臺灣博碩士論文加值系統

本論文主要目的在研究以有機化合物聚苯乙烯( polystyrene, PS )摻雜不同材料奈米顆粒與氧化鋅奈米柱複合物為主動層的金屬/絕緣層/氧化鋅奈米柱/金屬結構之電阻式記憶體電流電壓行為與電阻切換特性。我們發現使用聚苯乙烯(PS)與一定百分比的聚(N-乙基-2-乙烯基咔唑)(P2VK)混合物，可以改善元件穩定度，當P2VK摻入比例為4%能有效提高元件的穩定度，增加良率。加入不同材料奈米顆粒可以增強薄膜鍵結強度，改善漏電流，降低操作電流，添加二氧化鈦奈米顆粒可以獲得較好的電阻切換特性。
實驗結果顯示，異質材料接面元件呈現正負偏壓電流水平不同的二極體電流電壓特性；添加不同材料奈米顆粒會影響電流水平大小。所有元件的電流電壓曲線都呈現遲滯行為，其中又以添加二氧化鈦奈米顆粒遲滯現象最明顯。實驗中我們另外發現元件在正偏壓的遲滯方向原為逆(順)時針方向，經過長時間的放置後遲滯方向會變為順(逆)時針方向。經由1000秒的資料保持測試，元件基本上都具有記憶特性，其中以添加二氧化鈦奈米顆粒時表現最佳的記憶行為，此與元件的遲滯特性一致。
我們以能帶圖分析異質接面元件，發現在聚苯乙烯(PS)與氧化鋅奈米柱介面存在電洞井，其內建能障為 0.8 eV，而電子的能障達 2.5 eV，推測電洞主宰電流傳導機制。當假設偏壓所造成的電洞能量障礙改變主要發生在聚苯乙烯(PS)側，我們可以解釋元件所呈現的二極體電流電壓特性。由於聚苯乙烯(PS)與氧化鋅奈米柱介面存在電洞井，加上聚苯乙烯(PS)與氧化鋅奈米柱超高介面面積，我們相信元件的遲滯行為來自這些電洞在介面附近的捕捉與釋放。添加奈米顆粒(TiO2)可能增加陷阱捕捉中心，增加電洞的捕捉與釋放機會，因此產生較大的遲滯行為，此與元件的記憶特性一致。

關鍵字: 電阻式記憶體，聚苯乙烯，聚(N-乙基-2-乙烯基咔唑)，奈米顆粒，奈米柱。

The aim of this thesis is to study the effects of adding different nanoparticles (NPs) and ZnO nanorods (NRs) on the current-voltage (IV) and switching characteristics of metal/insulator/ZnO NRs/metal RRAM device using a polystyrene (PS) and poly (N- ethyl-2-vinyl carbazole) (P2VK) mixture as active layer. We found that a mixture of PS and 4 weight percent of P2VK could improve the stability of the device as well as increase the device yield. Adding different materials of NPs could effectively enhance the bond strength of the film and reduce the leakage as well as the operating currents. Device with the TiO2 NPs showed better switching characteristics.
Experimental results showed that all the hetrojunction structures of metal/insulator/ZnO NRs/metal devices exhibited the diode IV characteristics with different current levels in positive and negative biases. Adding different materials of NPs affected the magnitude of current levels in the positive bias region. Hysteresis was observed nearly for all the IV curves. It was found that IV curves of PS/ P2VK composite mixed with TiO2 NPs exhibited the largest hysteresis. We also found that the initially counterclockwise (clockwise) hysteresis loops of the IV curves might become clockwise (counterclockwise) after a long time placement. After a 1000 sec data retention test, the PS/ P2VK composite mixed with TiO2 NPs showed the best data retention performance, which was consistent with the hysteresis behavior of the IV curves.
Analysis of the hytrojuction energy band diagram for the metal/insulator/ZnO NRs/metal structure showed an energy well of hole in the PS/ZnO interface. The barrier height of the hole well is about 0.8 eV. However, the potential barrier of the conduction electron is about 2.5 eV. It was believed that the holes dominated the current conduction mechanism. We reasonably assumed that the change of barrier height caused by biasing was mainly in PS side, then the diode IV behavior could well explained. Because the presence of hole potential well, it was believed that the accumulated holes capture and release near the PS/ZnO NRs interface with ultra-large surface area caused the hysteresis of the IV curves. Adding NPs (TiO2) might increase the trapping centers and possibility of holes capture and release near the PS/ZnO NRs interface region, resulting in a larger hysteresis. It was consistent with a larger hysteresis was observed in adding the TiO2 NPs. We suggested that the memory characteristics of the devices attributed to the holes capture and release near the PS/ZnO NRs interface region


Key words: RRAM, polystyrene, poly (N- ethyl-2-vinyl carbazole), nanoparticles, nanorods.

目次
摘要 I
Abstract III
目次 V
圖目次 VII
第一章 緒論 1
1-1 前言 1
1-2 研究動機 2
第二章文獻回顧 3
2-1-1 聚苯乙烯( polystyrene, PS ) 3
2-1-2 氧化鋅(Zinc Oxide，ZnO) 3
2-2-1 電阻切換現象 4
2-2-2 燈絲理論 6
2-2-3 莫特變換 7
2-2-4 蕭特基接面電阻 8
2-2-5 元件反應機制 9
2-3材料能階圖 10
第三章實驗方法 11
3-1-1 使用藥品及機台 11
3-2-1 基板清洗 12
3-2-2 底電極 12
3-2-3 ZnO晶種層 12
3-2-4 ZnO奈米柱成長 12
3-2-5 主動層製備 12
3-2-6 頂電極 12
3-2-7 4156B電性量測 13
第四章結果與討論 18
4-1-1 Ti/聚苯乙烯( polystyrene, PS )/Ti 的電流電壓特性 18
4-1-2聚苯乙烯添加不同奈米顆粒的電流電壓特性 20
4-2-1聚苯乙烯添加不同比例(N-乙基-2-乙烯基咔唑) 的電流電壓特性 24
4-2-2聚苯乙烯P2VK薄膜添加不同奈米顆粒的電流電壓特性 27
4-2-3聚苯乙烯/P2VK薄膜添加氧化鋅奈米柱結構與奈米顆粒的電流電壓特性 36
4-2-4聚苯乙烯/P2VK薄膜添加氧化鋅奈米柱結構與奈米顆粒的記憶特性 43
4-2-5改變奈米柱結構成長條件添加奈米顆粒的電流電壓特性 52
4-2-6改變奈米柱結構成長條件添加奈米顆粒的遲滯特性探討 65
4-3-1元件能階圖(平衡態) 72
4-3-2元件能階圖(偏壓) 73
第五章結論 75
參考文獻 76

圖目次
圖2-1 氧化鋅結構圖 3
圖2-2 單極性電阻切換( unipolar )IV圖 5
圖2-3 雙極性電阻切換( bipolar )IV圖[13] 5
圖2-4 無極性電阻切換IV( nonpolar )圖[14] 5
圖2-5 燈絲理論示意圖 6
圖2-6 莫特變換理論示意圖 7
圖2-7 由 D. J. Seong 等人提出之蕭特基接面電阻轉換模型 8
圖2-8 (a)trap tunneling, (b)NDR I-V current, (c)trap-free 9
圖2-9材料能階圖 10
圖3-1聚苯乙烯元件加入不同奈米顆粒實驗流程圖 14
圖3-2聚苯乙烯元件加入不同奈米顆粒實驗示意圖 15
圖3-3聚苯乙烯元件加入不同奈米顆粒與ZnO奈米柱實驗流程圖 16
圖3-4聚苯乙烯元件加入不同奈米顆粒與ZnO奈米柱實驗示意圖 17
圖4-1 Ti/PS/Ti 電流電壓特性，限流: 100mA 19
圖4-2 Ti/PS/Ti 電流電壓特性，限流: 10mA 19
圖4-3 Ti/(TiO2)PS/Ti 電流電壓特性，限流:100mA 21
圖4-4 Ti/(TiO2)PS/Ti 電流電壓特性，限流:10mA 21
圖4-5 Ti/(Al2O3)PS/Ti 電流電壓特性，限流:100mA 22
圖4-6 Ti/(Al2O3)PS/Ti 電流電壓特性，限流:10mA 22
圖4-7 Ti/( SiO2)PS/Ti 電流電壓特性，限流:100mA 23
圖4-8 Ti/( SiO2)PS/Ti 電流電壓特性，限流:10mA 23
圖4-9 Ti/PS+P2VK(1%)/Ti 電流電壓特性，限流:100mA 25
圖4-10 Ti/PS+P2VK(1%)/Ti 電流電壓特性，限流:10mA 25
圖4-11 Ti/PS+P2VK(4%)/Ti 電流電壓特性，限流:100mA 26
圖4-12 Ti/PS+P2VK(4%)/Ti 電流電壓特性，限流:10mA 26
圖4-13 Ti/(TiO2)PS+P2VK(4%)/Ti 電流電壓特性，限流:100mA 28
圖4-14 Ti/(TiO2)PS+P2VK(4%)/Ti 電流電壓特性，限流:10mA Forming圖 28
圖4-15 Ti/(TiO2)PS+P2VK(4%)/Ti 電流電壓特性，限流:10mA 第一次循環 29
圖4-16 Ti/(TiO2)PS+P2VK(4%)/Ti 電流電壓特性，限流:10mA 第二次循環 29
圖4-17 Ti/(TiO2)PS+P2VK(4%)/Ti 電流電壓特性，限流:10mA 第三次循環 30
圖4-18 Ti/(TiO2)PS+P2VK(4%)/Ti 電流電壓特性，限流:10mA 第四次循環 30
圖4-19 Ti/(TiO2)PS+P2VK(4%)/Ti 電流電壓特性，限流:10mA 第五次循環 31
圖4-20 Ti/(TiO2)PS+P2VK(4%)/Ti 電流電壓特性，限流:10mA 第六次循環 31
圖4-21 Ti/(TiO2)PS+P2VK(4%)/Ti 電流電壓特性，限流:10mA 第七次循環 32
圖4-22 Ti/(TiO2)PS+P2VK(4%)/Ti 電流電壓特性，限流:10mA 第八次循環 32
圖4-23 Ti/(TiO2)PS+P2VK(4%)/Ti 電流電壓特性，限流:10mA 第九次循環 33
圖4-24 Ti/(SiO2)PS+P2VK(4%)/Ti 電流電壓特性，限流:100mA 第一次循環 33
圖4-25 Ti/(SiO2)PS+P2VK(4%)/Ti 電流電壓特性，限流:100mA 第二次循環 34
圖4-26 Ti/(SiO2)PS+P2VK(4%)/Ti 電流電壓特性，限流:100mA 第三次循環 34
圖4-27 Ti/(SiO2)PS+P2VK(4%)/Ti 電流電壓特性，限流:10mA 35
圖4-28 Ti /PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:100mA 37
圖4-29 Ti /PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 37
圖4-30 Ti /PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:100mA 38
圖4-31 Ti /PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 38
圖4-32 Ti /(TiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:100mA 39
圖4-33 Ti /(TiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 39
圖4-34 Ti /(TiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:100m 未Forming前I-V量測 40
圖4-35 Ti /(TiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 未Forming前I-V量測 40
圖4-36 Ti /(SiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:100mA 41
圖4-37 Ti /(SiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 41
圖4-38 Ti /(SiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:100mA 未Forming前I-V量測 42
圖4-39 Ti /(SiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 未Forming前I-V量測 42
圖4-40 Ti /(TiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 量測電壓為-1V and 1V 44
圖4-41 Ti /(TiO2)PS+P2VK(4%/ZnO NRs)/Ti 量測電壓為-1V and 1V的記憶保持特性 44
圖4-42 Ti /(TiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 量測電壓為-2V and 2V 45
圖4-43 Ti /(TiO2)PS+P2VK(4%)/ZnO NRs /Ti 量測電壓為-2V and 2V的記憶保持特性 45
圖4-44 Ti /(TiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 量測電壓為-3V and 3V 46
圖4-45 Ti /(TiO2)PS+P2VK(4%)/ZnO NRs /Ti 量測電壓為-3V and 3V的記憶保持特性 46
圖4-46 Ti /(TiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 量測電壓為-4V and 4V 47
圖4-47 Ti /(TiO2)PS+P2VK(4%)/ZnO NRs /Ti 量測電壓為-4V and 4V的記憶保持特性 47
圖4-48 Ti /(SiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 量測電壓為-1V and 1V 48
圖4-49 Ti /(SiO2)PS+P2VK(4%)/ZnO NRs /Ti 量測電壓為-1V and 1V的記憶保持特性 48
圖4-50 Ti /(SiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 量測電壓為-2V and 2V 49
圖4-51 Ti /(SiO2)PS+P2VK(4%)/ZnO NRs /Ti量測電壓為-2V and 2V的記憶保持特性 49
圖4-52 Ti /(SiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 量測電壓為-3V and 3V 50
圖4-53 Ti /(SiO2)PS+P2VK(4%)/ZnO NRs /Ti 量測電壓為-3V and 3V的記憶保持特性 50
圖4-54 Ti /(SiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 量測電壓為4V and -4V 51
圖4-55 Ti /(SiO2)PS+P2VK(4%)/ZnO NRs /Ti 量測電壓為-4V and 4V的記憶保持特性 51
圖4-56 Ti /PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 量測電壓為1V and -1V 53
圖4-57 Ti /PS+P2VK(4%)/ZnO NRs /Ti Hold電壓為-1V and 1V, 5s量測時間1000秒的記憶保持特性 53
圖4-58 Ti /PS+P2VK(4%)/ZnO NRs /Ti Hold電壓為-2V and 2V, 5s量測時間1000秒的記憶保持特性 54
圖4-59 Ti /PS+P2VK(4%)/ZnO NRs /Ti Hold電壓為-3V and 3V, 5s量測時間1000秒的記憶保持特性 54
圖4-60Ti /PS+P2VK(4%)/ZnO NRs /Ti Hold電壓為-4V and 4V, 5s量測時間1000秒的記憶保持特性 55
圖4-61 Ti /(TiO2)PS+P2VK(4%)/ZnO NRs /Ti電流電壓特性，限流:10mA 量測電壓為1V and -1V 56
圖4-62 Ti /(TiO2)PS+P2VK(4%)/ZnO NRs /Ti Hold電壓為-1V and 1V, 5s量測時間1000秒的記憶保持特性 56
圖4-63 Ti /(TiO2)PS+P2VK(4%)/ZnO NRs /Ti Hold電壓為-2V and 2V, 5s量測時間1000秒的記憶保持特性 57
圖4-64Ti /(TiO2)PS+P2VK(4%)/ZnO NRs /Ti Hold電壓為-3V and 3V, 5s量測時間1000秒的記憶保持特性 57
圖4-65 Ti /(TiO2)PS+P2VK(4%)/ZnO NRs /Ti Hold電壓為-4V and 4V, 5s量測時間1000秒的記憶保持特性 58
圖4-66 Ti /(SiO2)PS+P2VK(4%)/ZnO NRs /Ti電流電壓特性，限流:10mA 量測電壓為1V and -1V 59
圖4-67 Ti /(SiO2)PS+P2VK(4%)/ZnO NRs /Ti Hold電壓為-1V and 1V, 5s量測時間1000秒的記憶保持特性 59
圖4-68 Ti /(SiO2)PS+P2VK(4%)/ZnO NRs /Ti Hold電壓為-2V and 2V, 5s量測時間1000秒的記憶保持特性 60
圖4-69 Ti /(SiO2)PS+P2VK(4%)/ZnO NRs /Ti Hold電壓為-1V and 1V, 5s量測時間1000秒的記憶保持特性 60
圖4-70 Ti /(SiO2)PS+P2VK(4%)/ZnO NRs /Ti Hold電壓為-4V and 4V, 5s量測時間1000秒的記憶保持特性 61
圖4-71 Ti /(ZnO)PS+P2VK(4%/ZnO NRs)/Ti電流電壓特性，限流:10mA 量測電壓為1V and -1V 62
圖4-72 Ti /(ZnO)PS+P2VK(4%)/ZnO NRs /Ti Hold電壓為-1V and 1V, 5s量測時間1000秒的記憶保持特性 62
圖4-73 Ti /(ZnO)PS+P2VK(4%)/ZnO NRs /Ti Hold電壓為-2V and 2V, 5s量測時間1000秒的記憶保持特性 63
圖4-74 Ti /(ZnO)PS+P2VK(4%)/ZnO NRs /Ti Hold電壓為-3V and 3V, 5s量測時間1000秒的記憶保持特性 63
圖4-75 Ti /(ZnO)PS+P2VK(4%)/ZnO NRs /Ti Hold電壓為-4V and 4V, 5s量測時間1000秒的記憶保持特性 64
圖4-76 Ti /PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 量測電壓為 2V~5V 66
圖4-77 Ti /(TiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 量測電壓為 2V~5V 66
圖4-78 Ti /(SiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 量測電壓為 2V~5V 67
圖4-79 Ti /(ZnO)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 量測電壓為 2V~5V 67
圖4-80 Ti /PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 量測電壓為-1V ~ -5V 68
圖4-81 Ti /(TiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 量測電壓為 -1V ~ -5V 68
圖4-82 Ti /(SiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 量測電壓為 -1V ~ -5V 69
圖4-83 Ti /(ZnO)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 量測電壓為 -1V ~ -5V 69
圖4-84 Ti /PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 70
圖4-85 Ti /(TiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 70
圖4-86 Ti /(SiO2)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 71
圖4-87 Ti /(ZnO)PS+P2VK(4%)/ZnO NRs /Ti 電流電壓特性，限流:10mA 71
圖4-88元件能階圖(平衡態) 72
圖4-89 元件能階圖(正偏壓) 74
圖4-90 元件能階圖(負偏壓) 74

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