進階搜尋


下載電子全文  
系統識別號 U0026-2408202004043200
論文名稱(中文) 室溫下溶液製程氧化鎳及錳摻雜氧化鎳電阻式記憶體之研製
論文名稱(英文) Investigation of RRAM fabricated at room temperature with Solution-Processed NiO and Mn-doped NiO Nanoparticles
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 108
學期 2
出版年 109
研究生(中文) 李家文
研究生(英文) Chia-Wen Lee
學號 Q16071306
學位類別 碩士
語文別 英文
論文頁數 68頁
口試委員 指導教授-蘇炎坤
口試委員-林俊良
口試委員-吳孟奇
口試委員-黃俊元
口試委員-楊智強
中文關鍵字 非揮發性電阻式記憶體  室溫  溶液製程  奈米粒子  氧化鎳  雜質摻雜  錳摻雜氧化鎳  金屬氧化物  氧空缺 
英文關鍵字 non-volatile resistive random access memory  room temperature  solution process  nanoparticles  impurity doping  NiO  Mn:NiO  metal oxides  oxygen vacancy 
學科別分類
中文摘要 本論文以室溫溶液製程製作氧化鎳及錳摻雜氧化鎳電阻式記憶體。以旋轉塗布的方法在在氧化銦錫/玻璃基板上沉積氧化鎳及錳摻雜氧化鎳奈米粒子懸浮液,並在室溫下乾燥,製造ITO/NiO or Mn:NiO/Al (金屬-絕緣層-金屬) 結構之電阻式記憶體。本論文與傳統溶液製程(溶膠凝膠法)相比,成功降低了製程溫度及簡化了製程步驟。電阻式記憶體具有讀寫速度快、結構簡單、單元面積小、密度高、低耗電、非揮發性等優點。
以純氧化鎳製作的電阻式記憶體元件可以正常開達220次並具有4.93*103的開關比。並且證實摻雜金屬錳能夠增加氧化鎳絕緣層的氧空缺濃度,幫助導電燈絲的形成,並且改善了元件的性能。以錳摻雜氧化鎳製作的電阻式記憶體元件可以正常開關大約641次並具有4.3*104的開關比。相較於其他溶液製程的元件,我們的元件具有更好的表現,尤其是元件耐久性及可靠度的改進。

英文摘要 In this thesis, NiO and Mn-doped NiO resistive random access memory (RRAM) are fabricated by solution process at room temperature. NiO and Mn-doped NiO nanoparticles suspension were deposited on ITO/glass substrates by spin coating method and dried at room temperature to fabricate ITO/NiO or Mn:NiO/Al (Metal-Insulator-Metal) RRAM structure. Compared with the traditional solution process (sol-gel method), this study successfully reduced the process temperature and simplified the process procedure. Resistive memory has the advantages of fast read and write speed, simple structure, small unit area, high density, low power consumption, and non-volatile.
A pure NiO-based RRAM device has the switching cycles of 220 times and an on/off ratio of 4.93*103. It was also confirmed that doping metal Mn can increase the concentration of the oxygen vacancy in the NiO film and help with the formation of conducting filaments, which improved the performance of devices. The RRAM devices with Mn-doped NiO showed the switching cycles of 641 times and an on/off ratio of 4.3*104. Compared with the devices made by other solution methods, our devices have better performance, especially in endurance and reliability.
論文目次 摘要 I
Abstract II
致謝 IV
Contents V
List of Tables VIII
Figure Captions IX
Chapter 1: Introduction 1
1-1 Introduction of Memory Devices 1
1-1-1 Volatile Memory 1
1-1-1-1 Dynamic Random Access Memory 1
1-1-1-2 Static Random Access Memory 1
1-1-2 Non-Volatile Memory 2
1-1-2-1 Flash Memory 2
1-1-2-2 Ferroelectric Random Access Memory 3
1-1-2-3 Phase Change Random Access Memory 4
1-1-2-4 Resistive Random Access Memory 5
1-2 Motivation 5
1-3 Organization of This Thesis 7
Chapter 2: Literature Review 7
2-1 Resistive Switching Behavior 7
2-1-1 Unipolar Devices 7
2-1-2 Bipolar Devices 7
2-2 Resistive Switching Mechanisms 8
2-2-1 Filamentary Conducting Path 8
2-2-1-1 Thermochemical Mechanism 9
2-2-1-2 Electrochemical Metallization 9
2-2-1-3 Valence Change Mechanism 10
2-2-2 Interface-Type Path 11
2-3 Conduction Mechanisms 12
2-3-1 Electrode-Limited Conduction Mechanisms 13
2-3-1-1 Schottky emission 13
2-3-1-2 Fowler-Nordheim tunneling and direct tunneling 14
2-3-1-3 Thermionic-field Emission 15
2-3-2 Bulk-Limited Conduction Mechanisms 16
2-3-2-1 Poole-Frenkel emission 16
2-3-2-2 Hopping conduction 17
2-3-2-3 Ohmic conduction 18
2-3-2-4 Space-charge-limited conduction 19
2-3-2-5 Ionic conduction 20
Chapter 3: Processing Procedure of RRAM 22
3-1 Materials 22
3-1-1 Metal Bottom Electrode: ITO 22
3-1-2 Insulator: NiO 22
3-1-3 Metal Top Electrode: Al 22
3-2 Preparation of NiO thin film and RRAM 23
3-2-1 Synthesis of NiO Nanoparticles Suspension 23
3-2-2 Synthesis of Mn:NiO Nanoparticles Suspension 23
3-2-3 Device fabrication 24
3-3 Experimental Equipment 25
3-3-1 Electrical Measurement 25
3-3-2 X-ray Diffraction 26
3-3-3 X-ray Photoelectron Spectroscopy 27
3-3-4 Scanning Electron Microscope 28
3-3-5 Atomic Force Microscope 28
Chapter 4: Switching Memory Devices of ITO/NiO/Al 30
4-1 Motivation 30
4-2 Device Fabrication 31
4-3 Results and Discussion 32
4-3-1 (A) Devices with NiO deposited by two-step spin-coating method 32
4-3-1-1 I-V Characteristics 32
4-3-1-2 Endurance 33
4-3-1-3 Cumulative Probability 34
4-3-1-4 Comparison of devices with different spin rates 36
4-3-2 (B) Devices with NiO deposited by one-step spin-coating method 37
4-3-2-1 I-V Characteristic 37
4-3-2-2 Endurance 37
4-3-2-3 Cumulative Probability 38
4-3-3 Comparison of devices fabricated by (a) two-step and (b)one-step spin-coating method 39
4-3-3-1 SEM 39
4-3-3-2 AFM 39
4-3-4 XRD 40
4-3-5 XPS 41
4-3-6 Conduction Mechanisms 43
4-3-7 Resistive Switching Mechanisms 44
4-4 Summary 45
Chapter 5: Switching Memory Devices of ITO/Mn:NiO/Al 46
5-1 Motivation 46
5-2 Device fabrication 48
5-3 Results and Discussion 49
5-3-1 XPS 49
5-3-2 I-V characteristics 50
5-3-3 Endurance 51
5-3-4 Cumulative probability 52
5-3-5 SEM 53
5-3-6 AFM 54
5-3-7 Conduction Mechanisms 55
5-4 Summary 58
Chapter 6: Conclusions 60
Chapter 7: Future Work 62
7-1 Fabrication of the devices with flexible substrates 62
7-2 Effect of light exposure on the RRAM devices 62
References 64
參考文獻 [1] J. S. Meena, S. M. Sze, U. Chand, and T.-Y. Tseng, "Overview of emerging nonvolatile memory technologies," Nanoscale research letters, vol. 9, no. 1, p. 526, 2014.
[2] N. Papandreou et al., "Drift-tolerant multilevel phase-change memory," in 2011 3rd IEEE International Memory Workshop (IMW), 2011: IEEE, pp. 1-4.
[3] T. Perez and C. A. De Rose, "Non-volatile memory: Emerging technologies and their impacts on memory systems," Porto Alegre, 2010.
[4] F. Zahoor, T. Z. Azni Zulkifli, and F. A. Khanday, "Resistive random access memory (RRAM): an overview of materials, switching mechanism, performance, multilevel cell (MLC) storage, modeling, and applications," Nanoscale Research Letters, vol. 15, pp. 1-26, 2020.
[5] A. Sawa, "Resistive switching in transition metal oxides," Materials today, vol. 11, no. 6, pp. 28-36, 2008.
[6] R. Waser, R. Dittmann, G. Staikov, and K. Szot, "Redox‐based resistive switching memories–nanoionic mechanisms, prospects, and challenges," Advanced materials, vol. 21, no. 25-26, pp. 2632-2663, 2009.
[7] Y. Li, S. Long, Q. Liu, H. Lü, S. Liu, and M. Liu, "An overview of resistive random access memory devices," Chinese Science Bulletin, vol. 56, no. 28-29, p. 3072, 2011.
[8] J. Wu, J. Cao, W.-Q. Han, A. Janotti, and H.-C. Kim, Functional metal oxide nanostructures. Springer Science & Business Media, 2011.
[9] M. Sowinska, "In-operando hard X-ray photoelectron spectroscopy study on the resistive switching physics of HfO2-based RRAM," 2014.
[10] F.-C. Chiu, "A review on conduction mechanisms in dielectric films," Advances in Materials Science and Engineering, vol. 2014, 2014.
[11] E. W. Lim and R. Ismail, "Conduction mechanism of valence change resistive switching memory: a survey," Electronics, vol. 4, no. 3, pp. 586-613, 2015.
[12] M. Guziewicz et al., "Electrical and optical properties of NiO films deposited by magnetron sputtering," Optica Applicata, vol. 41, no. 2, 2011.
[13] D. Adler and J. Feinleib, "Electrical and optical properties of narrow-band materials," Physical Review B, vol. 2, no. 8, p. 3112, 1970.
[14] F. Jiang, W. C. Choy, X. Li, D. Zhang, and J. Cheng, "Post‐treatment‐free solution‐processed non‐stoichiometric NiOx nanoparticles for efficient hole‐transport layers of organic optoelectronic devices," Advanced Materials, vol. 27, no. 18, pp. 2930-2937, 2015.
[15] E. Papis-Polakowska et al., "X-Ray photoelectron spectroscopy-methodology and application," Acta Physica Polonica A, vol. 125, no. 4, pp. 1061-1064, 2014.
[16] J. Metson, "Charge compensation and binding energy referencing in XPS analysis," Surface and Interface Analysis: An International Journal devoted to the development and application of techniques for the analysis of surfaces, interfaces and thin films, vol. 27, no. 12, pp. 1069-1072, 1999.
[17] B. R. Kumar and T. S. Rao, "AFM studies on surface morphology, topography and texture of nanostructured zinc aluminum oxide thin films," Digest Journal of Nanomaterials and Biostructures, vol. 7, no. 4, pp. 1881-1889, 2012.
[18] L. Goux et al., "Evidences of oxygen-mediated resistive-switching mechanism in TiNHfO 2Pt cells," Applied Physics Letters, vol. 97, no. 24, p. 243509, 2010.
[19] H. Lee et al., "Low power and high speed bipolar switching with a thin reactive Ti buffer layer in robust HfO2 based RRAM," in 2008 IEEE International Electron Devices Meeting, 2008: IEEE, pp. 1-4.
[20] Y.-T. Su et al., "A method to reduce forming voltage without degrading device performance in hafnium oxide-based 1T1R resistive random access memory," IEEE Journal of the Electron Devices Society, vol. 6, pp. 341-345, 2018.
[21] D. Acharyya, A. Hazra, and P. Bhattacharyya, "A journey towards reliability improvement of TiO2 based resistive random access memory: a review," Microelectronics reliability, vol. 54, no. 3, pp. 541-560, 2014.
[22] S.-X. Chen, S.-P. Chang, S.-J. Chang, W.-K. Hsieh, and C.-H. Lin, "Highly Stable Ultrathin TiO2 Based Resistive Random Access Memory with Low Operation Voltage," ECS Journal of Solid State Science and Technology, vol. 7, no. 7, p. Q3183, 2018.
[23] Z. Wei et al., "Highly reliable TaOx ReRAM and direct evidence of redox reaction mechanism," in 2008 IEEE International Electron Devices Meeting, 2008: IEEE, pp. 1-4.
[24] F.-C. Chiu, W.-C. Shih, and J.-J. Feng, "Conduction mechanism of resistive switching films in MgO memory devices," Journal of Applied Physics, vol. 111, no. 9, p. 094104, 2012.
[25] X. Yu, T. J. Marks, and A. Facchetti, "Metal oxides for optoelectronic applications," Nature materials, vol. 15, no. 4, pp. 383-396, 2016.
[26] Q. Yang, J. Sha, X. Ma, and D. Yang, "Synthesis of NiO nanowires by a sol-gel process," Materials Letters, vol. 59, no. 14-15, pp. 1967-1970, 2005.
[27] N. N. M. Zorkipli, N. H. M. Kaus, and A. A. Mohamad, "Synthesis of NiO nanoparticles through sol-gel method," Procedia chemistry, vol. 19, pp. 626-631, 2016.
[28] M. Alagiri, S. Ponnusamy, and C. Muthamizhchelvan, "Synthesis and characterization of NiO nanoparticles by sol–gel method," Journal of Materials Science: Materials in Electronics, vol. 23, no. 3, pp. 728-732, 2012.
[29] A. Al-Ghamdi, W. E. Mahmoud, S. J. Yaghmour, and F. Al-Marzouki, "Structure and optical properties of nanocrystalline NiO thin film synthesized by sol–gel spin-coating method," Journal of Alloys and Compounds, vol. 486, no. 1-2, pp. 9-13, 2009.
[30] N.-N. Ge, C.-H. Gong, X.-C. Yuan, H.-Z. Zeng, and X.-H. Wei, "Effect of Mn doping on electroforming and threshold voltages of bipolar resistive switching in Al/Mn: NiO/ITO," RSC advances, vol. 8, no. 52, pp. 29499-29504, 2018.
[31] Y. Li et al., "Analog and digital bipolar resistive switching in solution-combustion-processed NiO memristor," ACS applied materials & interfaces, vol. 10, no. 29, pp. 24598-24606, 2018.
[32] J. Chu, Y. Li, X. Fan, H. Shao, W. Duan, and Y. Pei, "Multistate data storage in solution-processed NiO-based resistive switching memory," Semiconductor Science and Technology, vol. 33, no. 11, p. 115007, 2018.
[33] H. Zhang et al., "Pinhole-free and surface-nanostructured NiO x film by room-temperature solution process for high-performance flexible perovskite solar cells with good stability and reproducibility," ACS nano, vol. 10, no. 1, pp. 1503-1511, 2016.
[34] D. Ielmini, "Resistive switching memories based on metal oxides: mechanisms, reliability and scaling," Semiconductor Science and Technology, vol. 31, no. 6, p. 063002, 2016.
[35] M. C. Biesinger, B. P. Payne, L. W. Lau, A. Gerson, and R. S. C. Smart, "X‐ray photoelectron spectroscopic chemical state quantification of mixed nickel metal, oxide and hydroxide systems," Surface and Interface Analysis: An International Journal devoted to the development and application of techniques for the analysis of surfaces, interfaces and thin films, vol. 41, no. 4, pp. 324-332, 2009.
[36] M.-S. Wang et al., "Photoemission spectroscopy study of oxygen spectrum and the chemical failure process of Alq3-based light-emitting devices," Journal of Applied Physics, vol. 109, no. 9, p. 093502, 2011.
[37] D. S. Dalavi, R. S. Devan, R. S. Patil, Y.-R. Ma, and P. S. Patil, "Electrochromic performance of sol–gel deposited NiO thin film," Materials Letters, vol. 90, pp. 60-63, 2013.
[38] D. Ielmini, R. Bruchhaus, and R. Waser, "Thermochemical resistive switching: materials, mechanisms, and scaling projections," Phase Transitions, vol. 84, no. 7, pp. 570-602, 2011.
[39] X. Wu et al., "Transparent bipolar resistive switching memory devices based on Mn doped SnO2 films," Journal of Alloys and Compounds, vol. 602, pp. 175-179, 2014.
[40] J. Luo, H. Zhang, J. Wen, and X. Yang, "Effect of doping concentration and annealing temperature on threshold voltages of bipolar resistive switching in Mn-doped BiFeO 3 films," Journal of Sol-Gel Science and Technology, vol. 78, no. 1, pp. 166-170, 2016.
[41] X. Wang, Q. Shao, C. Leung, and A. Ruotolo, "Non-volatile, reversible switching of the magnetic moment in Mn-doped ZnO films," Journal of applied physics, vol. 113, no. 17, p. 17C301, 2013.
[42] K.-M. Chang, W.-H. Tzeng, K.-C. Liu, Y.-C. Chan, and C.-C. Kuo, "Investigation on the abnormal resistive switching induced by ultraviolet light exposure based on HfOx film," Microelectronics Reliability, vol. 50, no. 12, pp. 1931-1934, 2010.
[43] K. Tsunoda et al., "Low power and high speed switching of Ti-doped NiO ReRAM under the unipolar voltage source of less than 3 V," in 2007 IEEE International Electron Devices Meeting, 2007: IEEE, pp. 767-770.
[44] Z. Qiang et al., "Effects of interaction between defects on the uniformity of doping HfO2-based RRAM: a first principle study," Journal of Semiconductors, vol. 34, no. 3, p. 032001, 2013.
[45] X.-C. Yuan, X.-H. Wei, B. Dai, and H.-Z. Zeng, "Nonlinear switching in Al/Li: NiO/ITO forming-free resistive memories caused by interfacial layer," Applied Surface Science, vol. 362, pp. 506-511, 2016.
[46] M. Lee et al., "Comparative structural and electrical analysis of NiO and Ti doped NiO as materials for resistance random access memory," Journal of Applied Physics, vol. 103, no. 1, p. 013706, 2008.
[47] D. Ning, P. Hua, and W. Wei, "Effects of different dopants on switching behavior of HfO2-based resistive random access memory," Chinese Physics B, vol. 23, no. 10, p. 107306, 2014.
[48] X.-C. Yuan, J.-L. Tang, H.-Z. Zeng, and X.-H. Wei, "Abnormal coexistence of unipolar, bipolar, and threshold resistive switching in an Al/NiO/ITO structure," Nanoscale research letters, vol. 9, no. 1, pp. 1-5, 2014.
[49] S. Mitra, S. Chakraborty, and K. S. Menon, "Study of anti-clockwise bipolar resistive switching in Ag/NiO/ITO heterojunction assembly," Applied Physics A, vol. 115, no. 4, pp. 1173-1179, 2014.
[50] K.-K. Chiang, J.-S. Chen, and J.-J. Wu, "Aluminum electrode modulated bipolar resistive switching of Al/fuel-assisted NiO x/ITO memory devices modeled with a dual-oxygen-reservoir structure," ACS Applied Materials & Interfaces, vol. 4, no. 8, pp. 4237-4245, 2012.
[51] D. Liu and T. L. Kelly, "Perovskite solar cells with a planar heterojunction structure prepared using room-temperature solution processing techniques," Nature photonics, vol. 8, no. 2, pp. 133-138, 2014.
[52] Q. He, K. Yao, X. Wang, X. Xia, S. Leng, and F. Li, "Room-temperature and solution-processable Cu-doped nickel oxide nanoparticles for efficient hole-transport layers of flexible large-area perovskite solar cells," ACS applied materials & interfaces, vol. 9, no. 48, pp. 41887-41897, 2017.
[53] H. Cai et al., "All-inorganic perovskite Cs4PbBr6 thin films in optoelectronic resistive switching memory devices with a logic application," Ceramics International, vol. 45, no. 5, pp. 5724-5730, 2019.
論文全文使用權限
  • 同意授權校內瀏覽/列印電子全文服務,於2020-08-31起公開。
  • 同意授權校外瀏覽/列印電子全文服務,於2020-08-31起公開。


  • 如您有疑問,請聯絡圖書館
    聯絡電話:(06)2757575#65773
    聯絡E-mail:etds@email.ncku.edu.tw