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实验表明掺杂是一种改善阻变存储器性能的有效手段,但其物理机理鲜有研究.本文采用第一性原理方法系统研究了过渡金属元素X(X=Mn,Fe,Co,Ni)掺杂对ZnO基阻变存储器中氧空位迁移势垒和形成能的影响.计算结果表明Ni掺杂可同时有效降低+1和+2价氧空位在掺杂原子附近的迁移势垒,X掺杂均减小了氧空位的形成能,特别是掺杂Ni时氧空位的形成能减小最为显著(比未掺杂时减少了64%).基于该结果制备了未掺杂和Ni掺杂ZnO阻变存储器,研究表明通过掺杂控制体系中氧空位的迁移势垒和形成能,可以有效改善器件的初始化过程、操作电压、保持性等阻变性能.研究结果有助于理解探究影响阻变的微观机制,并可为掺杂提高阻变存储器性能提供一定的理论指导.Resistance random access memory (RRAM) based on resistive switching in metal oxides has attracted considerable attention as a promising candidate for next-generation nonvolatile memory due to its high operating speed, superior scalability, and low power consumption. However, some operating parameters of RRAM cannot meet the practical requirement, which impedes its commercialization. A lot of experimental results show that doping is an effective method of improving the performance of RRAM, while the study on the physical mechanism of doping is rare. It is generally believed that the formation and rupture of conducting filaments, caused by the migration of oxygen vacancies under electric field play a major role in resistive switching of metal oxide materials. In this work, the first principle calculation based on density functional theory is performed to study the effects of transition metal element X (X=Mn, Fe, Co, and Ni) doping on the migration barriers and formation energy of oxygen vacancy in ZnO. The calculation results show that the migration barriers of both the monovalent and divalent oxygen vacancy are reduced significantly by Ni doping. This result indicates that the movement of oxygen vacancies in Ni doped ZnO is easier than in undoped ZnO RRAM device, thus Ni doping is beneficial to the formation and rupture of oxygen vacancy conducting filaments. Furthermore, the calculation results show that the formation energy of the oxygen vacancy in ZnO system can be reduced by X doping, especially by Ni doping. The formation energy of the oxygen vacancy decreases from 0.854 for undoped ZnO to 0.307 eV for Ni doped ZnO. Based on the above calculated results, Ni doped and undoped ZnO RRAM device are prepared by using pulsed laser deposition method under an oxygen pressure of 2 Pa. The Ni doped ZnO RRAM device shows the optimized forming process, low operating voltage (0.24 V and 0.34 V for Set and Reset voltage), and long retention time (>104 s). Set and Reset voltage in Ni doped ZnO device decrease by 80% and 38% respectively compared with those in undoped ZnO device. It is known that the density of oxygen vacancies in the device is dependent on the oxygen pressure during preparation. The Ni doped ZnO RRAM device under a higher oxygen pressure (5 Pa) is also prepared. The Ni doped ZnO RRAM device prepared under 5 Pa oxygen pressure shows a little higher Set and Reset voltage than the device prepared under 2 Pa oxygen pressure, while the operating voltages are still lower than those of undoped ZnO RRAM. Thus, the doping effect in the ZnO system is affected by the density of oxygen vacancies in the device. Our work provides a guidance for optimizing the performance of the metal oxide based RRAM device through element doping.
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Keywords:
- resistance random access memory /
- doping /
- ZnO /
- first principle calculations
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[2] Liu D Q, Cheng H F, Zhu X, Wang N N, Zhang C Y 2014 Acta Phys. Sin. 63 187301 (in Chinese) [刘东青, 程海峰, 朱玄, 王楠楠, 张朝阳 2014 物理学报 63 187301]
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[11] Chen G, Song C, Chen C, Gao S, Zeng F, Pan F 2012 Adv. Mater. 24 3515
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[15] Ren S, Chen W, Guo J, Yang H, Zhao X 2017 J. Alloys Compd. 708 484
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[17] Perdew J P, Wang Y 1992 Phys. Rev. B 45 13244
[18] Vanderbilt D 1990 Phys. Rev. B 41 7892
[19] Zhao Q, Zhou M, Zhang W, Liu Q, Li X, Liu M, Dai Y 2013 J. Semicond. 34 032001
[20] Janotti A, van de Walle C G 2007 Phys. Rev. B 76 165202
[21] Ermoshin V A, Veryazov V A 1995 Phys. Status Solidi B 189 K49
[22] Zhao J, Dong J Y, Zhao X, Chen W 2014 Chin. Phys. Lett. 31 057307
[23] Wong H S P, Lee H Y, Yu S, Chen Y S, Wu Y, Chen P S, Lee B, Chen F T, Tsai M J 2012 Proc. IEEE 100 1951
[24] Kamiya K, Yang M Y, Nagata T, Park S G, Magyari Köpe B, Chikyow T, Yamada K, Niwa M, Nishi Y, Shiraishi K 2013 Phys. Rev. B 87 155201
[25] van de Walle C G, Neugebauer J 2004 J. Appl. Phys. 95 3851
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[1] Yang J J, Strukov D B, Stewart D R 2013 Nat. Nanotechnol. 8 13
[2] Liu D Q, Cheng H F, Zhu X, Wang N N, Zhang C Y 2014 Acta Phys. Sin. 63 187301 (in Chinese) [刘东青, 程海峰, 朱玄, 王楠楠, 张朝阳 2014 物理学报 63 187301]
[3] Cao M G, Chen Y S, Sun J R, Shang D S, Liu L F, Kang J F, Shen B G 2012 Appl. Phys. Lett. 101 203502
[4] Xiong Y Q, Zhou W P, Li Q, He M C, Du J, Cao Q Q, Wang D H, Du Y W 2014 Appl. Phys. Lett. 105 032410
[5] Pan F, Gao S, Chen C, Song C, Zeng F 2014 Mater. Sci. Eng. R-Rep. 83 1
[6] Yang C S, Shang D S, Liu N, Shi G, Shen X, Yu R C, Li Y Q, Sun Y 2017 Adv. Mater. 29 1700906
[7] Waser R, Dittmann R, Staikov G, Szot K 2009 Adv. Mater. 21 2632
[8] Zhang H, Liu L, Gao B, Qiu Y, Liu X, Lu J, Han R, Kang J, Yu B 2011 Appl. Phys. Lett. 98 042105
[9] Liu Q, Long S B, Wang W, Zuo Q Y, Zhang S, Chen J N, Liu M 2009 IEEE Electron Device Lett. 30 1335
[10] Jung K, Choi J, Kim Y, Im H, Seo S, Jung R, Kim D, Kim J S, Park B H, Hong J P 2008 J. Appl. Phys. 103 034504
[11] Chen G, Song C, Chen C, Gao S, Zeng F, Pan F 2012 Adv. Mater. 24 3515
[12] Chen G, Peng J J, Song C, Zeng F, Pan F 2013 J. Appl. Phys. 113 104503
[13] Ren S X, Sun G W, Zhao J, Dong J Y, Wei Y, Ma Z C, Zhao X, Chen W 2014 Appl. Phys. Lett. 104 232406
[14] Ren S, Dong J, Chen W, Zhang L, Guo J, Zhang L, Zhao J, Zhao X 2015 J. Appl. Phys. 118 233902
[15] Ren S, Chen W, Guo J, Yang H, Zhao X 2017 J. Alloys Compd. 708 484
[16] Segall M D, Philip J D L, Probert M J, Pickard C J, Hasnip P J, Clark S J, Payne M C 2002 J. Phys.:Condens. Matter 14 2717
[17] Perdew J P, Wang Y 1992 Phys. Rev. B 45 13244
[18] Vanderbilt D 1990 Phys. Rev. B 41 7892
[19] Zhao Q, Zhou M, Zhang W, Liu Q, Li X, Liu M, Dai Y 2013 J. Semicond. 34 032001
[20] Janotti A, van de Walle C G 2007 Phys. Rev. B 76 165202
[21] Ermoshin V A, Veryazov V A 1995 Phys. Status Solidi B 189 K49
[22] Zhao J, Dong J Y, Zhao X, Chen W 2014 Chin. Phys. Lett. 31 057307
[23] Wong H S P, Lee H Y, Yu S, Chen Y S, Wu Y, Chen P S, Lee B, Chen F T, Tsai M J 2012 Proc. IEEE 100 1951
[24] Kamiya K, Yang M Y, Nagata T, Park S G, Magyari Köpe B, Chikyow T, Yamada K, Niwa M, Nishi Y, Shiraishi K 2013 Phys. Rev. B 87 155201
[25] van de Walle C G, Neugebauer J 2004 J. Appl. Phys. 95 3851
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