室温下制备非晶ZnO薄膜及其电阻开关特性研究

室温下采用紫外固化的方法取代溶胶-凝胶方法中的高温退火制备了氧化锌薄膜, XRD分析结果表明薄膜为非晶的, XPS分析结果表明薄膜的主要成分是ZnO。在深紫外固化后的薄膜表面溅射Al作为顶电极获得Al/a-ZnO/FTO结构的器件,研究深紫外照射时间对器件电阻转变性能的影响, 进一步解释了深紫外固化的机制。研究表明: 经过充足时间(12 h)照射的器件表现出双极性电阻开关特性,阈值电压分布集中(-3.7 V<V_set<-2.9 V, 3.4 V< V_reset<4.3 V)且符合低电压工作的要求, 至少在4000 s内器件的高低阻态都没有发生明显的退化, 表现出了良好的存储器特性。Al/a-ZnO/FTO器件的这种电阻转变特性可以用空间电荷限制电流传导机制解释。     

Direct Evidence of Lithium Ion Migration in Resistive Switching of Lithium Cobalt Oxide Nanobatteries

Lithium cobalt oxide nanobatteries offer exciting prospects in the field of nonvolatile memories and neuromorphic circuits. However, the precise underlying resistive switching (RS) mechanism remains a matter of debate in two‐terminal cells. Herein, intriguing results, obtained by secondary ion mass spectroscopy (SIMS) 3D imaging, clearly demonstrate that the RS mechanism corresponds to lithium migration toward the outside of the Li_xCoO₂ layer. These observations are very well correlated with the observed insulator‐to‐metal transition of the oxide. Besides, smaller device area experimentally yields much faster switching kinetics, which is qualitatively well accounted for by a simple numerical simulation. Write/erase endurance is also highly improved with downscaling – much further than the present cycling life of usual lithium‐ion batteries. Hence very attractive possibilities can be envisaged for this class of materials in nanoelectronics.     

Collective Control of Potential-Constrained Oxygen Vacancies in Oxide Heterostructures for Gradual Resistive Switching

Filamentary resistive switching in oxides is one of the key strategies for developing next-generation non-volatile memory devices. However, despite numerous advantages, their practical applications in neuromorphic computing are still limited due to non-uniform and indeterministic switching behavior. Given the inherent stochasticity of point defect migration, the pursuit of reliable switching likely demands an innovative approach. Herein, a collective control of oxygen vacancies is introduced in LaAlO₃/SrTiO₃ (LAO/STO) heterostructures to achieve reliable and gradual resistive switching. By exploiting an electrostatic potential constraint in ultrathin LAO/STO heterostructures, the formation of conducting filaments is suppressed, but instead precisely control the concentration of oxygen vacancies. Since the conductance of the LAO/STO device is governed by the ensemble concentration of oxygen vacancies, not their individual probabilistic migrations, the resistive switching is more uniform and deterministic compared to conventional filamentary devices. It provides direct evidence for the collective control of oxygen vacancies by spectral noise analysis and modeling by Monte-Carlo simulation. As a proof of concept, the significantly-improved analog switching performance of the filament-free LAO/STO devices is demonstrated, revealing potential for neuromorphic applications. The results establish an approach to store information by point defect concentration, akin to biological ionic channels, for enhancing switching characteristics of oxide materials.     

Biodegradable Natural Pectin‐Based Flexible Multilevel Resistive Switching Memory for Transient Electronics

Transient electronics that can physically vanish in solution can offer opportunities to address the ecological challenges for dealing with the rapidly growing electronic waste. As one important component, it is desirable that memory devices combined with the transient feature can also be developed as secrecy information storage systems besides the above advantage. Resistive switching (RS) memory is one of the most promising technologies for next‐generation memory. Herein, the biocompatible pectin extracted from natural orange peel is introduced to fabricate RS memory devices (Ag/pectin/indium tin oxides (ITO)), which exhibit excellent RS characteristics, such as forming free characteristic, low operating voltages (≈1.1 V), fast switching speed (<70 ns), long retention time (>10⁴ s), and multilevel RS behaviors. The device performance is not degraded after 10⁴ bending cycles, which will be beneficial for flexible memory applications. Additionally, instead of using acid solution, the Ag/pectin/ITO memory device can be dissolved rapidly in deionized water within 10 min thanks to the good solubility arising from ionization of its carboxylic groups, which shows promising application for green electronics. The present biocompatible memory devices based on natural pectin suggest promising material candidates toward enabling high‐density secure information storage systems applications, flexible electronics, and green electronics.     

PLD法制备TiO2薄膜及电阻转变特性研究

采用脉冲激光沉积法（PLD）,以Pt(111)/Ti/SiO₂/Si为衬底,制备了具有电阻转变特性的TiO₂薄膜.X射线衍射（XRD）分析未发现明显的TiO₂结晶峰,薄膜呈纳米晶或非晶态.扫描电子显微镜（SEM）及原子力显微镜（AFM）分析表明,TiO₂薄膜表面平整、光滑致密.电学测试结果表明,TiO₂薄膜具有明显的单极性电阻转变特性,高低阻态比值达到10⁴.高阻态下薄膜的导电过程可用空间电荷限制电流模型解释,过程中存在软击穿现象.在此基础上,对薄膜中丝导电通道的产生及熔断过程进行了初步分析.     

PLD法制备TiO2薄膜及电阻转变特性研究

采用脉冲激光沉积法（PLD）,以Pt(111)/Ti/SiO₂/Si为衬底,制备了具有电阻转变特性的TiO₂薄膜.X射线衍射（XRD）分析未发现明显的TiO₂结晶峰,薄膜呈纳米晶或非晶态.扫描电子显微镜（SEM）及原子力显微镜（AFM）分析表明,TiO₂薄膜表面平整、光滑致密.电学测试结果表明,TiO₂薄膜具有明显的单极性电阻转变特性,高低阻态比值达到10⁴.高阻态下薄膜的导电过程可用空间电荷限制电流模型解释,过程中存在软击穿现象.在此基础上,对薄膜中丝导电通道的产生及熔断过程进行了初步分析.     

Unraveling the Origin and Mechanism of Nanofilament Formation in Polycrystalline SrTiO3 Resistive Switching Memories

Three central themes in the study of the phenomenon of resistive switching are the nature of the conducting phase, why it forms, and how it forms. In this study, the answers to all three questions are provided by performing switching experiments in situ in a transmission electron microscope on thin films of the model system polycrystalline SrTiO₃. On the basis of high‐resolution transmission electron microscopy, electron‐energy‐loss spectroscopy and in situ current–voltage measurements, the conducting phase is identified to be SrTi₁₁O₂₀. This phase is only observed at specific grain boundaries, and a Ruddlesden–Popper phase, Sr₃Ti₂O₇, is typically observed adjacent to the conducting phase. These results allow not only the proposal that filament formation in this system has a thermodynamic origin—it is driven by electrochemical polarization and the local oxygen activity in the film decreasing below a critical value—but also the deduction of a phase diagram for strongly reduced SrTiO₃. Furthermore, why many conducting filaments are nucleated at one electrode but only one filament wins the race to the opposite electrode is also explained. The work thus provides detailed insights into the origin and mechanisms of filament generation and rupture.     

Resistive Switching Behavior in Ferroelectric Heterostructures

Resistive random‐access memory (RRAM) is a promising candidate for next‐generation nonvolatile random‐access memory protocols. The information storage in RRAM is realized by the resistive switching (RS) effect. The RS behavior of ferroelectric heterostructures is mainly controlled by polarization‐dominated and defect‐dominated mechanisms. Under certain conditions, these two mechanisms can have synergistic effects on RS behavior. Therefore, RS performance can be effectively improved by optimizing ferroelectricity, conductivity, and interfacial structures. Many methods have been studied to improve the RS performance of ferroelectric heterostructures. Typical approaches include doping elements into the ferroelectric layer, controlling the oxygen vacancy concentration and optimizing the thickness of the ferroelectric layer, and constructing an insertion layer at the interface. Here, the mechanism of RS behavior in ferroelectric heterostructures is briefly introduced, and the methods used to improve RS performance in recent years are summarized. Finally, existing problems in this field are identified, and future development trends are highlighted.     

退火温度对TiO2基电阻开关器件性能的影响

采用直流磁控溅射法在n+-Si上制备了TiO2薄膜,采用电子束蒸发镀膜仪在TiO2薄膜上沉积Au电极,获得了Au/TiO2/n+-Si结构的器件.研究了退火温度对薄膜结晶性能及器件电阻开关特性的影响.Au/TiO2/n+-Si结构的器件具有单极性电阻开关特性,置位(set)电压,复位(reset)电压、reset电流及功率的大小随退火温度的不同而不同,并基于灯丝理论对器件的电阻开关效应的工作机理进行了探讨.研究结果表明,500℃退火的器件具有良好的非易失性.器件高低阻态的阻值比大于103,其信息保持特性可达10年之久.在读写次数为100次时,器件仍具有电阻开关效应.     

Filament-Free Bulk Resistive Memory Enables Deterministic Analogue Switching

Digital computing is nearing its physical limits as computing needs and energy consumption rapidly increase. Analogue-memory-based neuromorphic computing can be orders of magnitude more energy efficient at data-intensive tasks like deep neural networks, but has been limited by the inaccurate and unpredictable switching of analogue resistive memory. Filamentary resistive random access memory (RRAM) suffers from stochastic switching due to the random kinetic motion of discrete defects in the nanometer-sized filament. In this work, this stochasticity is overcome by incorporating a solid electrolyte interlayer, in this case, yttria-stabilized zirconia (YSZ), toward eliminating filaments. Filament-free, bulk-RRAM cells instead store analogue states using the bulk point defect concentration, yielding predictable switching because the statistical ensemble behavior of oxygen vacancy defects is deterministic even when individual defects are stochastic. Both experiments and modeling show bulk-RRAM devices using TiO_2-X switching layers and YSZ electrolytes yield deterministic and linear analogue switching for efficient inference and training. Bulk-RRAM solves many outstanding issues with memristor unpredictability that have inhibited commercialization, and can, therefore, enable unprecedented new applications for energy-efficient neuromorphic computing. Beyond RRAM, this work shows how harnessing bulk point defects in ionic materials can be used to engineer deterministic nanoelectronic materials and devices.