濺鍍氮氧化矽薄膜以及氮氧化矽/矽多層膜之結構與發光性質研究

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研究生：	廖藝澤 Yi-Tse Liao
論文名稱：	濺鍍氮氧化矽薄膜以及氮氧化矽/矽多層膜之結構與發光性質研究 Structural and Luminescent Properties of Sputter Deposited Silicon Oxynitride Films and Multi-layered Silicon Oxynitride/Silicon Stack
指導教授：	周賢鎧 Shyan-Kay Jou
口試委員:	黃柏仁 Bohr-Ran Huang 胡毅 Yi Hu
學位類別：	碩士 Master
系所名稱：	工程學院 - 材料科學與工程系 Department of Materials Science and Engineering
論文出版年：	2011
畢業學年度：	99
語文別：	中文
論文頁數：	96
中文關鍵詞：	氮氧化矽、磁控式濺鍍、量子點、光激發螢光、電激發光
外文關鍵詞：	Silicon oxynitride, Magnetron sputtering, Quantum dots, PL, EL
相關次數：	點閱：338 下載：28
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上一筆

本研究利用反應式磁控濺鍍(Magnetron sputtering)系統配合高真空下的熱退火製程，成功製備出含有不同氮、氧濃度之氮氧化矽(SiOxNy)單層薄膜以及氮氧化矽/矽(SiON/Si)之多層膜結構。
利用X光光電子能譜儀(XPS)的對Si 2p3/2、N 1s、O 1s進行分析，發現束縛能位置會隨著製備條件的不同而改變，根據不同的束縛能位置可將薄膜內部的鍵結狀態分為四類，Si─N4、Si─N3O、Si─O3N以及Si─O4，其對應到的四種鍵結單元分別為Si3N4、Si2ON2、Si6O9N2 以及SiO2。其中氮化矽(Si3N4)結構中含有大量的氮懸掛鍵(Nitrogen dangling bond)，而氮氧化矽(Si2ON2、Si6O9N2)結構中則含有大量的O─Si─N鍵結。經過拉曼光譜與穿透式電子顯微鏡的分析，證明氮氧化矽單層膜的內部在退火後並沒有矽團簇生成。
利用He-Cd 325 nm的雷射在室溫下進行光激發螢光光譜的量測，可觀察到三支來自於缺陷態的發光峰，分別位於約400 nm, 510 nm及780 nm的位置。在氮濃度較高、氧濃度較低的樣品中，其鍵結單元以氮化矽為主，因此由氮的懸掛鍵主導薄膜的發光性質，反映在PL光譜中為較強的藍色(400 nm)發光；在氧濃度較高、氮濃度較低的樣品中，其鍵結單元以氮氧化矽為主，因此由O─Si─N鍵結主導薄膜的發光性質，反映在PL光譜中為較強的綠色(510 nm)發光。位於780 nm的發光峰可能由N 2p及O 2p能態之間的復合行為所造成。在氮氧化矽/矽之多層膜結構中，利用PL的量測可觀察到偏綠之白色螢光現象，經過分峰後發現除了上述三支發光峰外，又額外增加了一支發光峰位於~610 nm的位置，此峰可能來自於矽層中形成的矽量子點，造成了量子侷限效應所貢獻。
最後將氮氧化矽(SiOxNy)單層薄膜以及氮氧化矽/矽(SiON/Si)之多層膜製備成ITO/SiON/Si Wafer/Al的元件，並成功觀察到電激發光的現象。由電壓-電流曲線指出其導電機制可能為空間電荷傳導，其發光現象源自載子於缺陷態中復合所造成。此外，光激發光與電激發光皆具有相似的發光波段，而且只出現在退火後的樣品中，證明了兩者的發光行為來自於相同的復合中心。

Silicon oxynitride (SiOxNy) and multi-layered silicon oxynitride/silicon structures (SiON/Si) with different nitrogen and oxygen concentrations were fabricated by reactive magnetron sputtering deposition followed by thermal annealing in high vacuum environment.
According to the x-ray photoelectron spectroscopy analyses, the binding energies of Si 2p3/2, N 1s and O 1s shift with deposition condition of SiON. Four tetrahedral phases such as Si─N4, Si─N3O, Si─O3N, and Si─O4 are possibly present, corresponding to the four bonding units Si3N4, Si2ON2, Si6O9N2 , SiO2. Si3N4 is believed to be the origin of nitrogen dangling bonds, and silicon oxynitride structures like Si2ON2 and Si6O9N2 are the origin of O─Si─N bonds. In combination with analyses of Raman spectroscopy and high resolution transmission electron microscopy, we demonstrate that there is no silicon clusters in the SiON films.
Strong room temperature photoluminescence, excited by He-Cd 325 nm laser, from defect– related states was observed in about 400 nm, 510 nm and 780 nm. It is found that blue emission peak arises from the nitrogen dangling bonds which dominate in the samples with relatively higher nitrogen concentration; the green emission peak originates from the luminescent center of O─Si─N bonds which dominate in the higher oxygen concentration ones; peaks at 780 nm is probably from the recombination between N 2p and O 2p. For multi-layered SiON/Si films, white photolumine- scence was observed due to the additional luminescence at ~610 nm from quantum dots formed in the silicon layers of the film.
Visible electroluminescence was obtained from SiOxNy and multi-layered SiON/Si films on p-type silicon substrate in a ITO/SiON/Si Wafer/Al structure. The I-V behavior is indicative of space charge-limited current, and the EL was possibly attributed to the recombination of carriers through the luminescent center in the SiON layer. The PL and EL were present only in annealed samples, and the emissions are similar from same samples which suggests the recombination centers from PL and EL are the same.

中文摘要........................................................................................................................I
英文摘要......................................................................................................................III
致謝..............................................................................................................................III
目錄..............................................................................................................................V
表目錄.......................................................................................................................VIII
圖目錄...........................................................................................................................X
第一章	前言...............................................................................................................1
第二章	文獻回顧與實驗原理...............................................................................3
   2-1  材料之發光機制介紹.................................................................................3
        2-1.1  光致發光............................................................................................3
        2-1.2  電致發光............................................................................................4
   2-2  矽基發光材料之發光原理........................................................................7
        2-2.1  量子侷限效應....................................................................................7
        2-2.2  缺陷發光..........................................................................................12
    2-3  多孔矽之發光介紹............................................................................13
   2-4  矽/二氧化矽之發光介紹...................................................................15
   2-5  矽/氮化矽之發光介紹.......................................................................18
2-6  氮氧化矽之發光介紹........................................................................... 21
2-6.1  氮氧化矽簡介..................................................................................21
        2-6.2  鍵結分析..........................................................................................21
        2-6.3  藍光之缺陷發光分析......................................................................23
        2-6.4  綠光之缺陷發光分析......................................................................25
  2-7  矽基發光元件之性質分析.......................................................................26
  2-8  真空鍍膜製程.............................................................................................29
        2-8.1  磁控式濺鍍………………………………………………………29
2-8.2  直流與射頻濺鍍系統……………………………………………30
2-8.3  反應式濺鍍……………………………………………………31
第三章	實驗方法與步驟......................................................................................33
   3-1  實驗材料與藥品規格..............................................................................33
   3-2  薄膜製程裝置...........................................................................................34
        3-2.1  磁控式濺鍍系統..............................................................................35
        3-2.2  石英管爐系統..................................................................................36
   3-3  實驗步驟....................................................................................................37
        3-3.1  實驗流程..........................................................................................37
        3-3.2  氮氧化矽薄膜之製備......................................................................39
        3-3.3  元件製作..........................................................................................41
   3-4  薄膜分析與鑑定……………………………………………………44
        3-4.1  表面輪廓儀(Alpha-Step) ................................................................45
        3-4.2  化學分析影像能譜儀(ESCA) ........................................................45
        3-4.3  傅立葉紅外線光譜儀(FTIR) .........................................................45
        3-4.4  顯微拉曼光譜儀(Micro-Raman Spectra) .......................................46
        3-4.5  光激發螢光光譜儀(PL) .................................................................46
3-4.6  電性與電激發光譜量測儀(I-V & EL)...........................................47
第四章	結果與討論...............................................................................................49
4-1  反應式濺鍍速率………………………………………………50
4-2  單層氮氧化矽發光薄膜…………………………………………51
    4-2.1 化學組成與鍵結分析………………………………………………51
    4-2.2 化學結構分析………………………………………………………63
    4-2.3 物理結構分析……………………………………………………73
    4-2.4 光學性質分析……………………………………………………75
4-3  多層氮氧化矽發光薄膜…………………………………………………79
    4-3.1 結構分析……………………………………………………………79
    4-3.2 光學性質分析………………………………………………………80
4-4  發光元件分析……………………………………………………81
第五章 結論……………………………………………………………84
參考文獻..............................................................................................86

                                

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