-
为了改善HfO2的阻变特性, 提高氧空位(VO)导电细丝形成的一致性和均匀性, 采用基于密度泛函理论的第一性原理计算方法研究了掺杂Al的HfO2阻变材料的微观特性. 结果表明, 间隙Al (Int-Al)更适合掺入到HfO2中, 并且Int-Al与VO相对位置越近, 阻变材料趋于稳定的收敛速度越快, 形成能越小. 不同Int-Al浓度对含有VO缺陷的HfO2超胞的影响结果显示, 当掺杂Int-Al浓度为4.04%时, 分波电荷态密度图能够形成相对较好的电荷通道, 最大等势面和临界等势面值均为最高, 有利于改善HfO2阻变材料中导电细丝形成的一致性和均匀性; 形成能计算结果显示, 当Int-Al浓度低于4.04%时形成能变化缓慢, 当高于4.04%时则异常增大, 表明缺陷体系随Int-Al浓度增大越来越难以形成; 进一步研究掺杂Int-Al浓度为4.04%时晶格结构的变化, 结果显示缺陷形成能显著降低, 有利于形成完美的导电通道. 该研究为改善基于HfO2阻变存储材料的性能有一定的借鉴意义.
In order to improve the resistance properties of HfO2 and increase the consistency and uniformity of conductive filaments formed by oxygen vacancies (VO), the first-principles calculation method based on density functional theory is used to study the micro-properties of Al-doped HfO2 resistive materials. The results show that the interval Al (Int-Al) is more suitable for being incorporated into HfO2, and the closer to the relative position of VO the Int-Al, the faster the convergence rate of the resistive material tends to be stable, and the smaller the formation energy. The effects of different Int-Al concentrations on the formation of HfO2 supercells with VO defects show that when the concentration of doped Int-Al is 4.04%, the fractional charge state density map can form relatively good charge channels. The maximum and critical equipotential surface values are highest, which is conducive to improving the consistency and uniformity of the formation of conductive filaments in HfO2 resistive materials. The calculation of energy formation shows that the change is slow when the concentration of Int-Al is lower than 4.04%. When the concentration of Int-Al is higher than 4.04%, the abnormal increase occurs, which indicates that the defect system becomes more and more difficult to form with the increase of the concentration of Int-Al. The introduction of the impurity and the VO defect destroy the original complete crystal structure, which causes the position of the atoms around the impurity to shift, and the valence electron orbit and the energy level of the crystal are changed, and the distribution of the internal charges of the HfO2 defect system is affected. In order to study the effect of the change of the lattice structure on the formation of the VO conductive filament, the VASP software package is used to calculate the relative ratio of the atoms in the lattice structure of the HfO2 defect system as the reference and the relative ratio of the HfO2 defect system after the optimizing the lattice structure. Further study of the change of lattice structure, when the concentration of doped Int-Al is 4.04%, shows that the defect formation energy decreases significantly, which is conducive to the formation of perfect conductive channel. The conductive channel has a certain reference significance for improving the performance of HfO2 based resistive variable memory materials. -
Keywords:
- HfO2 /
- first principles /
- interval Al /
- lattice structure
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图 1 HfO2缺陷超胞模型 (a) Sub-Al掺杂到含有VO的HfO2; (b)—(f) Int-Al掺杂含有VO的HfO2, 掺杂Int-Al的个数分别为1—5
Fig. 1. HfO2 defect supercell model: (a) Sub-Al doping into HfO2 containing VO; (b)−(f) Int-Al doping into HfO2 containing VO, the number of Int-Al is 1 to 5.
图 2 杂质Al的形成能 (插图中显示了杂质Al的存在方式, 虚线圆表示失去一个O原子后形成的VO)
Fig. 2. Formation energy of impurity Al, The illustration shows the existence of impurity Al. The dotted circle indicates the formation after losing an O atom.
图 3 VO缺陷HfO2体系中Int-Al形成能 (插图显示了Int-Al与VO不同间距的分波电荷态密度)
Fig. 3. Int-Al formation energy in VO deficient HfO2 system, the illustration shows the partial wave charge density of Int-Al and VO at different pitches.
图 4 不同浓度Int-Al体系的分波电荷态密度图 (a) 1.04%; (b) 2.06%; (c) 3.06%; (d) 4.04%; (e) 5%
Fig. 4. The partial wave charge density of Int-Al systems with different concentrations: (a) 1.04%; (b) 2.06%; (c) 3.06%; (d) 4.04%; (e) 5%.
图 5 变组分Int-Al掺杂VO缺陷HfO2体系的分波电荷密度等势面值, 插图为Int-Al与VO共掺时的形成能
Fig. 5. The partial wave charge density equipotential surface value of variable component Int-Al doped VO defect HfO2 system. The illustration shows the formation energy of Int-Al and VO co-doping.
图 6 HfO2缺陷超胞晶格结构不变的分波电荷态密度
Fig. 6. The partial wave charge density of in HfO2 defect supercell lattice with invariant lattice structure.
-
[1] 赵强 2013 硕士学位论文 (安徽: 安徽大学)
Zhao Q 2013 M. S. Thesis (Anhui: Anhui University) (in Chinese)
[2] 张文博, 王华, 许积文, 刘国保, 谢航, 杨玲 2018 材料导报 32 1932
Google Scholar
Zhang W B, Wang H, Xu J W, Liu G B, Xie H, Yang L 2018 Mater. Rev. 32 1932
Google Scholar
[3] 杨龙康 2014 硕士学位论文 (西安: 西安电子科技大学)
Yang L K 2014 M. S. Thesis (Xian: Xi'an University of Science and Technology) (in Chinese)
[4] 王源, 贾嵩, 甘学温 2011 北京大学学报 47 565
Google Scholar
Wang Y, Jia S, Gan X W 2011 Acta Sci. Natur. Univ. Pekinensis 47 565
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[5] Frascaroli J, Volpe F G, Brivio S, Spiga S 2015 Microelectron. Eng. 147 104
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[10] 张志超, 王芳, 吴仕剑, 李毅, 弭伟, 赵金石, 张楷亮 2018 物理学报 67 057301
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Zhao Y Y 2015 M. S. Thesis (Anhui: Anhui University) (in Chinese)
[13] Xue K H, Blaise P, Fonseca L R C, Nishi Y 2013 Phys. Rev. Lett. 110 065502
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[23] Gao B, Zhang H W, Yu S, Sun B, Liu L F, Liu X Y, Wang Y, Han R Q, Kang J F, Yu B, Wang Y Y 2009 Vlsi Technology Symposium on Kamakura Japan, September 7-9, 2009 p30
[24] 杨金 2014 博士学位论文 (安徽: 安徽大学)
Yang J 2014 Ph. D. Dissertation (Anhui: Anhui University) (in Chinese)
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