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研究生: 巫坤福
論文名稱: RF磁控濺鍍系統成長BSTO/LNO人工超晶格磊晶薄膜之特性研究
Characterization of epitaxial Ba<0.48>Sr<0.52>TiO<3>/LaNiO<3> artificial superlattices prepared by RF magnetron sputtering
指導教授: 李志浩
口試委員:
學位類別: 碩士
Master
系所名稱: 原子科學院 - 工程與系統科學系
Department of Engineering and System Science
論文出版年: 2005
畢業學年度: 93
語文別: 中文
論文頁數: 100
中文關鍵詞: 人工超晶格薄膜射頻磁控濺鍍X光分析原子力顯微鏡
外文關鍵詞: Superlattice, RF magnetron sputtering, X-ray, AFM, SIMS, BST, STO, LNO
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  • 本實驗成功的利用Radio Frequency磁控濺鍍法製造出磊晶之Ba0.48Sr0.52TiO3/LaNiO3(BST/LNO)人工超晶格薄膜於單晶鈦酸鍶基板與鎳酸鑭底電極薄膜上。藉由X-ray反射率與X-ray繞射以及SIMS之量測觀察超晶格磊晶薄膜微結構之情形。由 X-ray繞射分析顯示在超晶格磊晶薄膜之中的BST層,由c軸的晶格常數會因為界面處的應變而拉長,並造成介電常數之顯著提升,且由a軸晶格常數變化情形,可得薄膜界面產生的應變大小於超晶格薄膜不同之堆疊厚度之關係,並相對於c軸之變化,得知應變提升則有效將c軸晶格拉長;在超晶格磊晶薄膜系統上,space charge、dipolar 與超晶格磊晶薄膜系統上之影響,可藉由不同頻率變化觀察出,由實驗知space charge對於超晶格磊晶薄膜上之界面層多寡有明顯之影響。此外,比對BTO/LNO人工超晶格磊晶薄膜之文獻其結果是一致,所在於界面之應變能夠有效果提升介電性質,且由於Sr元素之加入可以減少介電損失。藉由X光反射率以及X光繞射的量測可發現幾乎固定的界面粗糙度存在於BST與LNO層之間。因此人工超晶格磊晶薄膜具有相同程度將介電常數提升。


    Artificial superlattices having ferroelectric Ba0.48Sr0.52TiO3(BST) and conductive LaNiO3(LNO) as modulation length were grown epitaxially on Nb-doped SrTiO3 (001) substrates and LNO bottom-layer prepared by dual-gun Radio Frequency magnetron sputtering system. The formation of superlattice structure was confirmed from the x-ray reflectivity curves and SIMS depth profiles and (0 0 L) Bragg reflection of x-ray. A partial but nearly constant relaxation of in-plane strain in the superlattices was observed. From a macroscopic point of view, the strain in the superlattice structure contributes significantly to the dielectric enhancement. These BTO/LNO and BST/LNO artificial superlattices show a significant enhancement of dielectric constant relative to BTO and BST single layers of the same effective thickness. X-ray reflectivity measurement reveals that the superlattices have about the same interface roughness of BST/LNO. Consequently, nearly the same extent of dielectric enhancement results from the strained BST layer, along with a highly conductive interface zone in the superlattiecs.

    摘要………………………………………………………… I 誌謝………………………………………………………… Ⅲ 目錄………………………………………………………… Ⅳ 第一章 簡介……………………………………………… 1 1.1 前言…………………………………………………… 1 1.2 研究背景與目的……………………………………… 2 1.3 研究內容 …………………………………………… 4 第二章 文獻回顧 ……………………………………… 6 2.1鐵電材料之特性 ……………………………………… 9 2.1.1 鈦酸鋇系鐵電材料………………………………… 11 2.1.2 鈦酸鍶鋇薄膜材料………………………………… 12 2.1.3 鎳酸鑭薄膜材料…………………………………… 13 2.1.4 鈦酸鍶薄膜材料…………………………………… 14 2.2 超晶格薄膜結構與現今發展………………………… 15 2.3 濺鍍系統……………………………………………… 17 2.3.1射頻濺鍍 …………………………………………… 18 2.3.2 磁控濺鍍…………………………………………… 19 2.4 X-ray分析術 ………………………………………… 20 2.4.1 X-ray反射率分析 ………………………………… 21 2.4.2 X-ray繞射分析 …………………………………… 24 2.5 SIMS質譜分析儀……………………………………… 26 第三章 實驗步驟………………………………………… 44 3.1 製備過程……………………………………………… 44 3.1.1 樣品製備…………………………………………… 44 3.1.2 靶材製備…………………………………………… 44 3.1.3 濺鍍系統…………………………………………… 45 3.2 X-ray反射率測量 …………………………………… 46 3.3 X-ray繞射測量 ……………………………………… 46 3.4 AFM …………………………………………………… 47 3.5 SIMS…………………………………………………… 47 3.6 電性量測……………………………………………… 47 第四章 結果與討論 ……………………………………… 55 4.1 (BSTm/LNOm)n人工超晶格磊晶薄膜之結構分析 … 56 4.1.1 X-ray繞射分析 …………………………………… 56 4.1.2 X-ray反射率分析與AFM微結構分析……………… 61 4.1.3 SIMS縱深分析……………………………………… 63 4.2電性分析 ……………………………………………… 64 4.2.1 介電常數與介電損失對頻率之關係……………… 66 4.2.2 晶格常數與介電性質之關係……………………… 67 4.3人工超晶格磊晶薄膜在STO基板與LNO底電極層比較… 68 4.4人工超晶格磊晶薄膜BST/LNO與BTO/LNO之比較……… 69 4.5 STO/BST人工超晶格磊晶薄膜………………………… 70 第五章 結論………………………………………………… 90 Reference…………………………………………………… 90 附錄 …………………………………………………………100

    1.J.F.Scott, “Ferroelectric Memories”,p1(2000).
    2.S. Ezhilvalavan, T.-Y. Tseng, “Progress in the development of (Ba,Sr)TiO3(BST)thin films for Gigabit era DRAMs”, Mater. Chem. Phys., vol. 65, p227(2000).
    3.K. Itoh, “Trends in megabit in DRAM circuit design”, IEEE J. Solid State Circuits, vol. 25, p778(1990).
    4.G. Bronner, “DRAM technology trends for 256Mb and beyond”, in International Electron Devices and Materials Symposium, Hsinchu, p75(1996).
    5.吳啟明, “The Study of BST Thin Films Deposition on LNO Electrode by RF Magnetron Sputtering for DRAMs Applications”,清華大學, 博士論文, p1-3(1997).
    6.H. S. Nalwa, “Handbook of Thin Film Materials” , p1 (2002).
    7.吳朗, “電子陶瓷-介電”, 全欣資訊圖書 , p149(1994).
    8.Y. Xu, “Ferroelectric Materials and Their Applications”, North-Holland Netherlands , p1(1991).
    9.A. J. Moulson, J. M. Herbert, “Electroceramics-Materials Ropertiesn application”, CHAPMAN & HALL , p53(1990).
    10.賴昇志, “以LaNiO下電極,開發PZT鐵電記憶體低溫製成之研究”, 清華大學, 碩士論文, p8(2001).
    11.C. Feldman, “Formation of thin films of BaTiO3 by Evaporation”, View of Science Instrument, Vol. 26, p463(1954).
    12.A.E. Feuersanger, A.K. Hagenlocher and A.L. Solomln, “Preparation and Properties of Thin Barium Titanate Films”, J. Electrochem. Soc. , vol. 111, p1387(1964).
    13.H. Pratt and S. Firestone, “Fabrication of rf-sputtered Barium Titanate”, J. Vac. Sci. Tech., vol. 8, p256(1971).
    14.P. C. V. Buskirk, R.Gardiner, P. S. Kirlin, S. Nutt, “Reduced-Pressure MOCVD of Highly Crystalline BaTiO3 Thin Films”, J. Mater. Res., vol. 7, p542(1992).
    15.L. A. Wills, B. W. Wessels, D. S. Richeson, and T. J. Marks, “Epitaxial Growth of BaTiO3 Thin Films By Organometallic Chemical Vapor Deposition”, Appl. Phys. Lett.,vol. 60, p41(1992).
    16.A. Nazeri, m. Kahn, T. Kidd, “Strontium-Barium-Titanate Thin Films by Sol-Gel Processing”, J. Mater. Sci. Lett., vol. 14, p1085(1993).
    17.S. G. Yoon, J. C. Lee, and A. Safari, “Preparation of Thin-Film (Ba0.5,Sr0.5)TiO3 by the Laser Ablation Technique and Electrical Properties”, J. Appl. Phys., vol. 76, p2999(1994).
    18.M. Suzuki, T. Ami “A proposal of epitaxial oxide thin film structures for future oxide electronics”, Mater. Sci. Eng., vol. 41, p166(1996)
    19.H. Tabata, T. Kawai, S. Kawai, “Crystal structure and superconductivity of (La,Sr)2CuO4/Sm3CuO4 superlattices prepared by excimer laser deposition” , Appl. Phys. Lett., vol. 58, p1443(1991).
    20.H. Z. Jin and Jing Zhu, “ Size effect and fatigue mechanism in ferroelectric thin films” ,J. Appl. Phys., vol.92, p8(2002).
    21.T. Tsurumi, T. Harigai,D. Tanaka, S. Nam, H. Kakemoto, “Artificial ferroelectricity in perovskite superlattices”, Appl. Phys. Lett., vol.85, p5016(2004).
    22.Y. Lin, Jang-Sik Lee, H. Wang, Y. Li, S. R. Foltyn, and Q. X. Jia, G. E. Collis, A. K. Burrell, and T. M. McCleskey, “ Structural and dielectric properties of epitaxial Ba1− xSr xTiO3 films grownon LaAlO3 substrates by polymer-assisted deposition”, Appl. Phys. Lett.,vol.85, p21(2004)
    23.C. C. Yang, M. S. Chen, T. J. Hong, C. M. Wu, and T. B. Wu, “Preparation of (100)-oriented metallic LaNiO3 thin films on Si substrates by radio frequency magnetron sputtering for the growth of textured Pb(Zr0.53Ti0.47)O3” , Appl. Phys. Lett. vol.66, p2643(1995).
    24.劉恆睿,“利用磁控濺鍍法以鎳酸鑭在電極上沈積鋯鈦酸鋇薄膜作為微波變容器之研究”, 清華大學, 碩士論文, p41(2001).
    25.梁元彰, "Characterization of epitaxial BaTiO3/LaNiO3 artificial superlattices",清華大學, 博士論文, p45(2004).
    26.H. Tabata, H. Tanaka, T. Kawai, and M. Okuyama, “Strained SrTiO3/BaTiO3 Superlattices Formed by Laser Ablation Technique and Their High Dielectric Properties”, Jpn. J. Appl. Phys., vol.34, p544(1995).
    27.H. Tabata, H. Tanaka, and T. Kawai, “Formation of artificial BaTiO3/SrTiO3 superlattices using pulsed laser deposition and their dielectric properties”, Appl. Phys. Lett., vol65,1970(1994).
    28.H. Tabata, and T. Kawai,“Dielectric properties of strained (Sr,Ca)TiO3/(Ba,Sr)TiO3 artificial lattices”, Appl. Phys. Lett. vol.70, p321(1997).
    29.J. Kim, Y. Kim, Y. S. Kim, J. Lee, L. Kim, and D. Jung, “Large nonlinear dielectric properties of artificial BaTiO3/SrTiO3 superlattices”, Appl. Phys. Lett., vol.80, p3581(2002).
    30.L. Kim, D. Jung, J. Kim, Y. S. Kim, and J. Lee, “Strain manipulation in BaTiO3/SrTiO3 artificial lattice toward high dielectric constant and its nonlinearity”,Appl. Phys. Lett., vol.82, p2118(2003).
    31.G. Koebernik, W. Haessler, R. Pantou, and F. Weiss, “Thickness dependence on the dielectric properties of BaTiO3/SrTiO3-multilayers”, Thin Solid Films , vol.80, p449, (2004).
    32.A. Nakagawara, T. Shimuta, T. Makino, S. Arai, H. Tabata, and T. Kawai, “Epitaxial growth and dielectric properties of (111) oriented BaTiO3/SrTiO3 superlattices by pulsed-laser deposition”, Appl. Phys. Lett., vol.77, p3257 (2000).
    33.T. Tsurumi, T. Harigai,D. Tanaka, H. Kakemoto, S. Wada, “Anomalous dielectric and optical properties in perovskite-type artificial superlattices”, Sci. Tech. Adv. Mater., vol.5, p425(2004).
    34.行政院國家科學委員會, “真空技術與應用”精密儀器發展中心”, p349(2003).
    35.董俊秀, “鈦酸鍶鋇薄膜之濺鍍研究”, 清華大學,碩士論文, p21 (1995).
    36.施修正, “利用濺鍍法以鎳酸鑭為電極製作動態記憶體之鋯鈦酸鋇薄膜之研究”, 清華大學, 博士論文, p34(1999).
    37.吳泰伯, 許樹恩, “X光繞射與材料結構分析”, 中國材料科學學會, p121(1996).
    38.汪建民, “材料分析”, 中國材料科學學會, p177(1998).
    39.科儀新知, “X光繞射技術專題”, 第二十二卷第二期, p31(2000).
    40.A. van der Lee, “Gracing incident specular reflectivity: theory, experiment, and applications”, Solid State Science, vol.2, p257 (2000).
    41.T.Tsurumi, T.Ichikawa, T.Harigai, H.Kakemoto, and S.Wada, “Dielectric and optical properties of BaTiO3/SrTiO3 and BaTiO3/BaZrO3 superlattices”, J. Appl. Phys., vol.91, p2284 (2002).
    42.F. Q. Tong, W. X. Yu, F. Liu, Y. Zuo, and X. Ge, “Microstructural study of BaTiO3/SrTiO3 superlattice” Mater. Sci. Eng. B, vol.98, p6 (2003).
    43.N. Wang, H. B. Lu,W. Z. Chen, T. Zhao, F. Chen, H. Y. Peng, S. T. Lee, and G. Z. Yang, “Morphology and microstructure of BaTiO3/SrTiO3 superlattices grown on SrTiO3 by laser molecular-beam epitaxy”, Appl. Phys. Lett., vol.75, p3464(1999).
    44.T. Tasrumi, T. Suzuki, M. Yamane, and M. Daimon, “J Fabrication of Barium Titanate/Strontium Titanate Artificial Superlattice by Atomic Layer Epitaxy”, Jpn. J. Appl. Phys., vol.33, p5192(1994).
    45.Y. Yoneda, K. Sakaue, and H. Terauchi, “Dielectric Investigation of [(SrTiO3)6(BaTiO3)6]2 Multilayer Capacitor”, Jpn. J. Appl. Phys., vol.40, p6888(2001).
    46.K. Shimoyama, M. Kiyohara, K. Kubo, A. Uedono, and Y. Yamabe, “Epitaxial growth of BaTiO3/SrTiO3 structures on SrTiO3 substrate with automatic feeding of oxygen from the substrate”, J. Appl. Phys., vol.92, p4625(2002).
    47.T. Harigai, D. Tanaka, H. Kakemoto, S.Wada, and T. Tsurumi, “Dielectric properties of BaTiO3/SrTiO3 superlattices measured with interdigital electrodes and electromagnetic field analysis”, J. Appl. Phys., vol.94, p7923(2003).
    48.Z. Wang, and S. Oda, “Electrical Properties of SrTiO[sub 3]/BaTiO[sub 3] Strained Superlattice Films Prepared by Atomic Layer Metallorganic Chemical Vapor Deposition”J. Electrochem. Soc. , vol.147, p4615(2000).
    49.T. Shimuta, O. Nakagawara, T. Makino, S. Arai, H. Tabata, and T. Kawai, “Enhancement of remanent polarization in epitaxial BaTiO3/SrTiO3 superlattices with "asymmetric" structure”, J. Appl. Phys., vol.91, p2290(2002).
    50.T. M. Shaw, A. Gupta, M. Y. Chen, P. E. Batson, R. B. Laibowitz, and B. A. Scott, “Atomic scale oxide superlattices grown by RHEED controlled pulsed laser deposition”, J. Mater. Res., vol.9, p2566(1994).
    51.A. Visinoiu, M. Alexe, H. N. Lee, D. N. Zakharov, A. Pignolet, D. Hesse, and U. Gosele, “Initial growth stages of epitaxial BaTiO3 films on vicinal SrTiO3 (001) substrate surfaces”, J. Appl. Phys., vol.91, p10157(2002).
    52.K. Iijima, T. Terashima, Y. Bando, K. Kamigaki, and H. Terauchi, “Atomic layer growth of oxide thin films with perovskite-type structure by reactive evaporation”, J. Appl. Phys., vol.72, p2840(1992).
    53.H. M. Christen, E. D. Specht, D. P. Norton, M. F. Chisholm, and L. A. Boatner, “Long-range ferroelectric interactions in KTaO3/KNbO3 superlattice structures”, Appl. Phys. Lett., vol.72, p2535(1998).

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