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HfO2基铁电薄膜的结构、性能调控及典型器件应用

袁国亮 ,  王琛皓 ,  唐文彬 ,  张睿 ,  陆旭兵

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HfO2基铁电薄膜的结构、性能调控及典型器件应用

袁国亮, 王琛皓, 唐文彬, 张睿, 陆旭兵
物理学报, 2023, 72(9): 097703.
doi: 10.7498/aps.72.20222221

Structure, performance regulation and typical device applications of HfO2-based ferroelectric films

Yuan Guo-Liang, Wang Chen-Hao, Tang Wen-Bin, Zhang Rui, Lu Xu-Bing
Acta Phys. Sin., 2023, 72(9): 097703.
doi: 10.7498/aps.72.20222221
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  • 摘要

    大数据、物联网和人工智能的快速发展对存储芯片、逻辑芯片和其他电子元器件的性能提出了越来越高的要求. 本文介绍了HfO2基铁电薄膜的铁电性起源, 通过掺杂元素改变晶体结构的对称性或引入适量的氧空位来降低相转变的能垒可以增强HfO2基薄膜的铁电性, 在衬底和电极之间引入应力、减小薄膜厚度、构建纳米层结构和降低退火温度等方法也可以稳定铁电相. 与钙钛矿氧化物铁电薄膜相比, HfO2基铁电薄膜具有与现有半导体工艺兼容性更强和在纳米级厚度下铁电性强等优点. 铁电存储器件理论上可以达到闪存的存储密度, 读写次数超过1010次, 同时具有读写速度快、低操作电压和低功耗等优点. 此外, 还总结了HfO2基薄膜在负电容晶体管、铁电隧道结、神经形态计算和反铁电储能等方面的主要研究成果. 最后, 讨论了HfO2基铁电薄膜器件当前面临的挑战和未来的机遇.

    Abstract

    The rapid developments of big data, the internet of things, and artificial intelligence have put forward more and more requirements for memory chips, logic chips and other electronic components. This study introduces the ferroelectric origin of HfO2-based ferroelectric film and explains how element doping, defects, stresses, surfaces and interfaces, regulate and enhance the ferroelectric polarization of the film. It is widely accepted that the ferroelectricity of HfO2-based ferroelectric film originates from the metastable tetragonal phase. The ferroelectricity of the HfO2-based film can be enhanced by doping some elements such as Zr, Si, Al, Gd, La, and Ta, thereby affecting the crystal structure symmetry. The introduction of an appropriate number of oxygen vacancy defects can reduce the potential barrier of phase transition between the tetragonal phase and the monoclinic phase, making the monoclinic phase easy to transition to tetragonal ferroelectric phase. The stability of the ferroelectric phase can be improved by some methods, including forming the stress between the substrate and electrode, reducing the film thickness, constructing a nanolayered structure, and reducing the annealing temperature. Compared with perovskite oxide ferroelectric thin films, HfO2-based films have the advantages of good complementary-metal-oxide-semiconductor compatibility and strong ferroelectricity at nanometer thickness, so they are expected to be used in ferroelectric memory. The HfO2-based 1T1C memory has the advantages of fast reading and writing speed, more than reading and writing 1012 times, and high storage density, and it is the fast reading and writing speed that the only commercial ferroelectric memory possesses at present. The 1T ferroelectric field effect transistor memory has the advantages of non-destructive reading and high storage density. Theoretically, these memories can achieve the same storage density as flash memory, more than reading 1010 times, the fast reading/writing speed, low operating voltage, and low power consumption, simultaneously. Besides, ferroelectric negative capacitance transistor can obtain a subthreshold swing lower than 60 mV/dec, which greatly reduces the power consumption of integrated circuits and provides an excellent solution for further reducing the size of transistors. Ferroelectric tunnel junction has the advantages of small size and easy integration since the tunneling current can be largely adjusted through ferroelectric polarization switching. In addition, the HfO2-based field effect transistors can be used to simulate biological synapses for applications in neural morphology calculations. Moreover, the HfO2-based films also have broad application prospects in antiferroelectric energy storage, capacitor dielectric energy storage, memristor, piezoelectric, and pyroelectric devices, etc. Finally, the current challenges and future opportunities of the HfO2-based thin films and devices are analyzed.

    作者及机构信息

    • 1.

      南京理工大学材料科学与工程学院, 南京　210094

    • 2.

      华南师范大学华南先进光电子研究院, 广州　510006

      • 通信作者: 袁国亮, yuanguoliang@njust.edu.cn ; 陆旭兵, luxubing@m.scnu.edu.cn
    • 基金项目: 国家自然科学基金(批准号: 92263105, 62174059)和中央高校基本科研业务费专项资金(批准号: 30921013108)资助的课题.

    Authors and contacts

    • 1.

      School of Material Science and Engineering, Nanjing University of Science and Technology, Nanjing 210094, China

    • 2.

      South China Academy of Advanced Optoelectronics, South China Normal University, Guangzhou 510006, China

      • Corresponding author: Yuan Guo-Liang, yuanguoliang@njust.edu.cn ; Lu Xu-Bing, luxubing@m.scnu.edu.cn
    • Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 92263105, 62174059) and the Fundamental Research Funds for the Central Universities, China (Grant No. 30921013108).

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  • 图 1  HfO2基薄膜可以具有优异的铁电、压电、介电、反铁电和热释电性, 在很多领域具有广泛的应用前景

    Fig. 1.  HfO2 based films exhibit excellent ferroelectric, piezoelectric, dielectric, antiferroelectric and pyroelectric properties, so they have wide application prospects in many fields.

    下载: 全尺寸图片 幻灯片

    图 2  (a)—(f) HfO2晶体结构示意图, 其中(a) m相, (b) t相, (c) c相, (d) oI相[24]以及(e)极化向下和(f)极化向上的oIII相; (g) Hf0.5Zr0.5O2薄膜的自由能曲线; (h) 不同晶粒尺寸的Hf0.5Zr0.5O2 薄膜在不同温度下的相图[33]; (i) Hf0.93Y0.07O2热处理过程中的相变流程图[36]

    Fig. 2.  Crystal structures of HfO2 with (a) m phase, (b) t phase, (c) c phase, (d) oI phase[24], oIII phase with (e) downward polarization and (f) upward polarization; (g) free energy curve of Hf0.5Zr0.5O2 films; (h) phase diagrams of Hf0.5Zr0.5O2 films with different grain sizes at different temperatures[33]; (i) phase evolution during Hf0.93Y0.07O2 heat treatment [36].

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    图 3  (a) Hf1–xZrxO2薄膜的P-E和εr-E曲线[19]; (b) Hf1–xYxO2–δ薄膜的P-V曲线[28]; (c) Hf1–xAxO2 (A = Si, Al, Y, Gd, La或Sr)薄膜的Pr值随晶体半径和A掺杂量变化的等值线图[18]

    Fig. 3.  (a) P-E and εr-E curve of Hf1–xZrxO2 films[19]; (b) P-V curves of Hf1–xYxO2–δ films[28]; (c) contour plot of the Pr of Hf1–xAxO2 (A = Si, Al, Y, Gd, La and Sr) as a function of crystal radius and dopant content[18].

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    图 4  (a)退火温度为300—500 ℃时Hf0.5Zr0.5O2薄膜的P-E曲线; (b) TiN电极的厚度为45—180 nm时Hf0.5Zr0.5O2薄膜的P-E曲线[71]; (c)不同电极的Hf0.5Zr0.5O2的o相比例; (d)不同电极的Hf0.5Zr0.5O2的2Pr值[74]; (e), (f)有无VOx上电极的Hf0.5Zr0.5O2薄膜的P-V曲线和不同次数铁电极化翻转后的Pr[76]

    Fig. 4.  P-E curves of Hf0.5Zr0.5O2 film at (a) 300–500 ℃ annealing temperatures or with (b) 45–180 nm thick TiN electrode[71]. (c) o-phase ratio and (d) 2Pr of Hf0.5Zr0.5O2 with different electrodes[74]. (e) P-E curves of Hf0.5Zr0.5O2 film with or without VOx top electrode[76]. (f) Pr values of Hf0.5Zr0.5O2 film with or without VOx top electrode after different polarization switching cycles 76].

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    图 5  (a) ALD和PVD制备的HfO2薄膜的2Pr与厚度的关系[95]; (b), (c)不同膜厚的(b) Hf0.5Zr0.5O2薄膜和(c) Hf0.5Zr0.5O2/Al2O3/Hf0.5Zr0.5O2薄膜的P-E曲线[101]; (d) 4×(HfO2(1 nm)/ ZrO2(1 nm))薄膜和8 nm Hf0.5Zr0.5O2固溶体薄膜的P-E曲线[107]; (e), (f) Al2O3/Hf0.5Zr0.5O2 (20 nm)双层薄膜随Al2O3厚度变化的(e) C-V和(f) P-V曲线[109]

    Fig. 5.  (a) Thickness dependence of the 2Pr of HfO2 films prepared by ALD and PVD[95]. P-E curves of the (b) Hf0.5Zr0.5O2 films and (c) Hf0.5Zr0.5O2/Al2O3/Hf0.5Zr0.5O2 films with various thicknesses[101]. (d) P-E curves of HfO2(1 nm)/ ZrO2(1 nm) × 4 nanolaminates and the Hf0.5Zr0.5O2 solid solution[107]. (e) C-V and (f) P-V curves of Al2O3/Hf0.5Zr0.5O2 with different Al2O3 thicknesses[109].

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    图 6  (a) 1T1C铁电随机存储器结构示意图; (b) 1T1C存储器的SHMOO图[121]; (c)平面型铁电场效应管结构示意图和(d)相应器件在上、下铁电极化方向时的转移特性曲线[122]; (e)铁电鳍片式场效应管结构示意图; (f) HfO2铁电鳍片式场效应管的转移特性曲线[123]

    Fig. 6.  (a) Structure diagram and (b) SHMOO plot of a 1T1C ferroelectric random-access memory[121]; (c) schematic diagram of planar ferroelectric field effect transistor and (d) the transfer characteristic curve of FeFET device with upward and downward polarization[122]; (e) structure diagram of fin field-effect transistor; (f) the transfer characteristic curve of HfO2 ferroelectric fin field-effect transistor [123].

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    图 7  (a)铁电电容器从正电容到负电容的能量-电荷变化曲线[127]; (b) 负电容对NC-FET亚阈值斜率的影响[127]; (c) Al2O3/Hf0.5Zr0.5O2TiN/Si[128]负电容晶体管; (d) HfO2/TiN/Hf0.5Zr0.5O2TiN/SiO2/Si[129]负电容晶体管

    Fig. 7.  (a) Energy landscape of a ferroelectric capacitor [127]; (b) effect of negative capacitance on the subthreshold (SS) slope of the NC-FET[127]; (c) device architecture of Al2O3/Hf0.5Zr0.5O2TiN/Si NC-FET[128]; (d) device architecture of HfO2/TiN/Hf0.5Zr0.5O2TiN/SiO2/Si NC-FET[129].

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    图 8  铁电薄膜(Fe)在(a)“低势垒Φ–”和(b) “高势垒Φ+”状态下的FTJ结构[132]; Au/Hf0.5Zr0.5O2/La2/3Sr1/3MnO3/NSTO FTJ在(c)不同脉冲电压Vp下和(d)多次铁电极化翻转循环后的电阻值[133]; (e) TiN/Hf0.5Zr0.5O2/W结构FTJ在1—108次铁电极化翻转后的隧穿电流值[134]; (f) W/Hf0.8Zr0.2O2(1 nm)/SiO2(1 nm)/Si结构 FTJ在1—103次铁电极化翻转后的隧穿电流密度[135]

    Fig. 8.  (a), (b) FTJ structures with low or high barrier potential states (i.e. Φ– or Φ+)[132]. Resistance of Au/Hf0.5Zr0.5O2/La2/3Sr1/3MnO3/NSTO FTJ as a function of (c) pulse voltage Vp and (d) polarization switching cycles[133]. (e) Tunneling current value of TiN/Hf0.5Zr0.5O2/W FTJ after different polarization switching cycles[134]. (f) Tunneling current density of W/Hf0.8Zr0.2O2(1 nm)/SiO2(1 nm)/Si FTJ after polarization switching cycles[135].

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    图 9  (a)生物突触和动作电位示意图[137]; (b) FeFET模拟生物突触示意图; (c) LTP和LTD的突触权重-时间曲线[141]; (d) FeFET的光子突触结构示意图及其光电导-衰减时间曲线; (e) HZO薄膜铁电极化向下时器件的突触权重-时间曲线[137]

    Fig. 9.  (a) Schematic illustrations of biological synapses and action potential[137]. (b) Sketches on how a FeFET based synapse device; (c) synaptic weight as a function of time (Δt), showing a biological STDP behavior[141]. (d) Schematic device structure of the photonic synapse and optical responses; (e) the synaptic weight as a function of relaxing time[137].

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    图 10  (a)线性介电、(b)铁电和(c)反铁电材料的P-E曲线, 其中蓝色区域代表储能密度[144], P表示材料的极化, E表示施加的电场; (d), (e) HfxZr1–xO2 (x = 0.1—0.4)薄膜的(d) P-E电滞回线和(e)储能密度[22]

    Fig. 10.  P-E curves of (a) linear dielectric, (b) ferroelectric, and (c) antiferroelectric materials, where P represents the polarization of the material, E represents the applied electric field and the blue area represents the energy storage density of each material144]. (d) P-E hysteresis loops and (e) energy storage density of HfxZr1–xO2 (x = 0.1–0.4) thin films[22].

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    表 1  常见HfO2基铁电薄膜的制备条件和铁电性能汇总

    Table 1.  Summary of preparation conditions and ferroelectric properties of common HfO2-based ferroelectric films.

    掺杂元素掺杂浓度结构沉积方法薄膜厚度/nm沉积温度/℃退火电场/(MV·cm–1)2Pr/(μC·m–2)2Ec/(MV·cm–1)极化翻转次数/cycle
    Si[37]4.4 mol%TiN/Si:HfO2/TiNALD9N/A800 ℃, N24.5481.74N/A
    Zr[38]50 at%W/Zr:HfO2/WALD10250700 ℃, N2, 5 s3.5652.4104 at3.0 MV cm–1
    Y[28]5.2 mol%TiN/Y:HfO2/TiNALD10N/A600 ℃, N2, 20 s4.5482.4N/A
    Gd[39]3.4 cat%TaN/Gd:HfO2/TaNALD10300800 ℃, N2, 20 s—70N/A105 at4.0 MV cm–1
    Al[40]6.4 mol%W/TiN/Al:HfO2/SiALD10280700 ℃, N2, 10 s81009.5106 at8.0 MV cm–1
    La[41]10.0 cat%TiN/La:HfO2/TiNALD12280800 ℃, N2, 20 s4.5552.85×105at 4 MV cm–1
    Sr[42]9.9 mol%TiN/Sr:HfO2/TiNALD10300800 ℃, N2, 20 s3.546$ \sim $3.2106 at3.0 MV cm–1
    Ta[43]16 at%Pt/Ta:HfO2/Pt/TiPVD60500No anneal1.251061.6107 at0.8 MV cm–1
    非掺杂[44]N/ATiN/HfO2/TiNPEALD 8N/A600 ℃, Ar, 30 s3.125262.4> 108 at2.5 MV cm–1
    对照[45] Pb(Zr0.53Ti0.47)O3PLD500650650 ℃, O2, 15 minN/A1510.141×1010
    对照[46]BiFeO3CSD525N/A650 ℃, N2N/A1421.0106 at0.4 MV cm–1
    下载: 导出CSV

    表 2  几种HfO2基反铁电薄膜与其他常见材料的储能性能

    Table 2.  Energy storage performance of some HfO2 based antiferroelectric film and other common materials.

    材料类型厚度/nm电场/(MV·cm–1)ESD/(J·cm–3)η/%Ref.
    Hf0.5Zr0.5O2铁电9.24.95557[22]
    Ta2O5/Hf0.5Zr0.5O2介电/反铁电257100>95[148]
    Hf0.5Zr0.5O2/Hf0.25Zr0.75O2铁电/反铁电10671.9557.8[149]
    Hf0.3Zr0.7O2反铁电9.24.354551[22]
    Si:Hf0.5Zr0.5O2反铁电1045382[147]
    Al:Hf0.5Zr0.5O2反铁电1055280[147]
    La:Hf0.5Zr0.5O2反铁电1045070[53]
    Al2O3线性5—50—[150]
    BiFeO3铁电$ \sim $40—3.2—[146]
    BaTiO3铁电$ \sim $3002.628.575[145]
    Pb(Zr0.52Ti0.48)O3铁电3501.1315.658.8[151]
    La:PbZrO3反铁电103117.380.8[152]
    PVDF-HFP铁电1047.931.2—[153]
    下载: 导出CSV
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目录
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出版历程
  • 收稿日期:  2022-11-20
  • 修回日期:  2022-12-17
  • 上网日期:  2023-01-07
  • 刊出日期:  2023-05-05

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