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系統識別號 U0026-0107201913111400
論文名稱(中文) 氧化銦鎵非揮發性電阻式記憶體之製作與研究
論文名稱(英文) Fabrication and Investigation of InxGa1-xO Insulator for Non-volatile RRAM
校院名稱 成功大學
系所名稱(中) 微電子工程研究所
系所名稱(英) Institute of Microelectronics
學年度 107
學期 2
出版年 108
研究生(中文) 林永哲
研究生(英文) Yong-Zhe Lin
電子信箱 anywaynomore@gmail.com
學號 Q16064024
學位類別 碩士
語文別 英文
論文頁數 127頁
口試委員 指導教授-張守進
口試委員-陳志方
口試委員-蘇炎坤
口試委員-張勝博
口試委員-薛漢鼎
中文關鍵字 非揮發性電阻式記憶體  氧化銦鎵  氧化銦  氧化鎵 
英文關鍵字 non-volatile RRAM  InxGa1-xO  In2O3  Ga2O3 
學科別分類
中文摘要 氧化銦鎵非揮發性電阻式記憶體之製作與研究


研究生:林永哲* 指導教授:張守進**
國立成功大學微電子工程研究所

摘要
本論文中,以氧化銦鎵作為非揮發性電阻式隨機存取記憶體的氧化層,主要是因為銦原子及鎵原子時常用來作為電晶體、感測器及太陽能電池的材料,且能經過銦鎵比的調變,改變其電性。
首先,我們探討在室溫下以InxGa1-xO作為電阻轉換層搭配白金、鈦和鋁作為上電極、白金作為下電極之電阻式記憶體的製備方法與其電特性。因為此三種金屬電極有不同的化學性質,因此我們以穿透式電子顯微鏡(TEM)及能量色散X射線譜(EDS)分析上電極與電阻轉換層的介面,確認此介面對於電阻式記憶體的電性影響,再分析三種上電極下,不同銦鎵比對於電阻式記憶體的電性影響。結果顯示製備完成的元件,有著雙極性的直流操作下,高低阻態轉換超過100次,並在室溫、100毫伏讀取電壓下,保持高低阻態各10000秒的穩定記憶能力。
另一部分,本論文針對上述記憶體中表現最好的Al/Ga2O3/Pt作改善,我們通過增加射頻磁控濺鍍製程時的氧分壓,達到下降電阻轉換層之氧空缺含量的目的。發現經由適當的減少氧空缺,將得到更穩定的電阻轉換特性,在雙極性的直流操作下,能夠高低阻態轉換超過2000次,並在室溫、100毫伏讀取電壓下,保持高低阻態各10000秒的穩定記憶特性。
最後我們研究以鋁為上電極、白金作為下電極,從靠近下電極往上電極分別為Ga2O3、In0.1Ga0.9O、In0.4Ga0.6O、In0.9Ga0.1O以及In2O3之五層漸變式二元氧化物電阻式記憶體,發現藉由氧化層漸變,電阻轉換將因為遷移率梯度和氧空缺濃度梯度而更輕易達成,得到更小的操作電壓以及穩定的阻值,意味著不只電極以及電阻轉換層材料,有著梯度漸變氧化層結構也是改善記憶體特性的重要方法之一。

關鍵字:非揮發性電阻式記憶體、氧化銦鎵、氧化銦、氧化鎵

作者*
指導教授**
英文摘要 Fabrication and Investigation of
InxGa1-xO Insulator for Non-volatile RRAM
Yong-Zhe Lin* Shoou-Jinn Chang**
Institute of Microelectronic &
Department of Electrical Engineering
National Cheng Kung University
Abstract
In this thesis, InxGa1-xO is used as the resistive switching layer of non-volatile random-access memory. This is because indium atoms and gallium atoms are always used as the materials of transistors, sensors and solar cells, and electrical property can be modulated by changing the ratio of indium atoms to gallium atoms.
First, Pt, Ti and Al are used as the top electrode and Pt is used as bottom electrode. We investigated the manufacturing process and electrical property of the RRAM devices. Because the three top electrodes has different chemical properties, transmission electron microscope (TEM) and energy-dispersive X-ray spectroscopy (EDS) are used to analyze the interface of the top electrode and the resistive switching layer and confirm the impact of the top electrode on the electrical properties. Moreover, we research Pt/InxGa1-xO/Pt RRAM, Ti/InxGa1-xO/Pt RRAM and Al/InxGa1-xO/Pt RRAM and investigate the impact of the In/Ga ratio on the electrical properties of the RRAM devices. As the results demonstrate, at room temperature, the fabricated devices can switch over 100 times and maintain high resistance state (HRS) and low resistance state (LRS) for 10000 seconds respectively in the bipolar switching mode with 100mV reading voltage.
Then, Al/Ga2O3/Pt RRAM is improved specially because its best performance among all the devices. The oxygen vacancies are diminished by increasing the oxygen partial pressure of RF sputtering system. As the results demonstrate, the resistive switching performance will be better if the oxygen vacancies are diminished appropriately. At room temperature, the Al/Ga2O3/Pt RRAM device can switch over 2000 times and maintain high resistance state and low resistance state for 10000 seconds respectively in the bipolar switching mode with 100mV reading voltage.
Finally, we use Al as the top electrode, Pt as the bottom electrode and from the bottom electrode to the top electrode, Ga2O3, In0.1Ga0.9O, In0.4Ga0.6O, In0.9Ga0.1O and In2O3 as the resistive switching layer to fabricate the penta-layer gradual binary oxide RRAM (Gradual RRAM). We find that the resistive switching performance is improved due to the gradient of the mobility and concentration gradient of the oxygen vacancies. It means that not only the electrode and the material of the resistive switching layer have impact on the performance of RRAM but also the structure of gradual binary oxide is one of the methods to improve the performance of RRAM.

Key words: non-volatile RRAM, InxGa1-xO, In2O3, Ga2O3

Author*
Advisors**
論文目次 Contents
Abstract (Chinses) I
Abstract (English) III
Acknowledgements V
Contents VI
Table Captions X
Figure Captions XI
Chapter 1 Introduction 1
1-1 Evolution of Memory 1
1-2 New Non-Volatile Memory 4
1-2-1 Magnetic Random-Access Memory 4
1-2-2 Phase Change Random-Access Memory 6
1-2-3 Resistive Random-Access Memory 7
1-2-3-1 Filamentary Model 10
1-2-3-2 Ion Migration 11
1-2-3-3 Impact of the Electrode Materials 11
1-2-3-4 Thermochemical Reaction 12
1-3 Motivation 15
References 16
Chapter 2 Conductive Mechanism of RRAM 20
2-1 Conductive Mechanism of Insulator 20
2-1-1 Schottky Emission 21
2-1-2 Fowler-Nordheim (F-N) and Direct Tunneling 22
2-1-3 Poole-Frenkel (P-F) Emission 22
2-1-4 Space-Charge-Limited-Conduction (SCLC) 23
2-1-5 Ionic Conduction 24
2-1-6 Ohmic Conduction 24
2-1-7 Nearest Neighbor Hopping (NNH) 25
2-1-8 Mott Variable Range Hopping (VRH) 25
2-1-9 Trap-Assisted Tunneling (TAT) 26
References 27
Chapter 3 Experimental Equipment 30
3-1 Introduction of Experimental Equipment 30
3-1-1 Radio Frequency (RF) Sputtering System 30
3-1-2 Energy-Dispersive X-ray Spectroscopy (EDS) 33
3-1-3 X-ray Photoelectron Spectroscopy (XPS) 34
3-1-4 Measurement Systems 35
References 36
Chapter 4 Experimental of InxGa1-xO based RRAM Devices 37
4-1 Role of Electrode Materials 37
4-2 Experimental Procedure 38
4-3 Analysis of Fabricated InxGa1-xO Thin Film 41
4-3-1 Structural Characteristic of Devices: TEM 41
4-3-2 Elemental Analysis 48
4-3-2-1 Elemental Analysis: EDS Analysis of In0.1Ga0.9O 48
4-3-2-2 Elemental Analysis: XPS Analysis of InxGa1-xO 56
4-4 Results and Discussion 61
4-4-1 Forming Process 61
4-4-2 Pt/InxGa1-xO/Pt RRAM 68
4-4-2-1 The IV Sweep of Pt/InxGa1-xO/Pt RRAM 68
4-4-2-2 Endurance Test of Pt/InxGa1-xO/Pt RRAM 70
4-4-2-3 Retention Test of Pt/InxGa1-xO/Pt RRAM 74
4-4-2-4 Conductive Mechanism of Pt/InxGa1-xO/Pt RRAM 76
4-4-3 Ti/InxGa1-xO/Pt RRAM 78
4-4-3-1 The IV Sweep of Ti/InxGa1-xO/Pt RRAM 78
4-4-3-2 Endurance Test of Ti/InxGa1-xO/Pt RRAM 79
4-4-3-3 Retention Test of Ti/InxGa1-xO/Pt RRAM 82
4-4-3-4 Conductive Mechanism of Ti/InxGa1-xO/Pt RRAM 84
4-4-4 Al/InxGa1-xO/Pt RRAM 86
4-4-4-1 The IV Sweep of Al/InxGa1-xO/Pt RRAM 86
4-4-4-2 Endurance Test of Al/InxGa1-xO/Pt RRAM 89
4-4-4-3 Retention Test of Al/InxGa1-xO/Pt RRAM 95
4-4-4-4 Conductive Mechanism of Al/InxGa1-xO/Pt RRAM 98
4-5 Effect of Interface of Electrode and Insulator 100
4-6 Improvement of Al/Ga2O3/Pt RRAM 104
4-6-1 Motivation 104
4-6-2 Experimental Procedure 105
4-6-3 Forming Process of Al/Ga2O3/Pt_O2 20% RRAM 106
4-6-4 IV Sweep of Al/Ga2O3/Pt_O2 20% RRAM 106
4-6-5 Endurance Test of Al/Ga2O3/Pt_O2 20% RRAM 107
4-6-6 Retention Test of Al/Ga2O3/Pt_O2 20% RRAM 109
4-6-7 Resistance Switching Mechanism 110
4-7 Gradual Binary Oxide RRAM 111
4-7-1 Motivation 111
4-7-2 Experimental Procedure 111
4-7-3 Forming Process of Gradual Binary Oxide RRAM 113
4-7-4 IV Sweep of Gradual Binary Oxide RRAM 114
4-7-5 Endurance Test of Gradual Binary Oxide RRAM 114
4-7-6 Retention Test of Gradual Binary Oxide RRAM 116
4-7-7 Resistance Switching Mechanism 117
Chapter 5 Conclusions and Future Work 119
5-1 Conclusions 119
5-2 Future work 122
5-2-1 Multi-bit RRAM 123
5-2-2 Flexible and Transparent RRAM 123
5-2-3 Boolean logic in 1T1R-RRAM 124
References 125












Table Captions
Table 4-1: The characterization of Pt/InxGa1-xO/Pt samples with different experimental processes 40
Table 4-2: The characterization of Ti/InxGa1-xO/Pt samples with different experimental processes 40
Table 4-3: The characterization of Al/InxGa1-xO/Pt samples with different experimental processes 41
Table 4-4: Ratio between indium, gallium and oxygen of Pt-B 49
Table 4-5: Ratio between indium, gallium and oxygen of Ti-B 49
Table 4-6: Ratio between indium, gallium and oxygen of Al-B 49
Table 4-7: The relative ratio of O_III⁄((O_I+O_II+O_III ) ) 59
Table 4-8: The XPS comparison of Ga2O3_O2 10%andGa2O3_O2 20%
60
Table 4-9: Forming voltage of samples of Pt TE 67
Table 4-10: Forming voltage of samples of Ti TE 67
Table 4-11: Forming voltage of samples of Al TE 67
Table 4-12: Performance of Pt/InxGa1-xO/Pt RRAM 73
Table 4-13: Performance of Ti/InxGa1-xO/Pt RRAM 82
Table 4-14: Performance of Al/InxGa1-xO/Pt RRAM 94
Table 4-15: Comparison of Sample Al-A and Al/Ga2O3/Pt_O2 20% 109
Table 4-16: Comparison of Al/Ga2O3/Pt_O2 20% and gradual RRAM
116
Table 4-17: Performance comparison of In-based and Ga-based RRAM 122
Figure Captions
Figure 1-1: The expansion of IoT year by year 2
Figure 1-2: Flow chart for the semiconductor memory classification according to their functional criteria 3
Figure 1-3: Basic MRAM cell structure 5
Figure 1-4: Basic PCRAM cell structure 7
Figure 1-5: (a) Typical I-V curve of unipolar and bipolar switching modes. (b) Sandwich structure of RRAM devices 9
Figure 1-6: Schematic of the switching mechanism of oxide RRAM 10
Figure 1-7: Experimentally extracted and calculated CF temperature as a function of applied voltage 14
Figure 1-8: Schematic representation of the reset operation. When the reset voltage Vreset is applied to the CF, the inner temperature is raised by Joule heating, and CF rupture occurs 14
Figure 3-1: The momentum exchange process 31
Figure 3-2: Schematic diagram of RF sputtering system 32
Figure 3-3: Schematic of EDS system 34
Figure 4-1: The process flow and device structure 39
Figure 4-2: Cross-section of Sample Pt-B 42
Figure 4-3: Thickness of Sample Pt-B 42
Figure 4-4: Crystal structure of Sample Pt-B 43
Figure 4-5: TEM diffraction pattern of Sample Pt-B 43
Figure 4-6: Cross-section of Sample Ti-B 44
Figure 4-7: Thickness of Sample Ti-B 44
Figure 4-8: Crystal structure of Sample Ti-B 45
Figure 4-9: TEM diffraction pattern of Sample Ti-B 45
Figure 4-10: Cross-section of Sample Al-B 46
Figure 4-11: Thickness of Sample Al-B 46
Figure 4-12: Crystal structure of Sample Al-B 47
Figure 4-13: TEM diffraction pattern of Sample Al-B 47
Figure 4-14: Sample Pt-B: The point selected of EDS analysis 50
Figure 4-15: Sample Pt-B Point 1: The element ratio of RS layer 50
Figure 4-16: Sample Pt-B Point 2: The element ratio of RS layer 51
Figure 4-17: Sample Pt-B Point 3: The element ratio of RS layer 51
Figure 4-18: Sample Ti-B: The point selected of EDS analysis 52
Figure 4-19: Sample Ti-B Point 4: The element ratio of RS layer 52
Figure 4-20: Sample Ti-B Point 5: The element ratio of RS layer 53
Figure 4-21: Sample Ti-B Point 6: The element ratio of RS layer 53
Figure 4-22: Sample Al-B: The point selected of EDS analysis 54
Figure 4-23: Sample Al-B Point 7: The element ratio of RS layer 54
Figure 4-24: Sample Al-B Point 8: The element ratio of RS layer 55
Figure 4-25: Sample Al-B Point 8: The element ratio of RS layer 55
Figure 4-26: XPS O1s spectra of Ga2O3 thin film 56
Figure 4-27: XPS O1s spectra of In0.1Ga0.9O thin film 57
Figure 4-28: XPS O1s spectra of In0.4Ga0.6O thin film 57
Figure 4-29: XPS O1s spectra of In0.9Ga0.1O thin film 58
Figure 4-30: XPS O1s spectra of In2O3 thin film 58
Figure 4-31: XPS O1s spectra of Ga2O3_O2 20% thin film 60
Figure 4-32: Forming process of Sample Pt-A 62
Figure 4-33: Forming process of Sample Pt-B 62
Figure 4-34: Forming process of Sample Pt-C 63
Figure 4-35: Forming process of Sample Ti-B 63
Figure 4-36: Forming process of Sample Ti-C 64
Figure 4-37: Forming process of Sample Al-A 64
Figure 4-38: Forming process of Sample Al-B 65
Figure 4-39: Forming process of Sample Al-C 65
Figure 4-40: Forming process of Sample Al-D 66
Figure 4-41: Forming process of Sample Al-E 66
Figure 4-42: IV sweep of Sample Pt-A 68
Figure 4-43: IV sweep of Sample Pt-B 69
Figure 4-44: IV sweep of Sample Pt-C 69
Figure 4-45: Sample Pt-A: Vset and Vreset over cycles 70
Figure 4-46: Sample Pt-B: Vset and Vreset over cycles 71
Figure 4-47: Sample Pt-C: Vset and Vreset over cycles 71
Figure 4-48: Sample Pt-A: LRS and HRS over cycles 72
Figure 4-49: Sample Pt-B: LRS and HRS over cycles 72
Figure 4-50: Sample Pt-C: LRS and HRS over cycles 73
Figure 4-51: Sample Pt-A: Retention test 74
Figure 4-52: Sample Pt-B: Retention test 75
Figure 4-53: Sample Pt-C: Retention test 75
Figure 4-54: Conduction mechanism of Sample Pt-C 77
Figure 4-55: The band diagram of Sample Pt-C 77
Figure 4-56: IV sweep of Sample Ti-B 78
Figure 4-57: IV sweep of Sample Ti-C 79
Figure 4-58: Sample Ti-B: Vset and Vreset over cycles 80
Figure 4-59: Sample Ti-C: Vset and Vreset over cycles 80
Figure 4-60: Sample Ti-B: LRS and HRS over cycles 81
Figure 4-61: Sample Ti-C: LRS and HRS over cycles 81
Figure 4-62: Sample Ti-B: Retention test 83
Figure 4-63: Sample Ti-C: Retention test 83
Figure 4-64: Conduction mechanism of Sample Ti-C 85
Figure 4-65: The band diagram of Sample Ti-C 85
Figure 4-66: IV sweep of Sample Al-A 86
Figure 4-67: IV sweep of Sample Al-B 87
Figure 4-68: IV sweep of Sample Al-C 87
Figure 4-69: IV sweep of Sample Al-D 88
Figure 4-70: IV sweep of Sample Al-E 88
Figure 4-71: Sample Al-A: Vset and Vreset over cycles 89
Figure 4-72: Sample Al-B: Vset and Vreset over cycles 90
Figure 4-73: Sample Al-C: Vset and Vreset over cycles 90
Figure 4-74: Sample Al-D: Vset and Vreset over cycles 91
Figure 4-75: Sample Al-E: Vset and Vreset over cycles 91
Figure 4-76: Sample Al-A: LRS and HRS over cycles 92
Figure 4-77: Sample Al-B: LRS and HRS over cycles 92
Figure 4-78: Sample Al-C: LRS and HRS over cycles 93
Figure 4-79: Sample Al-D: LRS and HRS over cycles 93
Figure 4-80: Sample Al-E: LRS and HRS over cycles 94
Figure 4-81: Sample Al-A: Retention test 95
Figure 4-82: Sample Al-B: Retention test 96
Figure 4-83: Sample Al-C: Retention test 96
Figure 4-84: Sample Al-D: Retention test 97
Figure 4-85: Sample Al-E: Retention test 97
Figure 4-86: Conduction mechanism of Sample Al-A 99
Figure 4-87: The band diagram of Sample Al-A 99
Figure 4-88: The filamentary model of Pt/InxGa1-xO/Pt RRAM 100
Figure 4-89: The filamentary model of Ti/InxGa1-xO/Pt RRAM 101
Figure 4-90: The filamentary model of Al/InxGa1-xO/Pt RRAM 102
Figure 4-91: The filamentary path model of Al/InxGa1-xO/Pt RRAM 103
Figure 4-92: Impact of In/Ga ratio 103
Figure 4-93: Forming process of Al/Ga2O3/Pt_O2 20% RRAM 106
Figure 4-94: IV sweep of Al/Ga2O3/Pt_O2 20% RRAM 107
Figure 4-95: Al/Ga2O3/Pt_O2 20%: Vset and Vreset over cycles 108
Figure 4-96: Al/Ga2O3/Pt_O2 20%: LRS and HRS over cycles 108
Figure 4-97: Al/Ga2O3/Pt_O2 20%: Retention test 109
Figure 4-98: The redox resistance switching mechanism of Al/Ga2O3/Pt_O2 20% RRAM 110
Figure 4-99: Structure of gradual binary oxide RRAM 112
Figure 4-100: Forming process of gradual binary oxide RRAM 113
Figure 4-101: IV sweep of gradual binary oxide RRAM 114
Figure 4-102: Gradual RRAM: Vset and Vreset over cycles 115
Figure 4-103: Gradual RRAM: LRS and HRS over cycles 115
Figure 4-104: Gradual binary oxide RRAM: Retention test 116
Figure 4-105: The set process of gradual RRAM 118
Figure 4-106: The reset process of gradual RRAM 118
參考文獻 Chapter 1 Introduction
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Chapter 2 Conductive Mechanism of RRAM
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Chapter 3 Experimental Equipment
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Chapter 5 Conclusions and Future Work
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