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標題: 低溫水熱化學電池法於氮化鈦膜上製備鈦酸鍶鋇薄膜之研究
Low-temperature hydrothermal galvanic couple synthesis of barium strontium titanate thin films on TiN/Si substrates
作者: 詹佩諠
Pei-Hsuan Chan
關鍵字: 水熱;化學電池;氮化鈦;鈦酸鍶鋇;hydrothermal;galvanic couple;TiN;BaxSr1-xTiO3(BST)
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鈦酸鍶鋇(BaxSr1-xTiO3, BST)為鈣鈦礦結構,是BaTiO3和SrTiO3之固溶體,具有優異的介電等特性,可應用於各種相關器件。本水熱-化學電池製程,主要是利用化學電池的自發性反應輔以降低水熱製程溫度要求,相當符合現今環保及節能之要求,在低於100 oC常壓下,並以導電性及特性優異氮化鈦(TiN)薄膜作為底材,製備多元金屬BaxSr1-xTiO3薄膜,相較過去相關文獻中多數使用Ti塊材製備BaxSr1-xTiO3薄膜,TiN薄膜不僅具奈米尺寸效應,近年來常被應用於電極上,相當具有發展潛力。本研究主要是利用水熱-化學電池法,於TiN/Si基材上製備BaxSr1-xTiO3薄膜,探討製程方式、底材及溶液成份變化對製備BaxSr1-xTiO3薄膜之影響。
在TiN膜、Ti膜及Ti塊材等不同底材製備鈦酸鋇膜,TiN/Si由於具有較小奈米顆粒的表面形貌,且本身結構特性影響,成長鈦酸鋇較Ti膜及Ti塊材成長之速率來的快,且製備出之BaTiO3膜具高優選方向,受試片底材本身的方向性及特性所影響,當反應時間固定2小時時,生成溫度高低比為Ti塊材(60oC) > Ti膜(52.5oC) > TiN膜(45oC)。
水熱-化學電池法於TiN上製備立方相之多元BaxSr1-xTiO3膜,薄膜具高結晶方向性,薄膜特性和微結構受薄膜成份影響,改變溶液中Ba與Sr離子的比例或總濃度,可控制BaxSr1-xTiO3膜成份及微結構變化,其中BaxSr1-xTiO3膜隨著Ba與Sr的含量不同其繞射峰有所偏移,因Ba與Sr離子半徑不同,導致晶格產生變化,也影響薄膜結晶性,另外因BaTiO3與TiN晶格之匹配率大於SrTiO3,也影響薄膜成長機制,而介電諧調率在Ba0.75Sr0.25TiO3膜上可達92%,顯示所製備出多元 BST膜具優異介電特性。

Barium titanate (BaxSr1-xTiO3, BST) is a solid solution of BaTiO3 and SrTiO3. It has excellent dielectric properties and can be applied to various related devices. The hydro-thermal-galvanic couple process utilizes the spontaneous reaction of the galvanic cell to reduce the hydrothermal process temperature requirements, which meets the current en-vironmental and energy-saving requirements. The preparation of multi-component BaxSr1-xTiO3 film over conductive TiN seeding layer was conducted at < 100oC under normal pressure by the hydrothermal-galvanic couple method. The reaction concentra-tions were 2 M NaOH mixed with various and concentrations of Ba(CH3COO)2 and Sr(CH3COO)2. The effects of process, substrate, and solution concentration on the preparation of BaxSr1-xTiO3 films were investigated.
The growth rate of BaTiO3 in the hydrothermal-galvanic couple method is much faster than that in sole hydrothermal method, and the reaction temperature could be also lowered. The reaction mechanism, crystallinity, and microstructure of films were similar to those prepared by a hydrothermal method. Compared with the hydrother-mal-electrochemical method, the hydrothermal-galvanic method without applying ex-ternal voltage/current though had a slower growth rate while possessed even film thick-ness and the films showed preferred orientation. BaTiO3 films were prepared on TiN and Ti-coated Si as well as bulk-Ti substrates by the hydrothermal method at temperatures below 100oC. The ease of forming BaTiO3 on TiN/Si is due to structural characteristics and the nano-grained nature of TiN films. The cubic BaTiO3 films were successfully formed on TiN/Si and Ti/Si over a period of 2 hr at temperatures as low as 45oC and 52.5oC, respectively while formation of BaTiO3 on bulk-Ti required temperatures ex-ceeding 60oC for the same reaction time.
The hydrothermal-galvanic couple method was used to prepare cubic BaxSr1-xTiO3 films on TiN. BaxSr1-xTiO3 films were found to grow epitaxially over the TiN underlayer with a strongly preferred orientation. BaxSr1-xTiO3 films with various grain sizes have been controlled by merely varying the total concentration or the Ba/(Ba+Sr) ratio of the reaction solutions during the hydrothermal-galvanic couple synthesis. The diffraction peaks of BaxSr1-xTiO3 film shifed due to the different contents of Ba and Sr. Because of the different radii of Ba and Sr ions, the lattice changes and the film crystallinity is also affected. The dielectric tenability of Ba0.75Sr0.25TiO3 can reach up to 92%, indications superior dielectric characteristics of BST.
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