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研究生: 吳允中
Yun Chung Wu.
論文名稱: 二氧化銥在下電極生成對鈦酸鍶鋇介電特性的影響
The study of IrO2 formed in bottom electrode and the dielectric properties of BaxSr1-xTiyO3+z
指導教授: 賴志煌
C. H. Lai
口試委員:
學位類別: 碩士
Master
系所名稱: 工學院 - 材料科學工程學系
Materials Science and Engineering
論文出版年: 2001
畢業學年度: 89
語文別: 中文
論文頁數: 79
中文關鍵詞: 退火IrIrO2雙層結構
外文關鍵詞: annealing, Ir, IrO2, double BST layer
相關次數: 點閱:3下載:0
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  • 隨著DRAM(dynamic random access memories)記憶密度的增加,單位記憶胞的大小也越來越小。而電子陶瓷薄膜因具有高介電常數,可以降低記憶胞之面積,故受到相當的矚目。其中之(Ba,Sr)TiO3(BST)由於具有高介電常數、低漏電流、高崩潰電場、室溫下是順電相、以及容易控制成分等優點,極具潛力成為下世代DRAN之記憶材料。
    在之前文獻報告中提到當以Ir為下電時極,BST具有較高之介電常數,其原因和退火後IrO2在BST及Ir界面生成有關。本論文研究即在高的Ar/O2混和氣壓下,在Ir下電極上鍍製BST,希望能在不需退火的情形下,在界面處自然會生成IrO2來提高介電常數。實驗結果發現當製成溫度為550℃時,初鍍膜之介電常數可達926,但相對的漏電流卻略顯過大。為了改善此現象,我們在純Ar氣氛下於Ir上先長一層薄的BST,來抑制IrO2過量成長所造成的表面粗糙度化,之後再以混和氣氛鍍製BST。此種雙層結構可減少IrO2形成量,降低表面粗糙度,達到高介電常數及低漏電流之高密度記憶材料之需要。


    The advancement of dynamic random access memories (DRAM's) has significantly decreased the available area per cell. Electroceramic thin films with high dielectric constant have attracted great attention for practical use in capacitors of gigabit DRAM's since the adoption of high-dielectric-constant materials can lower the height of the storage node and simplify the cell structure. One of the most promising materials for the capacitor dielectric films is (Ba,Sr)TiO3 (BST) because of its high dielectric constant, low leakage current density, high dielectric breakdown strength, paraelectric perovskite phase that does not exhibit fatigue, and the ease of composition control due to the absence of volatile lead oxide.
    The literature indicate the bottom electrode effects greatly the electric properties of BST. After annealing at 600~700℃ the BST with the bottom electrode of Ir possesses higher dielectric constant due to the IrO2 formation at the BST/Ir interface. To enhance the dielectric constant of BST without annealing process, the BST film were sputtered on the electrode of Ir under high working pressure of mixing Ar/O2 gas in this research. In the condition, the thin film of IrO2 was formed simultaneously at the interface between the BST and Ir films during the BST-deposited process. The best dielectric constant can achieve 926 at 550℃, but the leakage current is very poor. Finally, we apply the double BST layers, which was sputtering with pure Ar and mixing Ar/O2 gas, can not only have large dielectric constant but also have low leakage current.

    表目錄………………………………………………………………………………… 圖目錄………………………………………………………………………………… 第一章 緒論………………………………………………………………………….1 §1-1 簡介…………………………………………………………………………1 §1-2 研究動機…………………………………………………………………..3 第二章 文獻回顧…………………………………………………………………….5 §2-1 鐵電材料……………………………………………………………………5 §2-1-1 鐵電材料之結構與特性………………………………………………5 §2-1-2 鈣鈦礦結構…………………………………………………………..9 §2-2 鐵電薄膜之製作………………………………………………………….10 §2-3鐵電材料之特性………………………………………………………….13 §2-4 鈦酸鍶鋇系鐵電材料…………………………………………………….25 §2-5下電極之選取…………………………………………………………….29 第三章 實驗步驟…………………………………………………………………..45 §3-1 實驗參數的選取………………………………………………………….45 §3-2 實驗步驟………………………………………………………………….48 第四章 結果與討論………………………………………………………………..57 §4-1 室溫下鍍膜,再後退火………………………………………………….57 §4-2 高溫下鍍膜……………………………………………………………….58 參考資料…………………………………………………………………………

    1.J. F. Scott, C. A. P. de Araujo, L. D. McMillan, H. Yoshimori, H. Watanabe, T. Mihara, M. Azurna, T. Ueda, Tetsuk Ueda, D. Ueda, and G. Kano, "Ferroelectric Thin Films in Integrated Microelectronic Devices", Ferroelectrics, 133, (1992) 47.
    2. G. H. Haerting, "Ferroelectric Thin Film for Electronic Applications", J. Vac. Sci. Technol., A9(3), (1991) 414.
    3. L. M. Sheppard, "Advances in Processing of Ferroelectric Thin Films", Cerarnci Bulletin, 71(1), (1992) 85.
    4. M. Sayer and K. Sreenivas, "Ceramic Thin Films: Fabrication and Applications", Science, 247, (1990) 1056.
    5. G. Yi and M. Sayer, "Sol-Gel Processing of Complex Oxide Films", Cerarnci Bulletin, 70(7), (1991)1173.
    6.林諭男,"強介電陶瓷薄膜的應用",工業材料,107, (1995) 49.
    7.Auciello and R. Ramesh, "Electroceramic Thin Films Part 1: Processing", MRS Bulletin, 20(6), (1996) 21.
    8. H, Yamaguchi, S. Matsubara, and Y. Miyasaka, "Reactive Coevaporation Synthesis and Characterization of SrTiC)3 Thm Films", Jpn. J. Appl. Phys., 30(9B), (1991) 2197.
    9. K. lijima, T. Terashima, K. Yamamoto, K. Hirata, and Y. Bando,
    "Preparation of ferroelectric BaTiC)3 thin films by activated reactive evaporation", Appl. Phys. Lett., 56(6), (1990) 527.
    10.H. Terauchi, Y. Watanabe, H. Kasatani, K. Kamigaki, Y. Yano, T. Terashima, "Structural Study of Epitaxial BaTiC)3 Crystals", J. Phys. Soc. Jpn., 67(7), (1992) 2194.
    11. A. Mansingh and C. V. R. V. Kumar, "Effect of the target on the structure and optical properties of radio-frequency sputtered barium titanate films", J. Mater. Sci. Lett., 7, (1988) 1104.
    12. S. H. Nam, N. H. Cho, and H. G. Kim, "Characterization of SrTiC)3 Thin Films Prepared by RF Magnetron Sputtering", J. Phys. D: Appl. Phys., 25, (1992) 727. 13.Q. X. Jia, Z. Q. Shi and W. A. Anderson, "BaTiO@ Thin Film Capacitors Deposited by r.f. Magnetron Sputtering", Thin Solid Films, 209, (1992) 230.
    14. J. Gerblinger and H. Meixner, "Electrical Conductivity of Sputtered Films of Strontium Titanate", J. Appl. Phys., 67(12), (1990) 7453.
    15. A. Nazeri, M. Kahn, T. Kidd, "Strontium-Barium-Titanate Thin Films by Sol-Gel Processing", J. Mater. Sci. Lett., 14, (1993) 1085.
    16.M. N. Kamalasanan, S. Chandra, P. C. Joshi, and A. Mansingh, "Structure and Optical Properties of Sol-Gel-Processed BaTiO3 Ferroelectric Thin Films", Appl. Phys. Lett., 59(27), (1991) 3547.
    17.M. Klee and P. K. Larsen, "Ferroelectric Thin Films for Memory Applications: Sol-Gel Processing and Decomposition of Organo-Metallic Compounds", Ferroelectrics, 133, (1992) 91.
    18. P. C. Joshi and S. B. Krupanidhi, "Structural and Electrical Characteristics of SrTiC)3 Thin Films for Dynamic Random Access Memory Applications", J. Appl. Phys., 73(11), (1993) 7627.
    19. W. Ousi-Benomar, S. S. Xue, R. A. Lessard, A. Singh, Z. L. Wu,and P. K. Kuo, "Structural and Optical Characterization of BaTiO3 Thin Films Prepared by Metal-Organic Deposition from Barium 2-ethylhexanoate and Titanium Dimethoxy Dineodecanoate", J. Mater. Res., 9(4), (1994)970.
    20. P. C. V. Buskirk, R. Gardiner, P. S. Kirlin, S. Nutt, "Reduced- Pressure MOCVD of Highly Crystalline BaT@ Thin Films", J. Mater. Res., 7(3), 1992 (542).
    21.L. A. Wills, B. W. Wessels, D. S. Richeson, and T. J. Marks, "Epitaxial Growth of BaT@ Thin Films by Organometallic Chemical Vapor Deposition", Appl. Phys. Lett., 60(1), (1992) 41.
    22. C. S. Chem, J. Zhao, L. Luo, P. Lu, Y. Q. Li, P. Norris, B. Kear, F. Cosandey, C. J. Maggiore, B. Gallois, B. J. Wilkens, "Epitaxial Growth of BaTi03 Thin Films by Plasma-Enhanced Metalorganic Chemical Vapor Deposition", Appl. Phys. Lett., 60(9), (1992)1144.
    23. T. Kawahara, M. Yamarnuka, T. Makita, K. Tsutahara, A. Yuuki, K. Ono, and Y. Matsui, "Preparation of (Ba,Sr)Ti03 Thin Films by Chemical Vapor Deposition Using Liquid Sources", Jpn. J. Appl. Phys., 33(10), (1994) 5897.
    24. M. E. Pilleux and V. M. Fuenzalida, "Hydrothermal BaTiO3 Films on Silicon: Morphological and Chemical Characterization", J. Appl. Phys., 74(7), (1993) 4664.
    25. R. R. Bacsa, J. P. Dougherty, and L. J. Pilione, "Low-Temperature Synthesis of BaTiC@ Thin films on Silicon Substrates byHydrothermal Reaction", Appl. Phys. Lett., 63(8), (1993) 1053.
    26. K. Kajiyoshi, M. Yoshimura, Y. Hamaji, K. Tornono, and T. Kasanami, "Growth of (Ba,Sr)TiC)3 @" Films by the Hydrothermal-Electrochemical Method and Effect of Oxygen Evolution on Their Microstructrue", J. Mater. Res., 11(1), (1996) 169.
    27. C. J. Peng, H. Hu, and S. B. Krupanidhi, "Low-Energy Oxygen Ion Bombardment Effect on BaTi03 Thin Films Grown by Multi-Ion-Beam Reactive Sputtering Technique", Appl. Phys. Lett., 63(6),(1993) 734.
    28. S. Yamamichi, T. Sakuma, K. Takemura, and Y. Miyasaka, "SrTiO3 Thin Film Preparation by Ion Beam Sputtering and Its Dielectric Properties", Jpn. J. Appl. Phys., 30(9B), (1991) 2193.
    29. H. kawano, K. Morii, and Y. Nakayama, "Effects of Crystallization on Structural and Dielectric Properties of Thin Amorphous Films of (l-x)BaTi03-xSrTi03 (x=0-0.5, 1.0), J. Appl. Phys., 73(10), (1993) 5141.
    30. H. Kobayashi and T. Kobayashi, "Heteroepitaxial Growth of Quaternary Ba,(Sri.@Ti03 Thin Films by ArF Excimer Laser Ablation", Jpn. J. Appl. Phys. 2, 33(4A), (1994) L533.
    31.S. G. Yoon, J. C. Lee, and A. Safari, "Preparation of Thin-Film (Ba,Sr)Ti03 by the Laser Ablation Technique and Electrical Properties", Appl. Phys., 76(5), (1994) 2999.
    32. M. Hiratani, Y. Tarutani, T. Fukazawa, M. Okamoto, and K. Takagi, "Growth of SrTiC)3 Thin Films by Pulsed-Laser Deposition", Thin Solid Films, 227, (1993) 100.
    33. B. C. Cole, "Finally, It's Ferroelectric!", Electronics, Aug., (1989) 88.
    34. S. Weber, "A New Memory Technology is about to Hit the Market", Electronics, Feb., (1988) 91.
    35. J. T. Evans and R. Womack, "An Experimental 512-bit Nonvalatile Memory with Ferroelectric Storage Cell", IEEE J. Solid-State Circuits, 23, (1988) 1171.
    36. J. F. Scott and C. A. P. de Araujo, "Ferroelectric Memories", Science, 246, (1989) 1400.
    37. W. A. Geidman, "Progess in Ferroelectric Memory Technology",IEEE Trans. Ultrasonics, Ferroelectrics, and Frequency Control., 38(6), (1991) 704.
    38. P. K. Larsen, R. Cuppens, and G. A. C. M. Spierings, "Ferroelectric Memories", Ferroelectrics, 128, (1992) 265.
    39.0. Auciello and R. Ramesh, "Electroceramic Thin Films Part II: Device Applications", MRS Bulletin, 20(7), (1996) 29.
    41.H. N. AI-Shareef, 0. Auciello, A. 1. Kingon, "Electrical Properties of Ferroelectric Thin-Film Capacitors with Hybrid (Pr,RuO2) Electrodes for Nonvolatile Memory Applications", J. Appl. Phys.,77(5), (1995) 2146.
    42. C. B. Eom, R. B. V. Dover, J. M. Phillips, D. J. Werder, J. H. Marshall, C. H. Chen, R. J. Cava, and R. M. Fleming, "Fabrication and properties of epitaxial ferroelectric heterostructures with (SrRu03) isotropic metallic oxide electrodes", Appl. Phys. Lett.,63(18), (1993) 2570.
    42. M. S. Chen, T. B. Wu, and J. M. Wu, "Effects of Textured LaNiO3 Electrode on the Fatigue Improvement of Pb(ZrTi)O3 .Thin Films", Appl. Phys. Lett., 68(10), (1996) 1430.
    43.彭成鑑,"強介電陶瓷材料在動態隨機記憶體(DRAM)",工業材料,107,(1995)72.
    44. C. C. Yang, M. S. Chen, T. J. Hong, C. M. Wu, J. M. Wu, and T. B. Wu, "Preparation of(100)-0riented Metallic LaNiO3 Thin Films on Si Substrates by RF Magnetron Sputtering for the Growth of Textured P2T", Appl. Phys. Lett., 66(20), (1995) 2643.
    45.M. J. Shyu, T. J. Hong, T. J. Yang, and T. B. Wu, "Highly (100)- Oriented Thin Films of Sol-Gel Derived Pb[(Mg,Nb) Ti)03 Prepared on Textured LaNiC)3 Electrode", Jpn. J. Appl. Phys., 34(7A), (1995) 3647.
    46. M. J. Shyu, T. J. Hong, and T. B. Wu, "Properties of Highly (100)- Oriented Thin Films of Sol-Gel Derived Pb(Mg-Nb)TiO3 on (100)-Textured LaNiO3 Electrode", Mater. Lett., 23, (1995) 221.
    47.M. S. Chen, J. M. Wu, and T. B. Wu, "Effects of(100)-Textured LaNi03 Electrode on the Crystallization and Properties of Sol-gel Derived PbZrTiO3 Thin Films", Jpn. J. Appl. Phys., 34(9A),(1995)4870.
    48. T. F. Tseng, K. S. Liu, T. B. Wu, and 1. N. Lin, 1996, "Effect of LaNi03/Pt Double Layers on The Characteristics of (Pb,La)ZrTiO3 Thin Films", Appl. Phys. Lett., 68(18), (1996) 2505.
    49. H. Y. Lee, T. B. Wu, and J. F. Lee, "X-ray Absorption Spectroscopic Studies of Sputtered-Deposited LaNi03 Thin Films on Si Substrate", J. Appl. Phys., 80(4), (1996) 2175.
    50. T. F. Tseng, C. C. Yang, K. S. Liu, J. M. Wu, T. B. Wu, and 1. N. Lin, "Crystallization of LaNi03 Layers and "Their Effect on the Pulsed Laser Deposited (Pb,La). ZrTiO3 Thin Films", accepted for publication by Jpn. J. Appl. Phys., (1996).
    51.C. M. Wu, T. J. Hong, and T. B. Wu, "Effects of(100)-Textured LaNi03 Electrode on The Deposition and Characteristics of Pb/Ti Thin Films Prepared by RF Magnetron Sputtering", revised for publication by J. Mater. Res., (1996).
    52.楊清泉,電極製備高(100)優選方向性(Pb,La)TiO,
    53.洪天爵,"鈦酸鉛薄膜之研究-製程、微觀結構、優選晶向與鐵電特性。,清華大學,博士論文,(1995).
    54.徐鳴志,"應用在鐵電記憶體之(PbLa)(MgNbTiO3溶凝膠薄膜的研製。,清華大學,博士論文,(1995).
    55.陳銘森,"鎳酸鑭電極對鋯鈦酸鉛溶凝膠簿膜製作與特性影響之研究",清華大學,博士論文,(1996).
    56.劉裕文,"鎳酸鑭薄膜與矽晶介面結構及電性研究",清華大學,碩士論文,(1996).
    57.葉明華,"脈衝雷射鍍膜法製備鈣鈦礦型鐵電薄膜之研究",清華大學,博士論文,(1994).
    58.李雅明"固態電子學",全華科技,(1995).
    59.林居南,"添加劑對鈦酸鋇陶瓷電性及相變化之影響",清華大學,博士論文,(1990).
    60. Y. Xu, "Ferroelectric Materials and Their Applications", published by North-Holland Netherlands, (1991).
    61. B. Jaffe, W. R. Cook, Jr and H. Jaffe, "Piezoelectric Ceramics", published by Academic Press Limited, (1971)94.
    62. G. A. Smolenskii and V. A. lsupov, "The Ferroelectric of Solid Solution of Barium Stannate in Barium Titanate", Dokl. Akad. Nauk SSSR, 8, (1954) 1375.
    63. V. 1. Frisberg and B. N. Rolov, "Some Factors That Determine the
    Character of a Ferroelectric Phase Transition", lzv Akad. Nauk SSSR, Ser. Fiz., 28, (1964) 649.
    64. W. Kanzig, Helv. Phys. Acta, 24, (1951) 175.
    65. G. A. Smolenskii, "Physical Phenomena in Ferroelectrics with Diffused Phase Transition", J. Phys. Soc. Jpn., 28(suppl), (1970) 26.
    66. W. R. Buessern, L. E. Cross, and A. K. Goswami, "Phenomenological Theory of High Permittivity in Fine-Grained Barium Titanate", J. Am. Ceram. Soc., 49, (1966) 33.
    67. S. K. Chiang, W. E. Lee, and D. W. Readey, "Core-Shell Structure in Doped BaTiO@", Am. Ceram. Soc. Bull., 66(8), (1987) 1230.溶凝膠薄膜之研究",清華大學,碩士論文,(1995).
    68. T. R. Armstrong, L. E. Morgens, A. K. Maurice and R. C Buchanan, "Effects of Zirconia on Microstructure and Dielectric Properties of Barium Titanate Ceramics", J. Am. Ceram. Soc., 72(4),(1989) 605.
    69. H. Y. Lu, J. S. Bow, and W. H. Deng, "Core-Shell Structure in ZrO2-Added BaTiO3 Ceramics", J. Am. Ceram. Soc., 73(12), (1990) 3562.
    70. D. Barb, Eva Barbulescu, and A. Barbulescu, "On the Ferroelectric Structural Phase Transitions in Solid Solutions", Phys. Stat. Sol. (a), 73, (1982) 603.
    71.R. A. Roy, K. F. Etzold, J. J. Cuomo, and T. J. Watson, "Ferroelectric Film Synthesis, Past and Present: A Select Review", Mater. Res. Soc. Symp. Proc., 200, (1990) 141.
    72.何建成,"鐵電陶瓷之化學製備法及其特性研究",清華大學,博士論文,(1993).
    73.汪建氏彭成鑑,陳三元,"強介電陶瓷薄膜專題緒論",工業材料,107,(1995)44.
    74. C. Feidman, Rev. Sci. Instr., 26, (1955) 463.
    75. B. Chapman, "Glow Discharge Processes", published by John Wiley & Sons, Inc., (1980).
    76. 0. Auciello, A. 1. Kingon, and S. B. Krupanidlii, "Sputter Synthesis of Ferroelectric Films and Heterostructures", MRS Bulletin, 20,(1996)25.
    77.吳泰伯,"強介電薄膜之物理氣相沉積技術",工業材料,109,(1996)135.
    78.0. Auciello and R. Ramesh, "Laser-Ablation Deposition and Characterization of Ferroelectric Capacitors for Nonvolatile Memories", MRS Bulletin, 20(6), (1996)31.
    79. J. Dieleman, E. van de Riet, and J. C. S. Kools, "Laser Ablation Deposition: Mechanism and Application", Jpn. J. Appl. Phys., 31(6B), (1992) 1964.
    80. A. Yuuki, M.yamamuka, T. Makita, T. Horikawa, T. Shibano, N. Hirano, H. Maeda, K. Ono, H. Ogata, and H. Abe, "Novel stacked capacitor technology for 1 Gbit DRAM's with CVD-(Ba,Sr)TiO3 thin film on a thick storage node of Ru," in IEDM Tech. Dig., 1995, pp.115-115.
    81. K. Abe and S. komatsu, "Epitaxial growth and dielectric properties of Ba0.24Sr0.76TiO3 thin film," Jpn. J. Appl. Phys., vol. 33, pp.5297-5300, 1994.
    82. P. Bhattacharya, K. H. Park, and Y. Nishhioka, "Control of grain structure of laser-deposited (Ba,Sr)TiO3 films to reduce leakage current," Jpn. J. Appl. Phys., vol.33, pp.5231-5234, 1994.
    83. J. J. Lee, C. L. Thio, and S. B. Desu, "Electrode contacts on ferroelectric Pb(ZrxTi1-x)O3 and SrBi2Ta2O9 thin films and their influence on fatique properties," J. Appl. Phys., vol.78, pp. 5073-5078, 1995.
    84. Ming shiahn Tsai, S. C. Sun, Tseung-Tseng, "Effect of bottom electrode materials on the electrical and reliability characteristic of (Ba,Sr)TiO3 capacitors," IEEE Trans. Electron. Devices, vol. 46, No. 9, pp. 1829-1838, 1999.

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