National Institute of Standards and Technology , Gaithersburg , Maryland 20899 , United States.
Oak Ridge National Laboratory , Oak Ridge , Tennessee 37831 , United States.
ACS Appl Mater Interfaces. 2018 Jul 11;10(27):23187-23197. doi: 10.1021/acsami.8b03726. Epub 2018 Jun 29.
The distribution of tantalum and oxygen ions in electroformed and/or switched TaO -based resistive switching devices has been assessed by high-angle annular dark-field microscopy, X-ray energy-dispersive spectroscopy, and electron energy-loss spectroscopy. The experiments have been performed in the plan-view geometry on the cross-bar devices producing elemental distribution maps in the direction perpendicular to the electric field. The maps revealed an accumulation of +20% Ta in the inner part of the filament with a 3.5% Ta-depleted ring around it. The diameter of the entire structure was approximately 100 nm. The distribution of oxygen was uniform with changes, if any, below the detection limit of 5%. We interpret the elemental segregation as due to diffusion driven by the temperature gradient, which in turn is induced by the spontaneous current constriction associated with the negative differential resistance-type I- V characteristics of the as-fabricated metal/oxide/metal structures. A finite-element model was used to evaluate the distribution of temperature in the devices and correlated with the elemental maps. In addition, a fine-scale (∼5 nm) intensity contrast was observed within the filament and interpreted as due phase separation of the functional oxide in the two-phase composition region. Understanding the temperature-gradient-induced phenomena is central to the engineering of oxide memory cells.
采用高角度环形暗场显微镜、X 射线能量色散谱和电子能量损失谱评估了电成型和/或切换 TaO 基电阻开关器件中钽和氧离子的分布。在叉指器件的平面视图几何形状上进行了实验,在垂直于电场的方向上产生元素分布图。这些图揭示了在丝的内部有一个+20% Ta 的积累,周围有一个 3.5% Ta 耗尽的环。整个结构的直径约为 100nm。氧的分布是均匀的,如果有任何变化,其变化也低于 5%的检测限。我们将元素偏析解释为温度梯度驱动的扩散,而温度梯度反过来又是由与所制备的金属/氧化物/金属结构的负微分电阻型 I-V 特性相关的自发电流收缩引起的。使用有限元模型来评估器件中的温度分布,并与元素图相关联。此外,在丝内观察到精细尺度(约 5nm)的强度对比度,并解释为在两相组成区域中功能氧化物的相分离。理解温度梯度诱导的现象对于氧化物存储单元的工程设计至关重要。