臺灣博碩士論文加值系統

我們利用溶膠凝膠法製備非晶態LaNbOx(LNO)的薄膜，研究金屬(Al、Ti)/LNO/ITO元件的雙極電阻開關(BRS)特性。其中包括薄膜厚度、頂部電極、退火溫度和金屬後退火(PMA)以及雙層結構對電阻開關(RS)特性的影響。與原沉積的LNO薄膜元件相比，經PMA處理的元件表現出更好的電阻轉換特性，且無需施加一個大的Forming電壓即可使元件達到低組態，具有更低的Set/Reset電壓(VSet/VReset= –2.26V/0.9V)，更長的開關週期(~2466)和約101的記憶窗口。此外，在85℃時，保留時間超過104秒，這與室溫下的保留時間一樣，表明此材料在電阻式隨機存取記憶體(RRAM)的應用是具有潛力的。電阻轉換特性的改善可以歸因於在PMA處理後，在上層電極和絕緣層之間形成了一層氧化鋁介面，這增加了氧空缺的含量，此外在薄膜中發現有金屬離子的擴散，故推測電阻轉換特性而獲得改善。最後，我們在絕緣層上旋塗了一層氧化鋁層與自形成介面層進行比較，發現自形成介面層具有較多的氧空缺，以改善其RS特性。對於任何帶有Al頂部電極的器件來說，有兩種類型的傳導機制。一種是高阻態(HRS)中陷阱控制的空間電荷限制電流(SCLC)，另一種是低阻態(LRS)中的歐姆傳導機制。

Sol-gel thin films of amorphous LaNbOx (LNO) were prepared to study the bipolar resistive switching (BRS) properties of Metal/LNO/ITO devices. We investigated the influences of film thickness, top electrode, annealing temperature, post-metal annealing (PMA), and bilayer structure on the resistive switching (RS) characteristics. In comparison to the as-deposited LNO thin film devices, the PMA-treated devices demonstrated better RS characteristics, with lower set/reset voltages (VSet/VReset = –2.26V/0.9V), longer switching cycles (2466 cycles), and a >101 Ron/Roff ratio. Furthermore, at 85°C, the retention time exceeded 104 seconds, similar to the retention time at room temperature, indicating that random access memory (RRAM) may effectively function over 10 years. The improvement in RS characteristics can be attributed to the formation of an AlOx layer between the upper electrode and the insulating layer after PMA treatment, which increases the oxygen vacancy content and facilitates Al ion diffusion. The addition of a bilayer of Al was implemented to increase the thickness of AlOx, thereby improving the Ron/Roff ratio. However, this addition also degrades the RS properties of the device. Furthermore, the space charge-limited current (SCLC) conduction mechanism dominates in the high resistance state (HRS), while ohmic conduction prevails in the low resistance state (LRS) of the devices.

中文摘要 I
致謝 XV
目錄 XVII
表目錄XX
圖目錄 XXI
第一章 緒論 1
1.1 前言 1
1.2 研究目的與動機 2
第二章 文獻回顧 5
2.1 LANBOX 材料介紹 5
2.2 記憶體介紹 6
2.2.1 揮發性記憶體 (Volatile Memory, VM) 7
2.2.2 非揮發性記憶體 (Non-volatile Memory, NVM) 8
2.3 電阻式隨機存取記憶體(RRAM)介紹16
2.3.1 雙極電阻轉換 (Bipolar Resistive Switching, BRS) 19
2.3.2 單極電阻轉換 (Unipolar Resistive Switching, URS) 19
2.4 電阻轉換特性材料20
2.4.1 二元過渡金屬氧化物 (Transition Metal Oxide,TMO) 20
2.4.2 稀土族氧化物 (Rare Earth Oxide, REO) 20
2.4.3 鈣鈦礦結構氧化物21
2.4.4 有機/高分子材料21
2.5 電阻轉換機制22
2.5.1 導電燈絲機制 (Conducting Filaments Mechanism) 22
2.5.2 介面導電機制 (Interface-type conducting path) 25
2.6 漏電流傳導機制 25
2.6.1 電極限制的傳導機制 (Electrode-limited)26
2.6.2 本體限制傳導機制 (Bulk-limited) 28
第三章 實驗步驟與方法 32
3.1 溶膠凝膠法(SOL-GEL)介紹 32
3.1.1 薄膜製備33
3.1.2 低溫乾燥熱處理34
3.1.3 高溫退火熱處理34
3.2 實驗流程35
3.2.1 使用藥品藥35
3.2.2 Sol-Gel 調配36
3.2.3 ITO 玻璃基板清洗 37
3.2.4 薄膜塗佈與乾燥37
3.2.5 薄膜退火37
3.2.6 電子束蒸鍍38
3.2.7 金屬後退火38
3.3 實驗設備 40
3.3.1 磁石加熱攪拌器40
3.3.2 旋轉塗佈機40
3.3.3 石英爐管40
3.3.4 電子束蒸鍍機41
3.4 量測與分析儀器 41
3.4.1 低掠角薄膜 X 光繞射儀 (X-ray Diffractometer ,XRD) 42
3.4.2 高解析掃描式電子顯微鏡 (High Resolution Scanning Electron Microscope, HR-SEM)43
3.4.3 多功能原子力顯微鏡 (Atomic Force Microscope, AFM) 44
3.4.4 X 光光電子能譜儀 (X-ray Photoelectron Spectroscope, XPS) 45
3.4.5 高解析穿透式電子顯微鏡 (Ultrahigh Resolution Transmission Electron Microscope, HR-TEM)46
3.4.6 半導體參數分析儀46
第四章 結果與討論 47
4.1 LANBOX 薄膜分析47
4.1.1 XRD 晶相分析47
4.1.2 SEM表面與剖面分析48
4.1.3 AFM 表面形貌分析 50
4.1.4 XPS 表面化學分析 51
4.1.5 TEM 微區結構分析 56
4.2 電性分析 58
4.2.1 LNO 薄膜厚度對 Al/LNO/ITO 電阻轉換特性之影響58
4.2.2 不同上電極(Al、Ti)對元件電阻轉換特性之影響67
4.2.3 退火溫度對Al/LNO/ITO電阻轉換特性之影響73
4.2.4 金屬後退火製程對Al/LNO/ITO電阻轉換特性之影響80
4.2.5 Al/AlOx/LNO/ITO 電阻轉換特性之影響87
4.2.6 Al/LNO/ITO 元件之導通機制模型90
4.3 比較與討論93
第五章 結論95
參考文獻 97

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