應用混合薄膜及雙層結構改善單層二氧化鉿薄膜電阻轉換的均勻性

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張哲維(Jhe-wei Chang) 查詢紙本館藏

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化學工程與材料工程學系

論文名稱

應用混合薄膜及雙層結構改善單層二氧化鉿薄膜電阻轉換的均勻性
(Uniformity Improvement of Resistive Switching in HfO2 Thin Films with Mixed Oxide and Bilayer Structure)

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摘要(中)

電阻式記憶體(RRAM)結合了快閃記憶體的非揮發性、靜態存取記憶體的快速存取、動態存取記憶體的高密度，配合低耗能、低成本、構造簡單、保存資料能力佳的優勢，使其在非揮發性記憶中受到極大的矚目。但直至今日，電阻式記憶體的高低阻態隨著施加偏壓而改變的轉換機制尚未明瞭，導致電阻式記憶體的電阻轉換均勻性仍有待改善。
本實驗使用MOCVD方式沉積HfO2薄膜及不同厚度的Al2O3薄膜，利用混合以及雙層薄膜結構，濺鍍Ni金屬電極於薄膜上，開發金屬/氧化層/半導體的三明治(sandwich)結構之RRAM元件，藉此改善單層HfO2的電阻轉換均勻性缺點。以Al2O3薄膜在HfO2薄膜的上層或下層或者改變上層Al2O3薄膜厚度，去區分雙層薄膜的電阻轉換特性。當Al2O3薄膜在HfO2薄膜的下方時，只能操作Bipolar switching，而當Al2O3薄膜在HfO2薄膜的上方時，可以操作Nonpolar switching，但當Al2O3薄膜厚度達到一定厚度時，只能操作Bipolar switching。另外藉由單層薄膜的電性量測，去加以驗證其燈絲機制是以金屬Ni主導或是氧空缺主導。最後，本實驗利用此結果，建立其電阻轉換機制。

摘要(英)

Resistance Random Access Memory (RRAM) has attracted increasing attention in recent years as the next-generation nonvolatile memory, due to its non-volatile property like Flash memory, fast access speed like SRAM, high-density storage like DRAM. Furthermore, RRAM has the advantages of low-power operation, low cost, simple structure, and good retention. However, understandings of RRAM mechanisms behind resistive-switching (RS) were still unknown. So it is hard to well control the uniformity of RS behaviors.
In this study, various thickness of the Al2O3 layer and HfO2 layer by MOCVD deposition with the Ni top electrode. The improved uniformity of RS behaviors is demonstrated in the HfAlOX mixed oxide and the Al2O3/HfO2 bilayer RRAM devices. Furthermore, the RS properties of the bilayer structure with various Al2O3 thicknesses and the position of Al2O3 layer compared to the HfO2 have been investigated. Finally, we established the possible RS mechanisms in detail according to the electrical and physical analysis.

關鍵字(中)

★ 均勻性改善
★ 三氧化二鋁
★ 二氧化鉿
★ 雙層結構
★ 混合薄膜
★ 電阻式記憶體

關鍵字(英)

★ RRAM
★ Mixed oxide
★ Bilayer structure
★ HfO2
★ Al2O3
★ Uniformity improvement

論文目次

誌謝......................................................i
摘要......................................................i
Abstract.................................................ii
目錄....................................................iii
圖目錄...................................................ix
表目錄...................................................xv
第一章、緒論..............................................1
1-1 前言..................................................1
1-2 研究動機..............................................2
第二章、簡介及文獻回顧....................................3
2-1 記憶體簡介............................................3
2-1-1 磁阻式記憶體（MRAM).................................4
2-1-2 鐵電記憶體（FeRAM）.................................5
2-1-3 相變化記憶體（PCRAM）...............................5
2-1-4 電阻式記憶體（RRAM）................................6
2-2 電阻式記憶體轉換現象與量測方式........................8
2-2-1 電阻轉換現象（Switching phenomenon）................8
2-2-2 電阻式記憶體量測種類...............................10
2-3 電阻轉換現象機制.....................................11
2-3-1 熱化學效應.........................................12
2-3-2 金屬離子的電化學效應...............................13
2-3-3 價電子轉換效應.....................................14
2-4 電阻式記憶體材料....................................15
2-4-1 多元金屬氧化物.....................................16
2-4-2 過度金屬氧化物.....................................16
2-4-3 有機材料...........................................19
2-5 漏電流介紹...........................................21
2-5-1 歐姆電流(Ohmic current)............................21
2-5-2直接穿隧 (Direct tunneling).........................21
2-5-3傅勒−諾得翰穿隧 (Fowler−Nordheim tunneling).........22
2-5-4空間電荷限制傳導(Space charge limited conduction)...23
第三章實驗流程.........................................42
3-1 試片的製備...........................................42
3-1-1 下電極及基板的製備.................................42
3-1-2 介電層二氧化鉿（HfO2）以及三氧化二鋁 (Al2O3) 的沉積42
3-1-3 退火條件...........................................43
3-1-4 上電極的製備.......................................43
3-2 薄膜物性分析.........................................44
3-2-1 薄膜結晶性分析（XRD）..............................44
3-2-2 場發射穿透式電子顯微鏡（TEM）及X射線能量散佈分析儀（EDS）..................................................44
3-2-3 歐傑電子顯微鏡(AES) & 化學分析電子儀(ESCA).........45
3-2-4 二次離子質譜儀（SIMS）.............................45
3-3 電性量測.............................................46
3-3-1 電流-電壓量測（I-V curve）.........................46
3-3-2 電阻-時間之關係....................................46
3-3-3 電阻-溫度之關係....................................47
第四章、混合薄膜結果與討論...............................54
4-1 薄膜結構分析.........................................54
4-1-1 X光繞射分析（XRD）.................................54
4-1-2 X光光電子能譜儀（XPS）.............................54
4-2 電性量測分析.........................................56
4-2-1 HfAlOx薄膜的I-V特性................................56
4-2-2 HfO2薄膜與混合比例4:1的HfAlOx薄膜I-V特性比較......58
第五章、雙層結構結果與討論...............................74
5-1 薄膜結構分析.........................................74
5-1-1 場發射穿透式電子顯微鏡（TEM）......................74
5-1-2 X射線能量散佈分析儀（EDS）.........................75
5-1-3 歐傑電子顯微鏡(AES)................................75
5-2 電性量測分析.........................................75
5-2-1 不同的Al2O3厚度對Forming process的影響.............76
5-2-2 雙層薄膜結構的Forming curve 比較...................76
5-2-3 雙層薄膜結構的Bipolar特性..........................77
5-2-4 雙層薄膜結構的Unipolar特性.........................78
5-2-5 在限流50μA下的單層與雙層Ni/ Al2O3/ HfO2/ Si結構累積分布圖...................................................78
5-2-6 在限流100μA下的單層與雙層Ni/ Al2O3/ HfO2/ Si結構累積分布圖...................................................80
5-2-7 不同限流條件下的單層與雙層薄膜結構累積分布圖.......82
5-3電阻轉換機制..........................................82
5-3-1 單層結構電阻轉換發生的機制.........................82
5-3-2 Ni/ HfO2/ Al2O3/ Si結構電阻轉換發生的機制..........83
5-3-3 Ni/ Al2O3/ HfO2/ Si結構電阻轉換發生的機制..........84
第六章、結論............................................108
6-1 混合薄膜HfAlOX結構..................................108
6-2 雙層薄膜結構........................................109
第七章、未來與展望......................................110
參考文獻................................................111

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指導教授

周正堂(Cheng-tung Chou)

審核日期

2011-7-19

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