簡易檢索 / 詳目顯示

研究生: 李秉樺
Li, Ping-Hua
論文名稱: 以射頻磁控濺鍍製備釹鈰銅氧氧化物和鐵酸鉍之薄膜特性
The Properties of Nd1.85Ce0.15CuO4+y and BiFeO3 Thin Films grown By RF Magnetron Sputtering
指導教授: 齊孝定
Qi, Xiaoding
學位類別: 碩士
Master
系所名稱: 工學院 - 材料科學及工程學系
Department of Materials Science and Engineering
論文出版年: 2015
畢業學年度: 103
語文別: 中文
論文頁數: 92
中文關鍵詞: 鐵酸鉍釹鈰銅氧氧化物磁控濺鍍
外文關鍵詞: BiFeO3, Nd1.85Ce0.15CuO4+y, RF magnetron sputter
相關次數: 點閱:87下載:2
分享至:
查詢本校圖書館目錄 查詢臺灣博碩士論文知識加值系統 勘誤回報
  • 在鐵電材料中,鐵酸鉍(BiFeO3,BFO)是同時在室溫下具有鐵電性和反鐵磁性的材料,具有做成元件的潛力。但BFO仍有漏電流問題需克服,故本研究目的是想找導電的氧化物材料來當底電極層,期望克服此問題,並討論兩種材料製作過程所遇到的問題及薄膜特性。
    本研究企圖在SrTiO3 (STO)基板上成長Nd1.85Ce0.15CuO4+y (NCCO)氧化物磊晶薄膜,當作底電極,在其上成長多鐵性BiFeO3 (BFO)薄膜。NCCO單層膜以及BFO/NCCO/STO多層結構,均以射頻磁控濺鍍製備,所用之NCCO和BFO靶材則籍由固態反應燒結而成。為達到磊晶成長之目的,我們嘗試了多種濺鍍參數,并進行後續退火處理。成長於(001)STO基板上之NCCO單層膜雖有明顯的(001)擇優取向,但其中仍有少許的(110)取向,而NCCO的(110)晶粒由於晶格匹配的關係,在隨後的BFO成長中會誘導二次相Bi24Fe2O39的生成,導致BFO薄膜成長失去控制,無法形成磊晶。在電性方面,霍爾量測證實所成長之NCCO薄膜有很高的導電率,足以作爲電極。

    In this work, Nd1.85Ce0.15CuO4+y (NCCO) was studied as the bottom electrode for the epitaxial growth of multiferroic BiFeO3 (BFO) films on the SrTiO3 (STO) substrates. The growth of the single NCCO layer on (001) STO substrate, as well as the BFO/NCCO/STO multilayers, was attempted by the RF magnetron sputtering. The NCCO and BFO targets used in the sputtering deposition were homemade via the solid-state reaction method. Various growth parameters were studied in order to obtain epitaxial films. The phase purity, texture, surface morphology and electrical conductivity of the sputtered NCCO films were examined by X-ray diffraction, scanning electron microscopy and Hall-effect. The effects of the NCCO film property on the subsequent BFO film growth and its ferroelectric property were also studied.

    摘要…I Extended Abstract…II 致謝…IX 目錄…X 圖目錄…XIII 表目錄…XVII 第一章 緒論…1 1-1 前言…1 1-2 研究動機與目的…2 第二章 文獻回顧及理論基礎…4 2-1 鐵電材料介紹…4 2-1-1 鐵電材料結構…4 2-1-2 鐵電材料電滯曲線…7 2-2 極化機制…9 2-3 漏電流機制…12 2-4 釹鈰銅氧氧化物…16 2-4-1 晶體結構…16 2-4-2 〖" Nd" 〗_1.85 〖"Ce" 〗_0.15 CuO_(4+y)薄膜製程和特性…17 2-5 鐵酸鉍(BiFeO3)…18 2-5-1 晶體結構…18 2-5-2 電性性質…21 2-6 晶格匹配…23 第三章 實驗方法與步驟…25 3-1 實驗藥品…25 3-2 實驗流程…26 3-2-1 固相反應法製作氧化物靶材…28 3-2-2 基板清理步驟…30 3-3 實驗製程設備…30 3-3-1 靶材製程的實驗設備…30 3-3-2 射頻磁控濺鍍機原理和機台…31 3-4 實驗分析儀器…34 3-4-1 X光繞射儀(X-ray diffraction)…34 3-4-2 掃描式電子顯微鏡…39 3-4-3 霍爾量測…40 3-4-4 電滯曲線測量儀…43 3-4-5 X光光電子能譜儀(X-ray Photoelectron Spectroscopy)…44 3-4-6 表面粗度儀(Alpha-step Profilometer)…46 3-4-7 原子力顯微鏡 (Atomic force microscope)…47 3-4-8 電阻-溫度測量儀(Resistance-Temperture Measurement)…49 第四章 實驗結果與討論…50 4-1 〖" Nd" 〗_1.85 〖"Ce" 〗_0.15 CuO_(4+y) 樣品製備與分析…50 4-1-1〖" Nd" 〗_1.85 〖"Ce" 〗_0.15 CuO_(4+y) 靶材的製備與分析…50 4-1-2〖" Nd" 〗_1.85 〖"Ce" 〗_0.15 CuO_(4+y) 薄膜的製備與分析…53 4-2 BiFeO_3 樣品製備與分析…61 4-2-1 BiFeO_3 薄膜的製備與分析…61 4-3 〖"Nd" 〗_1.85 〖"Ce" 〗_0.15 CuO_(4+y) 和BiFeO_3 之表面形貌與成份分析…65 4-3-1 〖"Nd" 〗_1.85 〖"Ce" 〗_0.15 CuO_(4+y)塊材的表面形貌與成份分析…65 4-3-2 〖"Nd" 〗_1.85 〖"Ce" 〗_0.15 CuO_(4+y)薄膜的表面形貌與成份分析…66 4-3-3 BiFeO_3薄膜的表面形貌與成份分析…72 4-4 〖"Nd" 〗_1.85 〖"Ce" 〗_0.15 CuO_(4+y) 霍爾量測及電性分析…78 4-5 電滯曲線量測…81 第五章 結論…85 參考文獻…87

    [1].R. Ramesh, “Thin Film Ferroelectric Materials and Devices”, Kluwer Academic, London, Chap1-3 (1997).
    [2].J. F. Scott, and C. A. Araujo, “Ferroelectric Memory”, Sci., 246, 1400 (1989).
    [3].H. S. Nalwa, “Ferroelectric and dielectric thin films”, Academic press, New York (2002).
    [4].H. Uchida, R. Ueno, H. Nakaki, H. Funakubo and S. Koda, “Ion Modification for Improvement of Insulating and Ferroelectric Properties of BiFeO3 Thin Films Fabricated by Chemical Solution Deposition”, Appl. Phys., 44, l561 (2005).
    [5].K. U. H. Tabata and T. Kawai, “Coexistence of ferroelectricity and ferromagnetism in BiFeO3-BaTiO3 thin film at room temperature”, Appl. Phys. Lett., 75, 555 (1999).
    [6].X. Qi, J. Dho, R. Tomov, M. G. Blamire, J. L. MacManus-Driscoll, “Greatly reduced leakage current and conduction mechanism in aliovalent-ion-doped BiFeO3”, Appl. Phys. Lett., 86, 062903 (2005).
    [7].M. M. Kumar and V. R. Palka, “Ferroelectricity in a pure BiFeO3 ceramic”, Appl. Phys. Lett., 76, 2764 (2000).
    [8].呂正傑, 詹世雄, “鐵電記憶體簡介”, 奈米通訊, 第五卷, 第四期 (1998)
    [9].鄭佩慈, “鐵電材料隻特性運用”, 儀器科學中心簡訊, 68期 (2005)
    [10].P. Ghosez and K. M. Rabe, Appl. Phys. Lett., 76, 2767 (2000)
    [11].M. E. Lines and A. M. Glass, “Principles and Applications of Ferroelectrics and Related Materials”, Clarendon Press, Oxford (1977).
    [12].B. Meyer, D. Vanderbilt, Phys. Rev. B, 65, 104111 (2002).
    [13].R. Yu, H. Krakauer, Phys. Rev. Lett. 74, 4067 (1995).
    [14].曲遠方, “功能陶瓷材料”, 皢園出版社, 台北市 (2006年)
    [15].W.D.Kingery, H.K. Bowen and D.R. Uhlmann, “陶瓷材料概論”, 皢園出版社, 台北市 (1998年)
    [16].G.H.Hartling, “Ferroelectric Ceramics : History and Technology”, J. Am. Ceram. Soc., 82, 4, 797-818 (1999).
    [17].M. E. Lines and A. M. Glass, “ Principle and applications of ferroelectrics and related materials”, Oxford University, New York (2001)
    [18].M.Barsoum, “Fundamentals of Ceramics”, McGrAW Hill, New York (2001)
    [19].B. H. Park, B .S. Kang, S. D. Bu,T. W. Noh, J. Lee and W. Jo, “Lanthum-substituted bismuth titanate for use in non-volatile memories”, Nature, 401,682 (1999).
    [20].林麗娟, “X光繞射原理極其應用”,工業材料86期 (1994).
    [21].S. M. Sze, “Physics of Semiconductor Devices”Wiley, New York (1981)
    [22].I. Stolichnovb and A. Taganstev, “Space-charge influenced-injection modle forconduction in Pb(ZrxTi1-x)O3 thinfilms”, J. Apple. Phys. Lett., 84, 3216 (1998)
    [23].G. Spinolo, M. Scavini, P. Ghigna, G. Chiodelli, G. Flor, “Nature and amount of carriers in Ce doped Nd2CuO4 I. High-temperature characterization”, Phy. C, 254, 359-369 (1995)
    [24].Kojima et a1. , “United States Patent”, US (1995)
    [25].K .Setsune, S. Hayashi, H. Adachi, K. Hirochi, S. Kohiki, S. Hatta and K. Wasa, “ Superconducting thin films of n-type copper oxide prepared by rf magnetron sputtering”, Vacuum, 41,864- 866 (1990).
    [26].Y. Tokura, H. Takagi, S. Uchida. ,“A superconducting copper oxide compound with electrons as the charge carriers ”, Nature , 337, 345 – 347 (1989)
    [27].A. Guarino, R. Fittipaldi, A. Romano, A. Vecchione, A. Nigro, “ Correlation between structural and transport properties in epitaxial films of Nd 2− x Ce x CuO 4±δ”, Thin Solid Films , 524 , 282–289 (2012)
    [28].M. Hoek, F. Coneri, D. P. Leusink, P. D. Eerkes, X. R. Wang and H. Hilgenkamp, “Effect of high oxygen pressure annealing on superconducting Nd1.85Ce0.15CuO4 thin films by pulsed laser deposition from Cu-enriched targets”, January, 27, 4 (2014).
    [29].R. F. Jardim, E. A. Early, M. B. Maple, “Properties of polycrystalline Nd1.85Ceo.15CuO4-y prepared under different conditions”, Journal of Alloys and Compounds, 221, 1-14 (1995)
    [30].J. H. Lee, M. A. O, H. J. Choi, J. Y. Son and H. M. Jang, “Rhombohedral–orthorhombic morphotropic phase boundary in BiFeO3-based multiferroics: first-principles prediction”, J. Mater. Chem., 22, 1667-1672 (2012)
    [31].B. Ruette, MS thesis, Virginia Tech. (2003)
    [32].H. Naganuma, “Multifunctional Characteristics of B-site Substituted BiFeO3Films”, Department of Applied Physics, Tohoku University, Japan (2011)
    [33].N. Krainik, “On the room temperature multiferroic BiFeO3: Magnetic, dielectric and thermal properties”, Phys., 8, 654 (1966)
    [34].J. Wang, “Deposition and Characterization of Multiferroic BiFeO3 Thin Films”,PhD dissertation, University of Maryland, Department of Materials Science and Engineering (2005)
    [35].J. R. Teague, R. Gerson, W. J. James, “Dielectric hysteresis in single crystal BiFeO3”, Solid State Commun., 8, 1073 (1970)
    [36].X. Qi, J. Dho, R. Tomov, M. G. Blamire, J. L. MacManus-Driscoll, “Greatly reduced leakage current and conduction mechanism in aliovalent-ion-doped BiFeO3”, Appl. Phys. Lett., 86, 062903 (2005)
    [37].Y. P. Wang, L. Zhou , M. F. Zhang, X. Y. Chen, J. M. Liu and Z.G. Liu,“Room-temperature saturated ferroelectric polarization in BiFeO3 ceramics synthesized by rapid liquid phase sintering”, Appl. Phys. Lett., 84, 1731 (2004)
    [38].V. R. Palkar, K. G. Kumara and S. K. Malik, “Observation of room-temperature magnetoelectric coupling in pulsed – laser – deposited Bi0.6Tb0.3La0.1FeO3 thin films”, J. Phys., 58, 1003 (2002)
    [39].K. Y. Yun, M. Noda, M. Okuyama, H. Saeki, H. Tabata, K. Saito, “Structural and multiferroic properties of BiFeO3 thin films at room temperature”, J. Appl. Phys., 96, 3399 (2004)
    [40].M. I. Morozov, N. A. Lomanova, V. V. Gusarov, “Specific features of BiFeO3 formation in a mixture of bismuth(III) and iron(III) oxides”, Russian Journal of General Chemistry, 73, 11 (2003)
    [41].Y. E. Roginskaya, Y. Y. Tomashpol'Skiǐ, Y.N. Venevtsev, V. M. Petrov, G. S. Zhdanov, “The Nature of the Dielectric and Magnetic Properties of BiFeO3”, Soviet Physics JETP, 23, 47 (1996)
    [42].Sov. Phys.,23, 47, (1996)
    [43].林蔚叡, 博士論文, “以鐵酸鉍複鐵式材料為釘札層製作全氧化物自旋閥之研究,成功大學材料科學與工程學系” (2014)
    [44].汪建民, “材料分析”, 中國材料年會, 47-53和353-359 (1998)
    [45].鄭信民, 林麗娟, “ X光繞射應用簡介, 工業材料雜誌”, 181期,105-106 (2002)
    [46].D. A. Skoog, F. J. Holler, S. R. Crouch, “Principles of Instrumental Analysis 6rd”, Canada:BROOKS/COLE, 608-609 (2007)
    [47].黃調員譯, “半導體元件物理與製作技術(第二版)”, 新竹市:交大出版社, 87-90和96-98 (2010)
    [48].ARTHUR W.ADAMSON原著, 陶雨台譯, “表面物理化學”, 千華圖書出版事業有限公司 (1990)
    [49].J. C. Vickerman, “Surface Analysis- The Principal Techniques”, UK (1997).
    [50].K. Hayashi, S. Adachi, H. Mitsuyu, T. Hirao, T. Setsune, K. Wasa, K. Affiliation, “Optical properties of Nd2-xCexCuO4 thin films”, Physica C, 160 , 273-277 (1989)
    [51].羅建興, 碩士論文, “雷射蒸鍍法於釹鈰銅氧超導膜上磊晶生長鐵電膜之研究, 成功大學材料科學與工程學系” (1994)
    [52].X. Qi, W. C. Chang, J. C. Kuo, I. G. Chen, Y. C. Chen, C. H. Ko, J. C. A. Hung, “Growth and characterisation of multiferroic BiFeO3 films with fully saturated ferroelectric hysteresis loops and large remanent polarisations”, J. Eur. Ceram. Soc., 30, 2, 283-287 (2010)
    [53].X. Qi, P. C. Tsai, Y. C. Chen, C. H. Ko, J. C. A. Hung and I. G. Chen, “Ferroelectric properties and dielectric responses of multiferroic BiFeO3 films grown by RF magnetron sputtering” , J. Phys. D: Appl. Phys., 41, 23, 232001 (2008)
    [54].X. Qi, P. C. Tsai, Y. C. Chen, Q. R. Lin, J. C. A. Hung, “Optimal growth windows of multiferroic BiFeO3 films and characteristics of ferroelectric domain structures”, Thin Solid Films, 517, 20, 5862-5866 (2009)
    [55].Z. Quan, H. Hu, S. Xu , W. Liu, G. Fang, M. Li , X. Zhao, “Surface chemical bonding states and ferroelectricity of Ce-doped. BiFeO3 thin films prepared by sol–gel process”, J Sol-Gel Sci Technol, 48,261–266 (2008)
    [56].K. Hirochi, S. Hayashi, H. Adachi, T. Mitsuyu, T. Hirao, K. Setsune and K.Wasa, “OPTICAL PROPERTIES OF Nd2-xCexCuO4 THIN FILMS”, Physica C, 160, 273-277 ( 1989)

    下載圖示 校內:2025-12-31公開
    校外:2020-08-31公開
    QR CODE