電阻式記憶體為目前最具發展潛力的非揮發性記憶元件，其擁有極低的操作電壓、極短的寫入抹除時間及高度的元件可微縮性。因此深受學術界及各國際大廠的重視，並紛紛投入研究及開發，期望能儘速將電阻式記憶體元件商業化。本研究將以物理機制的釐清、發展具潛力的材料與結構、及穩定以穩定電阻式記憶體之操作特性為主要目標，特別是物理機制的釐清，將是電阻式記憶體能否商品化之關鍵因素。
對於filament導通為基礎的電阻式記憶體而言，目前研究指出不穩定導通路徑的filament造成電阻切換變異，而轉換層的氧元素的散逸可能會造成耐操度、阻值差異。所以在我們的研究中提出新材料(矽引入)及新結構(氧侷限層)的方式來達到抑制上述兩者的缺點，進而增進電阻式記憶體元件之阻態切換的穩定性、耐操度，元件間的均勻性。此外於切換能量為定值的實驗中有於篩選最佳的材料及結構，並經確的控制電阻式記憶體的操作條件。
物理機制的釐清方面，使用工研院提供穩定的HfO2電阻式記憶體元件，進行更深入的物理機制研究。電阻切換過程被證明是filament的形成及斷裂造成的。此外電阻式記憶體的切換速度極快，我們認為這是由於轉態反應是由數顆原子的切換主導。然而在如此微小的微度下，難以藉由材料即時動態解析此只涉及數顆原子的反應。我們由不同的電特性分析觀察電阻式記憶體數十顆原子的動態切換行為，更進一步分析求得此傳導途經的電阻率，證明此傳導途經是由金屬質的細絲所組成。並且同時證明電阻式記憶體在極低溫環境下(4K)的切換動作是由於金屬質細絲中逐顆(Atom by Atom)反應所形成的量化現象。

Resistive Random Access Memory (RRAM) is considered as the most promising candidate for the next-generation nonvolatile memories due to their superior properties such as low operation voltage, fast operation speed, non-destructive read, simple metal-insulator-metal (MIM) sandwich structure, good scale-down ability. The main targets of this research are to clarify the corresponding physical mechanism, develop the potential material and structure of RRAM and stabilize the resistive switching characteristics, in which clarifying the physical mechanism will be the key factor for RRAM into production in the future.
Recent research has suggested that variation of the low and high resistance states in RRAM could be caused due to the by instability in the formation and /disruption of the filament. In addition, the endurance and stability of RRAM may be related to the dissipation of oxygen ions in the switching layer. In this study, new material (Si Introduced) and structure (oxygen confined layer) are employed to improve RRAM performance and to clarify the physical mechanism. Furthermore, constant switching energy results can be used to select the optimal materials and structures also can be used to correctly allocate voltage and time to control RRAM.
The detail physical mechanism is studied by the stable RRAM device (Ti/HfO2/TiN) which is offered from Industrial Technology Research Institute (ITRI). The switching process is proved as the formation/disruption of the filament. Furthermore, the dynamic switching behaviors during reset procedure in RRAM were analyzed by the sequential experimental design to illustrate the procedure of atomic quantized reaction at the ultra-cryogenic temperature.

Contents
Abstract (Chinese).………………………...…………I
Abstract (English) …………………………....………II
Acknowledgement………………………………...…III
Contents……………………..………………………..IV
Figure Captions……...................................................VIII
Table Captions……....................................................VIII
Chapter1 Background
1-1. The Evolution of Memory 1
1-2. The Advanced Memory 2
1-2-1. MRAM (Magnetic RAM) 2
1-2-2. FeRAM (Ferroelectric RAM) 3
1-2-3. PCRAM (Phase Change RAM) 4
1-2-4. RRAM (Resistance RAM) 5
1-3. Motivation 5
Chapter2 Basic Introduction of RRAM
2-1. Introduction of RRAM 11
2-2. The Materials of RRAM 12
2-2-1. Perovskite Oxides 12
2-2-2. Organic Materials 13
2-2-3. Transition Metal Oxides 13
2-3. The Switching Mechanism of RRAM 15
2-3-1. Charge Trap in Small Domain 15
2-3-2. Filamentary Model 16
2-3-2-1. Joule Heating Effect 16
2-3-2-2. Redox Reaction with Cation Migration 17
2-3-2-3. Redox Reaction with Anion Migration 18
2-3-3. Modified Schottky Barrier Model 19
2-4. Conducting Mechanisms in Oxides 20
2-4-1. Ohmic Conduction 21
2-4-2. Schottky Emission 21
2-4-3. Poole-Frenkel Emission 22
V
2-4-4. Tunneling Conduction 22
2-4-5. Space Charge Limited Current 23
2-4-6. Hopping Conduction 23
Chapter3 Silicon Introduced Effect on Resistive Switching Properties of
WOX Thin Films
3-1. Introduction 35
3-2. Experiment 36
3-3. Discussion and Results 36
3-4. Conclusion 39
Chapter4 Asymmetric Carrier Conduction Mechanism by Tip Electric
Field in WSiOX Resistance Switching Device
4-1. Introduction 47
4-2. Experiment 48
4-3. Discussion and Results 48
4-4. Conclusion 51
Chapter5 Ultra-high Endurance Technology with Oxygen-confined
-layer Inserted in WSiOX Resistance Switching Device
5-1. Introduction 58
5-2. Experiment 59
5-3. Discussion and Results 59
5-4. Conclusion 61
Chapter6 Improving Resistance Switching Characteristics with SiGeOX
/SiGeON Double Layer for Nonvolatile Memory Applications
6-1. Introduction 69
6-2. Experiment 70
6-3. Discussion and Results 70
6-4. Conclusion 73
Chapter7 Redox Reaction Switching Mechanism in RRAM Device with
Pt/CoSiOX/TiN Structure
7-1. Introduction 81
7-2. Experiment 81
VI
7-3. Discussion and Results 82
7-4. Conclusion 85
Chapter8 Resistance Switching Mechanism of HfO2 RRAM
8-1. Introduction 91
8-2. Experiment 92
8-3. Discussion and Results 92
8-4. Conclusion 97
Chapter9 Atomic-Level Quantized Reaction of RRAM
9-1. Introduction 105
9-2. Experiment 106
9-3. Discussion and Results 107
9-4. Conclusion 109
Chapter10 Conclusion 114

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