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铈镁交替掺杂Ba0.6Sr0.4TiO3薄膜高调谐性能

胡一明 廖家轩 杨函于 王思哲 吴孟强 徐自强 冯婷婷 巩峰

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铈镁交替掺杂Ba0.6Sr0.4TiO3薄膜高调谐性能

胡一明, 廖家轩, 杨函于, 王思哲, 吴孟强, 徐自强, 冯婷婷, 巩峰

High tunable dielectric properties of Ce and Mg alternately doped Ba0.6Sr0.4TiO3 films

Hu Yi-Ming, Liao Jia-Xuan, Yang Han-Yu, Wang Si-Zhe, Wu Meng-Qiang, Xu Zi-Qiang, Feng Ting-Ting, Gong Feng
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  • 根据Ce掺杂、Mg掺杂以及Y和Mn交替掺杂可分别使Ba0.6Sr0.4TiO3 (BST)薄膜的介电调谐率、介电损耗和综合介电性能提高、降低和提高的特点, 采用改进的溶胶- 凝胶(sol-gel)法制备了6层Ce和Mg交替掺杂BST薄膜, 并研究其结构及介电性能. X射线衍射表明, 该薄膜为立方钙钛矿结构、主要沿(110)晶面生长、晶化明显增强. 扫描电子显微镜表明, 薄膜表面形貌极大改善, 首层薄膜与基体良好匹配, Ce掺杂层为首层的交替掺杂薄膜表面更均匀致密、晶粒更细小、晶化略微减弱. X射线光电子能谱表明, 薄膜表面非钙钛矿结构显著减少. 薄膜显示高调谐率和高优质因子. Mg掺杂层为首层的交替掺杂薄膜在高频范围的综合介电性能更稳定. Ce 掺杂层为首层的交替掺杂薄膜在低频范围的介电强度更高, 综合性能更突出, 在100 kHz 下, 10, 20和40 V偏压对应的调谐率分别为47.4%, 63.6% 和71.8%, 对应的优质因子分别为27.1, 77.5和86.5, 可满足微波调谐应用. 同时, 就有关机理进行了分析.
    For barium strontium titanate (Ba0.6Ti0.4TiO3, BST) films used in tunable microwave devices, they must have excellent structural characteristics and outstanding combination of dielectric properties i.e., a low loss tangent over the range of operating direct current (DC) bias voltages, a moderate dielectric constant for impedance matching purpose, a large variation in the dielectric constant with applied dc bias (high tunability, in particular high tunability at low applied dc bias), etc. To achieve such a high objective, the following two great improvements are carried out. A normal sol-gel method is modified to prepare multilayer BST films layer by layer. Each multilayer BST film is composed of six layers, where each layer is preheated at 600 ℃, thus the layers from the first layer to the sixth layer are successively preheated once to six times. Thus each BST film is smooth and dense, and contains almost no organic residues. On the other hand, as a new doped mode, Ce/Mn alternate doping is performed. For every six layer-BST films, when the odd number layers are doped with Ce, then the even number layers are doped with Mg, vice versa. The above two improvements result from the fact that Ce doping, Mg doping and Y and Mn alternate doping could make BST thin films significantly improve the dielectric tunability, reduce the dielectric loss, and improve the combination of dielectric properties, respectively. According to the above two improvements, 1 mol% Ce and 3 mol% Mg alternately doped BST thin films are prepared on Pt/Ti/SiO2/Si wafers (substrates). The prepared BST films are denoted by the doped element as follows: Ce/Mg/Ce/Mg/Ce/Mg with Ce doped BST layer is referred to as the first layer (for short Ce/Mg) and Mg/Ce/Mg/Ce/Mg/Ce with Mg doped BST layer as the first layer (Mg/Ce), and the structure and dielectric properties of the films are studied. X-ray diffraction results show that two films present cubic perovskite structures, mainly grow along (110) crystal face, and show strong crystallization. SEM results indicate that the surface morphologies of two films are greatly improved, and Ce or Mg doped BST layer as the first layer can be well matched with the substrate. The surface of the Ce/Mg film is more uniform and denser with slightly smaller grains and weaker crystallization. XPS results demonstrate that the non-perovskite structures on the surfaces of two films are significantly reduced. Each of the two films has high tunability at low applied dc bias and high figure of merit (FOM). The Mg/Ce film shows more stable combination of dielectric properties in a high frequency range. The Ce/Mg film shows more excellent combination of dielectric properties and higher dielectric strength in a low frequency range, where when the testing frequency is 100 kHz, 10 V, 20 V and 40 V applied dc bias voltages correspond to tunabilities of 47.4%, 63.6% and 71.8%, and FOMs of 71.8%, and 27.1, 77.5 and 86.5, respectively. Such good dielectric properties can fully satisfy the requirements for tunable microwave device applications. The relevant mechanisms are also analyzed.
      通信作者: 廖家轩, jxliao@uestc.edu.cn
    • 基金项目: 国家自然科学基金(批准号:51172034,61101030)和四川省科技计划(批准号:2015GZ0047,2015GZ0130)资助的课题.
      Corresponding author: Liao Jia-Xuan, jxliao@uestc.edu.cn
    • Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 51172034, 61101030) and the Science and Technology Project of Sichuan Province, China (Grant Nos. 2015GZ0047, 2015GZ0130).
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    Yu J, Liao J X, Jin L, Wei X B, Wang P, Wei X B, Xu Z Q 2011 Acta Phys. Sin. 60 077701 (in Chinese) [俞健, 廖家轩, 金龙, 魏雄邦, 汪澎, 尉旭波, 徐自强 2011 物理学报 60 077701]

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    Peng L S, Xi X X, Moeckly B H, Alpay S P 2003 Appl. Phys. Lett. 83 4592

    [22]

    Craciun V, Singh R K 2000 Appl. Phys. Lett. 76 1932

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    Liao J X, Wei X B, Xu Z Q, Wang P 2014 Vacuum 107 291

    [24]

    Kim K T, Kim C I 2003 Microelectron. Eng. 66 835

    [25]

    Kim K T, Kim C I 2005 Thin Solid Films 472 26

    [26]

    Wang S Y, Cheng B L, Wang C, Redfern S A T, Dai S Y, Jin K J, Lu H B, Zhou Y L, Chen Z H, Yang G Z 2005 J. Phys. D: Appl. Phys. 38 2253

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    Cole M W, Hubbard C, Ngo E, Ervin M, Wood M 2002 J. Appl. Phys. 92 475

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    Wu Q C, Wang H P, Tian Q, Liao H C 2007 Proceedings of the 6th Conference on Functional Materials and Applications in China Wuhan, China, November 15-19, 2007 p693 (in Chinese) [吴其昌, 王慧萍, 田琼, 廖恒成 2007 第六届中国功能材料及其应用学术会议论文集 武汉, 中国, 11月15日-11月19日, 2007 p693]

  • [1]

    Padminni P, Taylor T R, Lefevre M J, Nagra A S, York R A, Speck J S 1999 Appl. Phys. Lett. 75 3186

    [2]

    Pervez N K, Hansen P J, York R A 2004 Appl. Phys. Lett. 85 4451

    [3]

    Zou C, Xu Z M, Ma Z C, Wu X H, Peng J 2015 Acta Phys. Sin. 64 118101 (in Chinese) [邹超, 徐智谋, 马智超, 武兴会, 彭静 2015 物理学报 64 118101]

    [4]

    Cole M W, Nothwang W D, Hubbard C, Ngo E, Ervin M 2003 J. Appl. Phys. 93 9218

    [5]

    Cole M W, Joshi P C, Ervin M H 2001 J. Appl. Phys. 89 6336

    [6]

    Wang S Y, Cheng B L, Wang C, Dai S Y, Jin K J, Zhou Y L, Lu H B, Chen Z H, Yang G Z 2006 J. Appl. Phys. 99 013504

    [7]

    Liao J X, Pan X F, Wang H Q, Zhang J, Fu X J, Tian Z 2009 Rare Metal Mat. Eng. 38 1987

    [8]

    Chang W, Sengupta L 2002 J. Appl. Phys. 92 3941

    [9]

    Cole M W, Joshi P C, Ervin M H, Wooda M C, Pfeffer R L 2000 Thin Solid Films 374 34

    [10]

    Liao J X, Xu Z Q, Wei X B, Wei X B, Wang P, Yang B C 2012 Surf. Coat. Tech. 206 4518

    [11]

    Wang B, Liao J X, Zhang B, Xu C Y 2013 Rare Metal Mat. Eng. 42 96 (in Chinese) [王滨, 廖家轩, 张宝, 徐从玉 2013 稀有金属材料与工程 42 96]

    [12]

    Zhou Q G, Zhai J W, Yao X 2007 J. Inorg. Mater. 22 519 (in Chinese) [周歧刚, 翟继卫, 姚熹 2007 无机材料学报 22 519]

    [13]

    Liao J X, Wei X B, Xu Z Q, Wei X B, Wang P 2012 Mater. Chem. Phys. 135 1030

    [14]

    Huang J Q, Liao J X, Wang P, Zhang W F, Wei X B, Xu Z Q 2014 Surf. Coat. Tech. 251 307

    [15]

    Huang J Q, Liao J X, Zhang W F, Wang S Z, Yang H Y, Wu M Q 2015 Integr. Ferroelectr. 162 94

    [16]

    Liao J X, Zhang W F, Huang J Q, Wang P, Yang H Y, Wang S Z, Wu M Q 2015 Integr. Ferroelectr. 164 74

    [17]

    Bao J B, Ren T L, Liu J S, Liu L T, Li Z J, Li X J 2002 PiezoElectr. Acoustoopt 24 389

    [18]

    Ahn K H, Baik S, Kim S S 2002 J. Appl. Phys. 92 2651

    [19]

    Chang W, Horwitz J S, Carter A C, Pond J M, Kirchoefer S W, Gilmore C M, Chrisey D B 1999 Appl. Phys. Lett. 74 1033

    [20]

    Yu J, Liao J X, Jin L, Wei X B, Wang P, Wei X B, Xu Z Q 2011 Acta Phys. Sin. 60 077701 (in Chinese) [俞健, 廖家轩, 金龙, 魏雄邦, 汪澎, 尉旭波, 徐自强 2011 物理学报 60 077701]

    [21]

    Peng L S, Xi X X, Moeckly B H, Alpay S P 2003 Appl. Phys. Lett. 83 4592

    [22]

    Craciun V, Singh R K 2000 Appl. Phys. Lett. 76 1932

    [23]

    Liao J X, Wei X B, Xu Z Q, Wang P 2014 Vacuum 107 291

    [24]

    Kim K T, Kim C I 2003 Microelectron. Eng. 66 835

    [25]

    Kim K T, Kim C I 2005 Thin Solid Films 472 26

    [26]

    Wang S Y, Cheng B L, Wang C, Redfern S A T, Dai S Y, Jin K J, Lu H B, Zhou Y L, Chen Z H, Yang G Z 2005 J. Phys. D: Appl. Phys. 38 2253

    [27]

    Cole M W, Hubbard C, Ngo E, Ervin M, Wood M 2002 J. Appl. Phys. 92 475

    [28]

    Wu Q C, Wang H P, Tian Q, Liao H C 2007 Proceedings of the 6th Conference on Functional Materials and Applications in China Wuhan, China, November 15-19, 2007 p693 (in Chinese) [吴其昌, 王慧萍, 田琼, 廖恒成 2007 第六届中国功能材料及其应用学术会议论文集 武汉, 中国, 11月15日-11月19日, 2007 p693]

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出版历程
  • 收稿日期:  2016-03-28
  • 修回日期:  2016-05-05
  • 刊出日期:  2016-07-05

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