近年來由於記憶體的大量使用，因此必須微縮記憶體面積提高密度。因為電阻式記憶體(RRAM)有高密度與低功耗的特性，故有潛力成為下一世代非揮發性記憶體。最近SiO2摻雜石墨被發現亦具RRAM特性，而其電阻之記憶特性相較一般金屬氧化物具有奇異之氧化石墨烯切換機制。故本論文研究利用非晶碳做為RRAM的電阻切換材料，探討碳基(carbon based) RRAM反應機制與元件特性。

本論文所使用的非晶碳薄膜製作有濺鍍法與電漿輔助化學沉積法。元件的結構為在TiN下電極沉積非晶碳層再覆蓋Pt上電極。透過薄膜的材料特性與電性量測分析，發現濺鍍碳RRAM的電阻切換機制是以氫離子與碳-碳雙鍵反應造成阻絲的高低阻態(HRS與LRS)。元件在施予一大偏壓形成軟崩潰後(forming)，於濺鍍碳層形成sp2碳為主的阻絲。在負偏壓下氫離子受到電場吸引並與碳-碳共軛雙鍵反應，將導通sp2結構轉換成絕緣的sp3結構之HRS。反之正偏壓下sp3結構中的氫離子受到電場排斥到Pt電極，而碳-碳之間再度形成sp2碳之LRS。此外CVD鍍膜DLC之RRAM實驗結果發現也具有與濺鍍碳相同的RRAM電子傳導機制，故非晶碳薄膜的電阻切換機制主要是由氫離子與碳-碳鍵反應所造成。

此外，不同HfO2與DLC堆疊主動層：DLC-T RRAM (DLC/HfO2) 與DLC-B RRAM (HfO2/DLC)用來研究Pt電極與TiN電極對於非晶碳的電阻切換機制所造成的影響。根據電性分析結果，DLC-T RRAM的電子傳導機制與DLC RRAM類似，顯示非晶碳薄膜的切換是發生在Pt電極端，符合所提出的氫離子造成的電阻切換模型。然而DLC-B RRAM的電子傳導機制與氧化石墨烯相同，係因元件經過forming後，HfO2層的氧離子受電場吸引並移動到TiN端，並與DLC層中sp2碳進行反應，改變電子跳躍所經碳-碳共軛雙鍵之鍵長，造成阻態切換。

The increasing demand for flash memory densities by scaling dimension is a formidable challenge due to physical limitations. Recently, carbon-based resistive random access memory (RRAM) exhibits to be a promising candidate for high density and low power consumption. In this study, the resistive switching property of amorphous carbon material was investigated for RRAM application.

In this study, the amorphous carbon films were prepared by RF megetron sputtering and PECVD methods. The RRAM devices were constructed by an amorphous carbon layer between Pt top and TiN bottom electrodes. A bias was applied to the bottom electrode (TiN), and the top electrode (Pt) was grounded during the electrical measurement. Based on material characterization and electrical analysis, it is found that the switching of high and low resistive state (HRS and LRS) of sputtered carbon RRAM is attributed to hydrogenation and dehydrogenation reactions of C-C double bonds and hydrogen ions. After an electroformation, a sp2 carbon dominated filament was formed in the carbon layer. Appling a negative bias, hydrogen ions are attracted by electrical field and reacted with C-C conjugated double bonds, leading the transformation of conductive sp2 structure in to insulated sp3 structure. In contrast, hydrogen atoms in the sp3 structure are repelled into Pt electrode by a positive bias, which results the transformation of sp2 carbon. In addition, the experiment result of DLC RRAM also shows the same electron transport mechanism to the sputtered RRAM. Therefore, the resistance switching (RS) mechanism of amorphous carbon is concluded to hydrogen reacting with C-C double bonds.
 
Furthermore, the influences of Pt electrode and TiN electrode on the RS mechanism of amorphous carbon RRAM were investigated by two devices with HfO2 and DLC stacking, DLC-T RRAM (Pt/DLC/HfO2/TiN) and DLC-B RRAM (Pt/HfO2/DLC/TiN). By contrast, RS mechanism of DLC-T RRAM is similar to DLC RRAM. It demonstrates that the RS occurs in DLC layer near Pt electrode, which is consistent with the hydrogen induced RS model. Further, DLC-B RRAM is consistent to the RS model of graphine-oxide RRAM, that after a forming process, oxygen atoms in HfO2 are attracted by the positive electrical filed and then move to TiN electrode, in which oxygen ions absorb and eliminate with sp2 carbon (C-C conjugated double bonds), resulting to the RS in DLC-B RRAM.

致謝 iii
摘要 iv
Abstract v
目錄 vii
圖目錄 x
表目錄 xiii
物理常數 xiii
符號表 xiv
縮寫表 xv
1. 序論 1
1.1. 前言 1
1.2. 研究動機 2
1.3. 文獻回顧 3
1.3.1. 鐵電式記憶體 3
1.3.2. 相變化記憶體 4
1.3.3. 磁阻式記憶體 5
1.3.4. 電阻式記憶體 6
2. 基本原理 7
2.1. 電阻式記憶體切換機制 7
2.2. 絕緣體載子傳導機制 9
2.2.1. 穿隧 9
2.2.2. 熱離子發射 11
2.2.3. 普爾-法蘭克發射 12
2.2.4. 歐姆傳導 13
2.2.5. 離子電導 14
2.2.6. 空間電荷限制電流 14
2.2.7. 跳躍傳導 15
3. 試片製作與分析 16
3.1. 製作過程 16
3.1.1. 薄膜沉積 16
3.1.2. 元件製作流程 18
3.2. 薄膜特性分析設備 20
3.2.1. N&K薄膜特性分析儀 20
3.2.2. 傅立葉轉換紅外光譜儀(FTIR) 20
3.2.3. 拉曼光譜(Raman) 23
3.2.4. X光光電子能譜儀(XPS) 25
3.3. 電性量測系統 27
4. 實驗I-非晶濺鍍碳電阻切換 28
4.1. 薄膜成份分析 28
4.1.1. XPS分析 28
4.1.2. Raman分析 29
4.1.3. FTIR分析 30
4.2. 濺鍍碳RRAM電性分析 32
4.2.1. Forming過程 32
4.2.2. RRAM切換特性量測 33
4.2.3. 不同面積的元件尺寸效應 35
4.2.4. 記憶窗之持久性 36
4.2.5. 元件耐受度 37
4.3. 濺鍍碳RRAM電流傳導機制擬合 38
4.4. 濺鍍碳RRAM電阻切換機制模型 40
5. 實驗II-DLC RRAM電阻切換 44
5.1. DLC薄膜成份分析 44
5.2. DLC薄膜電性量測與分析 47
5.3. DLC RRAM電流傳導機制擬合 51
5.4. DLC RRAM與濺鍍碳 RRAM特性比較 52
6. 實驗III-HfO2與DLC堆疊元件電阻切換 53
6.1. DLC-T RRAM之電性量測 53
6.2. DLC-B RRAM之電性量測 54
6.3. DLC RRAM與HfO2/DLC堆疊RRAMs傳導特性比較 55
6.4. 雙層RRAM的電阻切換機制模型 57
7. 結論 61
參考文獻 63
附錄A Fitting之I vs. V曲線 74
附錄B 電子傳導能障計算 80
簡歷 81
著作清單 82

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