Carta D, Hitchcock A P, Guttmann P, Regoutz A, Khiat A, Serb A, Gupta I, Prodromakis T
Nano Group, Nanofabrication Centre, Electronics and Computer Science, Faculty of Physical Sciences and Engineering, University of Southampton, United Kingdom.
Chemistry and Chemical Biology and Brockhouse Institute for Materials Research, McMaster University, L8S4M1 Hamilton, ON, Canada.
Sci Rep. 2016 Feb 19;6:21525. doi: 10.1038/srep21525.
Reduction in metal-oxide thin films has been suggested as the key mechanism responsible for forming conductive phases within solid-state memory devices, enabling their resistive switching capacity. The quantitative spatial identification of such conductive regions is a daunting task, particularly for metal-oxides capable of exhibiting multiple phases as in the case of TiOx. Here, we spatially resolve and chemically characterize distinct TiOx phases in localized regions of a TiOx-based memristive device by combining full-field transmission X-ray microscopy with soft X-ray spectroscopic analysis that is performed on lamella samples. We particularly show that electrically pre-switched devices in low-resistive states comprise reduced disordered phases with O/Ti ratios around 1.37 that aggregate in a ~100 nm highly localized region electrically conducting the top and bottom electrodes of the devices. We have also identified crystalline rutile and orthorhombic-like TiO2 phases in the region adjacent to the main reduced area, suggesting that the temperature increases locally up to 1000 K, validating the role of Joule heating in resistive switching. Contrary to previous studies, our approach enables to simultaneously investigate morphological and chemical changes in a quantitative manner without incurring difficulties imposed by interpretation of electron diffraction patterns acquired via conventional electron microscopy techniques.
金属氧化物薄膜的还原被认为是在固态存储器件中形成导电相并实现其电阻切换能力的关键机制。对这种导电区域进行定量空间识别是一项艰巨的任务,特别是对于像TiO₂这样能够呈现多种相的金属氧化物而言。在这里,我们通过将全场透射X射线显微镜与对薄片样品进行的软X射线光谱分析相结合,在基于TiO₂的忆阻器件的局部区域中对不同的TiO₂相进行空间分辨和化学表征。我们特别表明,处于低电阻状态的电预切换器件包含O/Ti比约为1.37的还原无序相,这些相聚集在一个~100 nm的高度局部区域中,该区域连接着器件的顶部和底部电极并实现导电。我们还在主要还原区域附近的区域中识别出了结晶金红石相和正交晶系状的TiO₂相,这表明局部温度升高至1000 K,证实了焦耳热在电阻切换中的作用。与先前的研究相反,我们的方法能够以定量方式同时研究形态和化学变化,而不会遇到通过传统电子显微镜技术获取的电子衍射图案解释所带来的困难。