非挥发性阻变存储器阻变机理及性能研究
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摘要
随着半导体技术节点的不断向前推进,目前主流的基于电荷存储机制的浮栅Flash存储器正面临着严重的技术挑战,如浮栅耦合、电荷泄漏、相邻单元之间的串扰问题等,因此亟需寻找下一代非挥发性存储器。目前,国际上研究较多的新型非挥发性存储器主要有：相变存储器(PRAM),磁阻存储器(MRAM),铁电存储器(FRAM)和可逆的电致阻变随机存储器(RRAM),其中对RRAM的研究如火如荼,RRAM因其结构简单、功耗低、器件密度高、编程／擦写速度快、且与CMOS工艺兼容等一系列突出优点而成为替代多晶硅浮栅存储器的有力竞争者之一,其作为一种采用非电荷存储机制的存储器在32nm工艺节点以下将有很大的发展空间。
目前,制约RRAM技术发展和应用的主要瓶颈之一是发生电阻转变效应的物理机制、电荷存储机理尚不明确,同时,RRAM器件在稳定性、均匀性、可重复性、擦写速度以及数据保持性等方面都还存在问题,而目前对器件的研究主要是通过实验研制、显微表征及实时监测基础上进行观察和分析,存在实验平台要求高、表征和测试仪器高端、实验周期长等问题。针对上述问题,本论文结合并行计算与第一性原理开展多层次、多维度的模拟手段,从物理角度解释载流子的输运过程和存储机理,通过掺杂、制造缺陷和控制化合价等手段对阻变材料进行改性,给出材料的微观参数和存储器的宏观电学量的定量关系,为RRAM的优化设计及可靠集成提供理论指导和设计工具。
针对RRAM的研究现状进行统计,了解其阻变的宏观特性等方面的不足,研究了纳米尺度下RRAM二元金属氧化物阻变材料HfO2的氧空位(Vo)陷阱效应、掺杂效应(Ag)等对器件特性的影响以及阻变存储器的微观阻变机理。研究表明单独Vo缺陷和单独Ag杂质均可以在禁带中引入杂质能级,且都分别可以形成导电细丝；针对Vo和Ag都能形成导电细丝的情况,研究了Ag和Vo共掺杂的复合缺陷体系,结果表明共掺杂体系的导电性能增强、稳定性更好；而在相同浓度下,Ag杂质能级能够通过Ag离子的作用加以Hf离子的辅助下形成导电细丝,而Vo缺陷能级没有导电细丝的形成。且在Vo存在的前提下,Ag离子的迁移将变得更加容易,即Vo可以辅助Ag离子迁移,增强了体系电化学性能。
电极以及阻变材料的选择将直接影响着复合材料的性能,其界面结合的状态对整个阻变存储器的性能起着至关重要的作用,对比研究了Cu/HfO2不同切面组合的复合材料界面模型。结果表明,复合材料的界面不同,对RRAM器件的性能会产生很大影响。在研究的所有界面体系中,Cu(111)/HfO2(010)失配率最小,界面束缚能最大,界面体系相对最稳定；且只有Cu(111)/HfO2(010)复合材料体系出现了垂直Cu电极方向完整连通的电子通道,界面处有电子的相互转移、成键的存在,表明电子在此方向上具有局域性、连通性,与阻变存储器(RRAM)器件导通方向一致。针对Cu(111)/HfO2(010)复合材料界面体系,探讨了其整体性能,并研究了电极对界面处及阻变材料的影响。研究表明越靠近界面处,Cu和Vo缺陷越容易形成和存在,Cu原子越容易进入HfO2体内,也即Cu将呈阶梯状往HfO2内部扩散以形成缺陷体系,在外加电压下易发生电化学反应,从而导致Cu导电细丝的形成与断裂,更有利于RRAM器件电阻开关特性的产生。
对二元金属氧化物阻变材料进行掺杂可以改变其存储特性、电学特性,而对于掺杂元素进入材料体内后所具有的价电子数或化合价态的研究较少,鉴于此,研究了掺杂金属元素进入阻变材料后是否具有化合价态以及不同化合价态对阻变存储器材料性能的影响,首先通过电子亲和能以及缺陷形成能确定掺杂元素得失电子情况；其次通过差分电荷密度和修正的Bader分析确定了得失电子的具体位置；最后系统研究了掺杂元素具有不同化合价态对RRAM阻变材料及其性能的影响。
结果将为RRAM存储器的制备及性能提高提供理论指导和设计工具,必将在更深层次上理解和发展RRAM起到关键作用。
With the development of semiconductor technology node, the Flash memory confronts many problems, such as the coupling between floating gates, charge leakage, cross-coupling between cells and so on. Therefore, it is essential to explore the next generation of non-volatile memory. At present, the explorations mainly concentrate on the followings:phase random access memory (PRAM), magnetic random access memory (MRAM), ferroelectric random access memory (FRAM) and resistive random access memory (RRAM). Moreover, due to the advantages including simple structure, low power consumption, high density, fast program/erase speed and compatibility with CMOS technology, RRAM is regard as the most promising candidate for the next generation non-volatile memory to replace Flash memory.
Now, the uncertainty about the resistive physical mechanism becomes the bottleneck impediment to the development of RRAM. For the device, there are still some aspects that could be enhanced, such as stability, speed and so on. The study on RRAM is mainly based on the experimental research, microstructure characterization and real-time monitoring. It is obvious that the analytical tools above are time and money consuming. In this paper, we adopt first-principle method to have an intense simulation about RRAM device. First, we study the physical mechanism of carrier transportation and storage in the resistive material. Then we discuss the performance improvement by doping, making defect and controlling valence state. Finally, we quantify the correlation between material micro-parameter and RRAM device macroscopic property, thus guiding the design and optimization of RRAM device.
With a comprehensive review of the developments in RRAM research, we have got an overview about RRAM. In this paper, we explore the role of oxygen vacancy (Vo) and doped Ag when conductive filaments form in HfO2. The results show that Vo and Ag can form conductive filaments alone by inducing impurity levels in the gap. Then we study the composite system, i.e. Vo and Ag co-exist in HfO2, it is found that both conductivity and stability are enhanced. At the same concentration, Ag can form filament with the of Hf; however, Vo fails. For the composite system, the performance enhancement benefit from the existence of Vo. One step further, Vo assist Ag to migrate in HfO2, thus improving the conductivity and stability.
Electrode and resistive materials will directly affect the performance of the composite material and the interface is especially crucial to the performance of RRAM device. So we set up different Cu/HfO2interface models and compare their properties. The results show that different interface will have a great impact on the performance of RRAM devices. For all potential interface models, the mismatch ratio and the interface adhesion energy implying that Cu (111)/HfO2(010) is the most stable. Furthermore, Cu(111)/HfO2(010) is the only case that can form connective electronic channel along the vertical direction of the Cu electrode. And the electrons transfer mutually and bond at Cu(111)/HfO2(010) interface indicate that electrons possess the localizability and connectivity along the direction, which corresponds to the switching-on direction of the RRAM device. For Cu(111)/HfO2(010), we research the impact of electrode material on the interface and resistive material. The results show that the closer Cu or Vo defect is to the interface, the easier it is to form. And Cu atoms can migrate into HfO2more easily. This indicates that the electrochemical reaction takes place more easily under the biased voltage, resulting in the formation and rupture of Cu conductive filaments.
The fact that doping can improve the electrical characteristics of metal oxide resistive materials is widely understood. But the effects of the defect valence state are still unknown. Therefore, we pay a close attention to the defect valence state in HfO2. Firstly, based on the analysis of electron affinity and formation energy, we grasp the gain and loss of electrons in the doped element; secondly, we focus on the electrons location by charge density difference and modified Bader charge. Finally, we draw an instructional conclusion about the influence of different valence state on the performance of resistive material.
The results will provide theoretical guidance to design and improve the performances of RRAM devices. It definitely will help to understand and develop RRAM toward a higher stage.
目前,制约RRAM技术发展和应用的主要瓶颈之一是发生电阻转变效应的物理机制、电荷存储机理尚不明确,同时,RRAM器件在稳定性、均匀性、可重复性、擦写速度以及数据保持性等方面都还存在问题,而目前对器件的研究主要是通过实验研制、显微表征及实时监测基础上进行观察和分析,存在实验平台要求高、表征和测试仪器高端、实验周期长等问题。针对上述问题,本论文结合并行计算与第一性原理开展多层次、多维度的模拟手段,从物理角度解释载流子的输运过程和存储机理,通过掺杂、制造缺陷和控制化合价等手段对阻变材料进行改性,给出材料的微观参数和存储器的宏观电学量的定量关系,为RRAM的优化设计及可靠集成提供理论指导和设计工具。
针对RRAM的研究现状进行统计,了解其阻变的宏观特性等方面的不足,研究了纳米尺度下RRAM二元金属氧化物阻变材料HfO2的氧空位(Vo)陷阱效应、掺杂效应(Ag)等对器件特性的影响以及阻变存储器的微观阻变机理。研究表明单独Vo缺陷和单独Ag杂质均可以在禁带中引入杂质能级,且都分别可以形成导电细丝；针对Vo和Ag都能形成导电细丝的情况,研究了Ag和Vo共掺杂的复合缺陷体系,结果表明共掺杂体系的导电性能增强、稳定性更好；而在相同浓度下,Ag杂质能级能够通过Ag离子的作用加以Hf离子的辅助下形成导电细丝,而Vo缺陷能级没有导电细丝的形成。且在Vo存在的前提下,Ag离子的迁移将变得更加容易,即Vo可以辅助Ag离子迁移,增强了体系电化学性能。
电极以及阻变材料的选择将直接影响着复合材料的性能,其界面结合的状态对整个阻变存储器的性能起着至关重要的作用,对比研究了Cu/HfO2不同切面组合的复合材料界面模型。结果表明,复合材料的界面不同,对RRAM器件的性能会产生很大影响。在研究的所有界面体系中,Cu(111)/HfO2(010)失配率最小,界面束缚能最大,界面体系相对最稳定；且只有Cu(111)/HfO2(010)复合材料体系出现了垂直Cu电极方向完整连通的电子通道,界面处有电子的相互转移、成键的存在,表明电子在此方向上具有局域性、连通性,与阻变存储器(RRAM)器件导通方向一致。针对Cu(111)/HfO2(010)复合材料界面体系,探讨了其整体性能,并研究了电极对界面处及阻变材料的影响。研究表明越靠近界面处,Cu和Vo缺陷越容易形成和存在,Cu原子越容易进入HfO2体内,也即Cu将呈阶梯状往HfO2内部扩散以形成缺陷体系,在外加电压下易发生电化学反应,从而导致Cu导电细丝的形成与断裂,更有利于RRAM器件电阻开关特性的产生。
对二元金属氧化物阻变材料进行掺杂可以改变其存储特性、电学特性,而对于掺杂元素进入材料体内后所具有的价电子数或化合价态的研究较少,鉴于此,研究了掺杂金属元素进入阻变材料后是否具有化合价态以及不同化合价态对阻变存储器材料性能的影响,首先通过电子亲和能以及缺陷形成能确定掺杂元素得失电子情况；其次通过差分电荷密度和修正的Bader分析确定了得失电子的具体位置；最后系统研究了掺杂元素具有不同化合价态对RRAM阻变材料及其性能的影响。
结果将为RRAM存储器的制备及性能提高提供理论指导和设计工具,必将在更深层次上理解和发展RRAM起到关键作用。
With the development of semiconductor technology node, the Flash memory confronts many problems, such as the coupling between floating gates, charge leakage, cross-coupling between cells and so on. Therefore, it is essential to explore the next generation of non-volatile memory. At present, the explorations mainly concentrate on the followings:phase random access memory (PRAM), magnetic random access memory (MRAM), ferroelectric random access memory (FRAM) and resistive random access memory (RRAM). Moreover, due to the advantages including simple structure, low power consumption, high density, fast program/erase speed and compatibility with CMOS technology, RRAM is regard as the most promising candidate for the next generation non-volatile memory to replace Flash memory.
Now, the uncertainty about the resistive physical mechanism becomes the bottleneck impediment to the development of RRAM. For the device, there are still some aspects that could be enhanced, such as stability, speed and so on. The study on RRAM is mainly based on the experimental research, microstructure characterization and real-time monitoring. It is obvious that the analytical tools above are time and money consuming. In this paper, we adopt first-principle method to have an intense simulation about RRAM device. First, we study the physical mechanism of carrier transportation and storage in the resistive material. Then we discuss the performance improvement by doping, making defect and controlling valence state. Finally, we quantify the correlation between material micro-parameter and RRAM device macroscopic property, thus guiding the design and optimization of RRAM device.
With a comprehensive review of the developments in RRAM research, we have got an overview about RRAM. In this paper, we explore the role of oxygen vacancy (Vo) and doped Ag when conductive filaments form in HfO2. The results show that Vo and Ag can form conductive filaments alone by inducing impurity levels in the gap. Then we study the composite system, i.e. Vo and Ag co-exist in HfO2, it is found that both conductivity and stability are enhanced. At the same concentration, Ag can form filament with the of Hf; however, Vo fails. For the composite system, the performance enhancement benefit from the existence of Vo. One step further, Vo assist Ag to migrate in HfO2, thus improving the conductivity and stability.
Electrode and resistive materials will directly affect the performance of the composite material and the interface is especially crucial to the performance of RRAM device. So we set up different Cu/HfO2interface models and compare their properties. The results show that different interface will have a great impact on the performance of RRAM devices. For all potential interface models, the mismatch ratio and the interface adhesion energy implying that Cu (111)/HfO2(010) is the most stable. Furthermore, Cu(111)/HfO2(010) is the only case that can form connective electronic channel along the vertical direction of the Cu electrode. And the electrons transfer mutually and bond at Cu(111)/HfO2(010) interface indicate that electrons possess the localizability and connectivity along the direction, which corresponds to the switching-on direction of the RRAM device. For Cu(111)/HfO2(010), we research the impact of electrode material on the interface and resistive material. The results show that the closer Cu or Vo defect is to the interface, the easier it is to form. And Cu atoms can migrate into HfO2more easily. This indicates that the electrochemical reaction takes place more easily under the biased voltage, resulting in the formation and rupture of Cu conductive filaments.
The fact that doping can improve the electrical characteristics of metal oxide resistive materials is widely understood. But the effects of the defect valence state are still unknown. Therefore, we pay a close attention to the defect valence state in HfO2. Firstly, based on the analysis of electron affinity and formation energy, we grasp the gain and loss of electrons in the doped element; secondly, we focus on the electrons location by charge density difference and modified Bader charge. Finally, we draw an instructional conclusion about the influence of different valence state on the performance of resistive material.
The results will provide theoretical guidance to design and improve the performances of RRAM devices. It definitely will help to understand and develop RRAM toward a higher stage.
引文
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