臺灣博碩士論文加值系統

本研究以積體電路相匹配之Al、TaN作為上、下電極，以取代昂貴之白金(Pt)作為電極，並採用微波電漿氧化或反應式濺鍍製備中間電阻層TaOxNy，製成Al/TaOxNy/TaN、TaN/TaOxNy/Al之MIM結構之電阻式記憶體，比較兩種元件之電性掃描特性，且探討Al與TaOxNy界面處之界面氧化層AlOz對元件之影響。
當以微波電漿氧化或以反應式濺鍍製備中間層TaOxNy，並製作成Al/TaOxNy/TaN元件時，於循環掃描時高低電阻切換較不穩定，且不能長時間地作高低電阻切換，而高低電阻值會隨掃描時間增加而增加之趨勢，並直到元件產生永久絕緣現象而損壞。當以反應式濺鍍製備中間層TaOxNy，並製作成TaN/TaOxNy/Al元件時，元件於循環掃描時高低電阻切換穩定，且可循環操作高達1000次，而高低電阻值比值約2.5倍。
在TaN/TaOxNy/Al元件之導電機制方面，高電阻態之電性分析結果認為在低電壓時為Ohmic conduction，高電壓時為Poole-Frenkel emission；低電阻態則為Ohmic conduction。在電極面積效應方面，TaN/TaOxNy/Al元件之HRS電阻值會隨著面積增大而有下降之趨勢，LRS電阻值則維持不變，推測元件之導電方式是以導電燈絲作為主要導電機制。而於升溫電性量測分析，TaN/TaOxNy/Al元件之電阻值會隨著溫度上升而下降，可得知其導電燈絲為氧空缺燈絲作為主要載子傳遞路徑。

In this study, we demonstrate the effect of interfacial aluminum oxide (AlOz) layer near the Al-TaOxNy interface and compare reversible switching behaviors of the Al/TaOxNy/TaN and TaN/TaOxNy/Al resistance random access memory (RRAM) devices. The TaN and Al films which are compatible with the integrated circuits technology were prepared by sputter deposition as the electrode layers to replace expensive Pt electrode, and the tantalum oxynitride (TaOxNy) film was prepared by reactive sputtering or microwave plasma oxidation of the TaN films as the insulating layer.
The resistance swiching operation was unstable for the Al/TaOxNy/TaN devices whose TaOxNy films were prepared by reactive sputtering or microwave plasma oxidation, and the resistance of HRS and LRS increased with increased resistance switching cycles. In comparison, the switching behavior of TaN/TaOxNy/Al device whose TaOxNy film was prepared by reactive sputtering exhibited good stability. The resistance ratio of RHRS/RLRS measured at -0.2 V of the TaN/TaOxNy/Al device was about 2.5, and the numbers of resistance switching could be up to 1000 cycles at room temperature.
On the mechanism analysis of TaN/TaOxNy/Al device, HRS were the Ohmic conduction at the low operation voltages and the Poole-Frenkel emission at high operation voltages, respectively, and LRS was the Ohmic conduction. To elucidate the conduction mechanism, we carried out electrical measurements of the RRAM with different cell areas and at various temperatures. The TaN/TaOxNy/Al device in LRS had constant resistance with increased cell’s area and decreased resistance with increased temperature. It suggests that the electron transport is probably attributed to oxygen vacancies in conduction filaments.

摘要 I
Abstract II
致謝 III
目錄 V
圖目錄 X
表目錄 XVII
第1章 前言 1
1.1 介紹 1
1.2 研究動機 2
第2章 文獻回顧 3
2.1 記憶體簡介 3
2.1.1 鐵電式記憶體(Ferroelectric Random Access Memory, FeRAM) 2
2.1.2 磁阻式記憶體(Magnetoresistive Random Access Memory, MRAM) 2
2.1.3 相變化式記憶體(Phase-Change Random Access Memory, PRAM) 2
2.1.4 電阻式記憶體(Resistive Random Access Memory, RRAM) 3
2.1.4a 單極性電阻切換 6
2.1.4b 雙極性電阻切換 6
2.2 電阻式記憶體之電阻切換機構 7
2.2.1 導電燈絲機構(Filamentary conducting path) 7
2.2.2 離子遷徙機構(Ionic migration) 10
2.2.3 界面型導電機構(Interface-type conducting path) 11
2.3 漏電流導電機制 13
2.3.1 蕭特基發射(Schottky emission) 13
2.3.2 歐姆接觸(Ohmic contact) 15
2.3.3 傅勒-諾德翰穿隧(Fowler-Nordheim tunneling, FNT) 15
2.3.4 空間電荷限制傳導(Space-charge-limited conduction) 16
2.3.5 普爾-法蘭克發射(Poole-Frenkel emission) 19
2.4 TaON、TaOx及Ta2O5之電阻切換相關研究 21
2.4.1 TaON作為電阻層之研究 21
2.4.2 TaOx作為電阻層之研究 23
2.4.3 Ta2O5作為固態電解質型電阻層之研究 28
2.4.4 Ta2O5-x-TaO2-x作為電阻層之研究 30
2.5 電極與絕緣層之間界面氧化物膜層對電阻切換之影響 32
2.6 AlxOy、Al2O3作為電阻層之研究 38
第3章 實驗方法與步驟 41
3.1 電阻式記憶體元件之製備 41
3.1.1 實驗耗材與藥品規格 41
3.1.2 實驗流程 42
3.1.3 基材簡介及清洗製程 43
3.1.4 元件製備 44
3.2 實驗儀器與裝置 47
3.2.1 實驗儀器簡表 47
3.2.2 磁控式濺鍍系統 (Magnetic Sputtering) 47
3.2.3 微波電漿氧化系統 (Microwave Plasma Oxidation) 49
3.3 材料分析與鑑定之儀器 50
3.3.1 材料分析儀器簡表 50
3.3.2 表面輪廓儀 (Surface Profiler, α-step) 51
3.3.3 X-ray繞射分析儀(X-ray Diffractometer, XRD) 51
3.3.4 場發射掃描式電子顯微鏡(Field Emission Scanning Electron Microscopy, FESEM) 52
3.3.5 高解析度場發射穿透式電子顯微鏡(Field Emission Transmission Electron Microscopy, FETEM) 53
3.3.6 場發射雙束型聚焦離子束顯微鏡(Dual Beam FIB) 54
3.3.7 X射線光電子能譜儀(X-ray Photoelectron Spectrum, XPS) 54
3.3.8 半導體電性量測儀 56
第4章 結果與討論 58
4.1 以微波電漿氧化製備中間電阻層之Al/TaOxNy/TaN MIM元件之材料特性分析 58
4.1.1 電極之電阻係數及XRD分析 58
4.1.2 界面電阻層之成分分析 62
4.1.3 薄膜微觀結構分析 71
4.2 以微波電漿氧化製備中間電阻層之Al/TaOxNy/TaN MIM元件之電性量測與分析 76
4.2.1 交叉隔條電極組成之元件之I-V分析 76
4.2.2 點狀電極組成之元件之I-V分析 79
4.2.3 電阻切換機構分析 81
4.3 以反應式濺鍍製備TaOxNy中間電阻層之MIM元件之材料特性分析 84
4.3.1 電極與中間電阻層TaOxNy之電阻係數及XRD分析 84
4.3.2 Al/TaOxNy/TaN 87
4.3.2a 界面電阻層之成分分析 87
4.3.2b 薄膜微觀結構分析 96
4.3.3 TaN/TaOxNy/Al 101
4.3.3a 界面電阻層之成分分析 101
4.3.3b 薄膜微觀結構分析 110
4.4 以反應式濺鍍製備TaOxNy中間電阻層之MIM元件之電性量測與分析 113
4.4.1 點狀電極組成之元件 113
4.4.1a Al/TaOxNy/TaN 113
4.4.1b TaN/TaOxNy/Al 115
4.4.2 電阻切換機構分析 123
4.4.2a Al/TaOxNy/TaN 123
4.4.2b TaN/TaOxNy/Al 126
4.4.3 Al/TaOxNy/TaN與TaN/TaOxNy/Al元件之比較 129
第5章 結論與未來展望 131
5.1 結論 131
5.2 未來展望 132
參考文獻 133
附錄 143
JCPDS cards-TaN (fcc) 143
JCPDS cards-TaN (hcp) 144
JCPDS cards-Ta2N 145
JCPDS cards-TaON 146
JCPDS cards-Ta 147
JCPDS cards-Al 148
JCPDS cards-Al2O3 149
JCPDS cards-Si 150
JCPDS cards-SiO2 151
Spectrum of XPS-C 152
Spectrum of XPS-N 153
Spectrum of XPS-O 154
Spectrum of XPS-Al 155
Spectrum of XPS-Ta 156
以微波電漿氧化製備中間電阻層之Al/TaOxNy/TaN元件之XPS分析-蝕刻時間570~660 s之Al 2p之XPS圖譜 157
以反應式濺鍍製備TaOxNy中間電阻層之Al/TaOxNy/TaN元件之XPS分析-蝕刻時間186~222 s之Al 2p之XPS圖譜 158

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