11974155)资助的课题

Authors and contacts

1.
School of Materials Science and Engineering, Nanchang University, Nanchang 330031, China

2.
State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China

Corresponding author: Zheng Ren-Kui, zrk@ustc.edu

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 51572278, 11974155)

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施引文献

图 1 结构示意图　(a) 中间插层的二维材料^[10]; (b) 石墨烯/MoS₂/PMN-PT异质结^[11]; (c) MoS₂/P(VDF-TrFE)/SiO₂/Si异质结^[5]

Fig. 1. The schematic diagrams: (a) 2D Materials with intercalation^[10]; (b) graphene/MoS₂/PMN-PT heterostructure^[11]; (c) MoS₂/P(VDF-TrFE)/SiO₂/Si heterostructure^[5].

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图 2 (a) PMN-PT未被极化时具有8个自发极化方向: r1⁺, r2⁺, r3⁺, r4⁺, r1^–, r2^–, r3^–, r4^–^[12]; (b) PMN-PT(001)单晶的应变-电场曲线^[13]; (c) 不同应变状态下, MoS₂的光致发光谱^[11]; (d) 不同外加电场下, PMN-PT(011)单晶的应变-电场曲线^[15]

Fig. 2. (a) The eight possible polarization directions for an unpoled PMN-PT single crystal: r1⁺, r2⁺, r3⁺, r4⁺, r1^–, r2^–, r3^–, r4^–^[12]; (b) ε_xx – E curves for PMN-PT(001) single crystals^[13]; (c) photoluminescence spectra of the MoS₂ under various strains^[11]; (d) ε_xx – E curves for PMN-PT(011) single crystals^[15].

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图 3 (a) PMN-PT铁电单晶衬底的极化-电场(P-E)曲线, 及外加电场下石墨烯/PMN-PT铁电场效应晶体管的界面电荷效应示意图^[16]; (b) 石墨烯/PMN-PT铁电场效应晶体管的I_ds–V_g曲线^[16]

Fig. 3. (a) Polarization-Electric field (P-E) hysteresis loop of PMN-PT substrate, and schematic diagrams of interface charge effects in graphene/PMN-PT FeFET^[16]; (b) the I_ds–V_g curves of graphene on PMN-PT^[16].

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图 4 (a) 石墨烯/PZT/STO异质结的示意图^[20]; (b) 300 nm PZT上的多层石墨烯AFM图^[21]; (c) 不同栅压走向下, 石墨烯/PZT FeFET的电阻率ρ随栅压V_g的变化曲线^[21]

Fig. 4. (a) Schematic of the graphene/PZT/STO heterostructure^[20]; (b) AFM image of a multilayer graphene sheet on a 300 nm PZT film^[21]; (c) the channel resistivity of graphene/PZT FeFET as a function of the gate voltage with different memory operation^[21].

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图 5 (a) 机械剥离-石墨烯/PZT FeFET的I_DS-V_G曲线^[23]; (b) CVD-石墨烯/PZT FeFET的I_DS-V_G曲线^[23]; (c) V_DS = 50 mV时, 石墨烯/PZT FeFET中的I_DS-V_G曲线^[25]; (d) 不同栅压下, 真空和空气中分别测得的I_DS-V_G曲线^[25]

Fig. 5. (a) I_DS-V_G characteristics of the exfoliated-graphene/PZT FeFET^[23]; (b) I_DS-V_G characteristics of the CVD-graphene/PZT FeFET^[23]; (c) I_DS-V_G of the graphene/PZT FeFET under a drain voltage at 50 mV^[25]; (d) drain current as a function of gate voltage of graphene/PZT FeFET in air and vacuum, respectively^[25].

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图 6 (a) PZT处于不同极化状态时, 石墨烯/PZT的I_DS-V_G曲线^[28]; (b) 在施加V_G = –6 V和V_G = 6 V的擦写电压后, 石墨烯/PZT FET分别处于“ON”态和“OFF”时的漏极电流随时间的变化曲线^[28]; (c) 石墨烯/PZT FET结构示意图^[29]; (d) 在PZT薄膜翻转为向上和向下的极化状态后, 分别在真空中放置250 s和24 h后测得的I_d-V_G曲线^[29]

Fig. 6. (a) Scheme of the electrical measurements of graphene/PZT FeFETs at different polarization state of PZT^[28]; (b) after application of the write (V_G = –6 V) or erase (V_G = +6 V) voltages, the ON and OFF drain–source currents at the read voltage (V_G = 0) and an auxiliary pulse (V_G = –1.25 V) were measured as a function of time^[28]; (c) schematic device structure of the graphene/PZT FeFET^[29]; (d) I_d-V_G characteristics measured in vacuum 250 s and 24 h after switching for both the UP and DOWN polarization states^[29].

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图 7 (a)对石墨烯/PMN-PT施加电场的示意图^[33]; (b) 石墨烯的D, G, 2D和2D’峰位随面内应变的变化曲线^[33]; (c) 石墨烯/PMN-PT异质结构示意图^[34]; (d) 不同外场下PMN-PT(002)峰的XRD图^[34]; (e) 不同外场下石墨烯的2D拉曼峰图^[34]

Fig. 7. (a) Schematic of the electro-mechanical device used to apply in-plane biaxial strain to the graphene^[33]; (b) D, G, 2D and 2D’ peaks plotted as a function of the biaxial strain ε_||^[33]; (c) schematic of graphene/PMNPT heterostructure^[34]; (d) the PMN-PT (002) peaks of XRD 2θ scanning patterns with different bias voltage^[34]; (e) 2D peaks of graphene under different bias voltage^[34].

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图 8 (a) 石墨烯/PMN-PT FeFET的I_ds-V_g曲线^[16]; (b) 石墨烯的载流子浓度随栅压的变化曲线^[35]; (c) 石墨烯/h-BN/PMN-PT FET示意图^[36]; (d) 不同栅压范围下的I_ds-V_g曲线^[36]

Fig. 8. (a) The I_ds-V_g curves of graphene on PMN-PT^[16]; (b) charge carrier density of graphene on PMN-PT as a function of the gate voltage^[35]; (c) schematic diagrams of the graphene/h-BN/PMN-PT FET^[36]; (d) I_ds-V_g curves of graphene at different gate-voltage sweep ranges^[36].

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图 9 (a) 石墨烯/P(VDF-TrFE)的电位移D和P(VDF-TrFE)的电位移D’随外加电场的变化曲线^[42]; (b) 石墨烯/P(VDF-TrFE)的电阻持久性能^[43]; (c) 石墨烯/P(VDF-TrFE)柔性透明导电器件光学照片^[44]; (d) 石墨烯/P(VDF-TrFE)的I_sd和I_tg随栅极电压的变化曲线^[46]

Fig. 9. (a) The electric displacement field D of the graphene/P(VDF-TrFE) FeFET and D’ of P(VDF-TrFE) thin film as a function of the applied electric field^[42]; (b) the resistance endurance property of the graphene/P(VDF-TrFE) FeFET^[43]; (c) optical image of the flexible transparent graphene/P(VDF-TrFE) FeFET device^[44]; (d) I_sd and I_tg vs V_tg curves of the graphene/P(VDF-TrFE) FeFET^[46].

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图 10 (a) 基于石墨烯/P(VDF-TrFE)/石墨烯复合结构的声压器件和测试回路照片^[47]; (b) 基于石墨烯/P(VDF-TrFE)/石墨烯复合结构的声压驱动器和纳米发电机的示意图^[47]; (c) 基于P(VDF-TrFE)/石墨烯复合结构的发电机和话筒的示意图和照片^[48]; (d) 基于P(VDF-TrFE)/石墨烯复合结构的压力测试装置^[49]; (e) 当被粘贴在手上时P(VDF-TrFE)/PMN-PT/GO薄膜的短路电流^[51]; (f) 用PFM探针在GO/P(VDF-TrFE)上写入和读取数据的示意图^[52]

Fig. 10. (a) Photograph of the graphene/P(VDF-TrFE)/graphene based acoustic device and the measurement circuit^[47]; (b) schematic depiction showing graphene/P(VDF-TrFE)/graphene-based device can work as an actuator as well as a nanogenerator^[47]; (c) schematics and photograph of graphene/PVDF/graphene based generator and loudspeaker^[48]; (d) photographic image of the pressure measurement setup showing the pressurized gas inlet, the sensor mounting, and the data acquisition system^[49]; (e) short-circuit current of the P(VDF-TrFE)/PMN-PT/GO film when attached on the human hand^[51]; (f) a schematic of data writing and reading on GO/P(VDF-TrFE) Multilayer film by a PFM tip^[52].

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图 11 (a) 以PZT为背栅的MoS₂ FET示意图^[57]; (b) MoS₂/PZT FET的转移特性曲线, 插图为存储窗口随最大扫描电压的变化曲线^[57]; (c) 不同表面粗糙度的MoS₂/PZT FET转移特性曲线^[59]; (d) MoS₂/PZT FET在不同温度下的转移特性曲线^[61]

Fig. 11. (a) Schematic diagram of the PZT back gated MoS₂ FeFET^[57]; (b) the transfer curves of MoS₂/PZT FET. Memory window variation with increasing V_G sweep range as shown in the inset^[57]; (c) the transfer characteristics of MoS₂ transistors fabricated on PZT films with different surface qualities^[59]; (d) the I_ds-V_gs curves of MoS₂/PZT FETs under different temperatures rising from 300 to 380 K and V_gmax at 8 V^[61].

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图 12 (a) 同一个MoS₂/PZT FeFET在加栅压的同时和加栅压静置5 min后的I_DS-V_G曲线^[63]; (b) 光照对FeFET器件开关持续能力的影响^[63]; (c) 以向下的铁电畴为栅极的MoS₂-PZT FeFET的PFM相位图^[64]; (d) 不同数量导电通道的I_DS-V_DS曲线^[64]

Fig. 12. (a) I_DS-V_G characteristics for the same MoS₂/PZT FeFET measured while V_G was applied and 5 min after the corresponding gate voltages were applied, respectively^[63]; (b) effect of light illumination on the retention properties of the FeFET^[63]; (c) PFM phase images of a MoS₂-PZT FeFET with one and three conductive paths gated by the domains with the downward polarization^[64]; (d) I_DS-V_DS curves for different numbers of conductive paths^[64].

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图 13 (a) 2D/PZT FeFET的结构示意图^[65]; (b) PZT不同极化态对WSe₂ PL光谱的影响^[65]; (c, d) PZT不同极化态下, WSe₂的PL发光分布图^[65]; (e) PZT不同极化态下, WS₂的PL发光分布图^[66]; (f) PZT不同极化态下, WS₂的PL光谱及拟合曲线^[66]

Fig. 13. (a) Device schematic of the 2D TMD/PZT heterostructure^[65]; (b) effect of different polarization state for PZT on the PL spectra of WSe₂^[65]; (c, d) the maps of integrated PL intensity under down- and up-polarized states, respectively^[64]; (e) PL peak intensity map obtained from the WS₂ monolayer over a 30 × 30 μm² area under different polarized states^[66]; (f) raw PL spectra (solid black line) and fits (dashed green line) using two Lorentzians centered at 2.01 eV (red line) and 1.99 eV (blue line)^[66].

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图 14 (a) MoS₂/PMN-PT的结构示意图^[11]; (b) 不同应力作用下MoS₂的光致发光光谱^[11]; (c) 不同应力作用下MoS₂的能带示意图^[11]; (d) PMN-PT/MoS₂ FET的结构示意图^[67]; (e) 无栅极电压时, PMN-PT/MoS₂ FET在不同强度光照下的伏安特性曲线^[67]; (f) PMN-PT/MoS₂ FET的沟道电流随红外光照开/关的响应曲线^[67]

Fig. 14. (a) Schematic diagram of MoS₂/PMN-PT composite^[11]; (b) in-situ photoluminescence (PL) spectra of MoS₂/PMN-PT composite under different strain states^[11]; (c) calculated band structure of trilayer MoS₂ as a function of the strain^[11]; (d) schematic of MoS₂/PMN-PT FET^[67]; (e) I_ds – V_ds curves of MoS₂/PMN-PT FET under different light illumination with gate voltage V_G = 0 V^[67]; (f) the time-resolved photocurrent in response to IR on/off at an irradiance of 6 mW/mm²^[67].

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图 15 (a) 磁性、半导体性、压电性相互耦合示意图^[68]; (b) MoS₂基MIPG-FET的3D示意图^[68]; (c) PMN-PT正向极化态下, MoS₂基MIPG-FET对H = 33 mT的瞬态响应^[68]; (d) PMN-PT负向极化态下, MoS₂基MIPG-FET对H = 42 mT的瞬态响应^[68]

Fig. 15. (a) Schematic showing the three-phase coupling among magnetism, semiconductor, and piezoelectricity^[68]; (b) 3D schematic illustration of an MoS₂-based MIPG-FET^[68]; (c) transient response of the MIPG-FET at H = 33 mT at Pr⁺ state^[68]; (d) transient response of the MIPG-FET at H = 42 mT at Pr^– state^[68].

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图 16 (a) MoS₂基FET的3D模型图^[69]; (b) 亚阈值摆幅和电导随沟道长度的变化曲线^[73]; (c) 以P(VDF-TrFE)为顶栅的MoSe₂基FeFET的3D模型图^[74]; (b) MoSe₂基FeFET在写入和擦除状态下的持久性能^[74]

Fig. 16. (a) Schematic 3D top-view of the MoS₂-FET^[69]; (b) Detailed plots of SS and g_m as a function of L_ch^[73]; (c) 3D schematic diagram of the P(VDF-TrFE) top gated MoSe₂ FeFET^[74]; (d) retention performance of this device at the write and erase states^[74].

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图 17 (a) P(VDF-TrFE)顶栅MoS₂光电FET在光照下的3D模型图^[75]; (b) P(VDF-TrFE)处于不同极化状态时, MoS₂光电FET的光开关行为^[75]; (c) 以P(VDF-TrFE)顶栅并中插HfO₂薄膜的MoTe₂光电FET示意图^[77]; (d) 在黑暗及不同光照强度(520−1550 nm)下, In₂Se₃光电FET的伏安特性曲线^[76]

Fig. 17. (a) 3D schematic diagram of the P(VDF-TrFE) top gated MoS₂ phtodetector with light beam^[75]; (b) photoswitching behavior of ferroelectric polarization gating triple-layer MoS₂ photodetector at three states^[75]; (c) the schematic diagram of back-gate MoTe₂ FET in which HfO₂ of 30 nm is deposited on MoTe₂ before coating P(VDF-TrFE) polymer^[77]; (d) drain-source characteristics of the In₂Se₃ phtodetector in the dark and under different illuminating light wavelength (520−1550 nm)^[76].

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图 18 (a) 单层薄膜在LiNbO₃铁电畴上择优生长的光学照片和在单极化域上的双层^[80]; (b) MoSe₂和(c) WSe₂的光致发光分布图^[81]; (d) 在MoS₂/BaTiO₃/SrRuO₃上的测试示意图^[85]; (e−f) MoS₂/BaTiO₃/SrRuO₃在紫外光照前后的PFM相图^[85]

Fig. 18. (a) The optical micrograph shows preferential growth of single-layer MoS₂ on LiNbO₃ domains^[80]; PL mapping of exfoliated monolayer (b) MoSe₂ and (c) WSe₂ on a single polarized domain. The gold dashed line indicates one single dipole^[81]; (d) a sketch of the experiment geometry in MoS₂/BaTiO₃/SrRuO₃ junctions^[85]; (e)−(f) PFM phase images of MoS₂/BaTiO₃/SrRuO₃ junctions acquired in the dark before and after UV illumination^[85].

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图 19 (a) PMN-PT衬底分别处于P_r⁺, P_r^–态时, CBS薄膜的电阻R随温度T的变化曲线, 插图: CBS薄膜的载流子浓度随温度T的变化曲线^[92]; (b) PMN-PT衬底极化翻转引起的CBS薄膜费米能级移动的示意图^[92]; (c) P(VDF-TrFE)/BP/MoS₂/SiO₂/Si结构FeFET示意图^[94]; (d) 在BP/PZT/LNO/SiO₂/Si结构的FeFET中光电存储原理图^[95]; (e) 在BP/PZT/LNO/SiO₂/Si结构存储器中的“电写光读”动态循环曲线^[95]

Fig. 19. (a) The resistance R as a function of the temperature T for the CBS films at P_r⁺ state and P_r^– state, respectively^[92]; (b) schematic band diagrams of the Fermi level shift induced by polarization Switching^[92]; (c) schematic of dual-gated P(VDF-TrFE)/BP/MoS₂/SiO₂/Si FeFET^[94]; (d) schematic illustration of the photoelectric memory in FeFET with BP/PZT heterostructure fabricated on LNO/SiO₂/Si substrate^[95]; (e) dynamic cycles of the “electrical writing-optical reading” process of the BP/PZT/LNO/SiO₂/Si memory^[95]

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