导电细丝的形成与断裂是氧化还原类忆阻器实现0-1存储的内在机制。因此，通过调控离子输运行为和导电细丝生长与演化过程是忆阻器研究的核心问题。本文围绕新型存储所追求的“高密度、高能效、多功能”目标，通过对导电细丝生长的位置、形态、成分等方面的多维度调控，探索材料选择与器件设计对电学性能的操控，进而构建出有实用化前景的忆阻器。利用纳米压痕技术制备了Ag/SiO2/Pt和W/TaOx/Pt器件，采用物理方法实现了尖端电极产生集中电场对导电细丝生长位置的精准调控。利用双层膜结构制备了Ag/TaOx/TaOy/Pt器件，证明了多层膜结构对于阳离子迁移的限制作用，实现了导电细丝的自我精准调控。通过对导电细丝生长位置的调控有效地提升了忆阻器的综合性能，尤其是均一性。利用完全对称的三层膜结构开发了Ag/TaOx/TaOz/TaOx/Ag器件，在介质层中形成了沙漏形的导电细丝，提升了氧化钽基忆阻器作为选通器的工作电流至1mA。利用部分掺杂活性金属方法开发了Pt/TaOx:Ag/TaOx/Pt器件，形成了纳米团簇型导电细丝，降低了氧化钽基忆阻器作为存储器的工作电流至1μA。二者工作电流范围实现了3个数量级的匹配，一定程度上打破了阳离子迁移型忆阻器中经典的“电流-保持特性”困局。通过对导电细丝生长形态的调控开发出能够面向高密度和高能效存储的选通器和存储器。制备了Ag/CH3NH3PbI3/FTO忆阻器，通过薄膜厚度的改变实现了金属型（厚度为90nm）和空位缺陷型（150nm及以上）导电细丝的转换，建立双导电细丝模型阐明了甲胺铅碘忆阻器的忆阻机制。同时利用该材料与光的耦合作用在碘空位导电细丝的体系中实现了光学的非易失RESET操作。通过对导电细丝组成成分的调控实现了忆阻器多功能化的拓展。从介质层材料选择的角度，阐明了导电细丝的生长模式、鲁棒性和长度分别取决于介质层中阳离子迁移与形核过程、薄膜致密程度和薄膜厚度。从电极相关器件结构的角度，区分了单侧活性电极体系Ag/HfOx/Pt中不同初始化过程对于操作模式的影响，利用双侧活性电极结构开发的Ag/Li4Ti5O12/Ag忆阻器保证了双向开关的选通器操作。同时利用单侧活性电极、不同生长模式的双层膜介质开发了Ag/SiO2/TaOx/Pt忆阻器，可作为双极性自选择忆阻器应用于高密度集成阵列。
The formation and rupture of conductive filaments are the key mechanism of 0-1 storage in redox-based memristors. Therefore, modulating ion transport and the growth and evolution of conductive filaments is the core problem of memristor research. Focusing on the goal of "high-density, high-energy-efficiency and multi-function" pursued by the emerging memory technology, this dissertation explores the control of electrical performance by material selection and device design through multi-dimensional regulation of the filament growth including the position, morphology and composition, and then constructs a series of promising memristors.We proposed Ag/SiO2/Pt and W/TaOx/Pt memristors decorated by nano-indentation technology. The precise control of the filament growth position was realized by the fully physical method. The Ag/TaOx/TaOy/Pt memristor was fabricated by using a bi-layer dielectric, which proved that the multi-layer structure could limit the cation migration and realize the self- regulation of conductive filaments. By controlling the filament growth position, the comprehensive performances of the memristor, especially the uniformity, are effectively improved.The Ag/TaOx/TaOz/TaOx/Ag memristor was developed by using a fully symmetrical tri-layer structure. An hourglass-shaped filament was generated and the operation current of the tantalum oxide-based memristor as a selector was increased to 1 mA. The Pt/TaOx:Ag/TaOx/Pt memristor was developed by a partially active-metal-doping method. A nano-cluster filament was formed and the operating current of tantalum oxid-based memristors as a memory was reduced to 1 μA. The operation current ranges of the two devices match by three orders of magnitude, which breaks the classic "current-retention" dilemma in cation-based memristors to a certain extent. By regulating the filament morphology, the proposed selector and memory devices can be used for high-density and high-energy-efficiency information storage is developed.The conversion between metallic filaments and vacancy defect filaments in the proposed Ag/CH3NH3PbI3/FTO memristor was realized by changing the thickness of the dielectric film. A double filament model was established to illuminate the underlying mechanism of the CH3NH3PbI3-based memristors. The light-coupling effect of CH3NH3PbI3 was used to realize the optical non-volatile RESET operation in the iodine vacancy filament system. By modulating the filament composition, the multifunction of memristors is extended.In the aspect of dielectric material selection, the growth mode, robustness and length of filaments are mainly determined by the cation migration and nucleation process, the compactness and the film thickness. In the aspect of electrode-related structure, the effect of different electro-forming processes on the operation mode was differentiated in the uni-side active electrode system Ag/HfOx/Pt. The dual-side active electrode structure of Ag/Li4Ti5O12/Ag ensured the selector application of bidirectional switches. The Ag/SiO2/TaOx/Pt memristor was developed by using a uni-side active electrode and a bi-layer dielectric with different growth modes, which could be applied as a bipolar self-selective memristor for high-density integrated crossbar arrays.
