阐明用于阻变开关器件的非晶锂镧钛氧化物中的动态导电态变化
Elucidating Dynamic Conductive State Changes in Amorphous Lithium Lanthanum Titanate for Resistive Switching Devices
AI总结：
本文通过电压扫描、FIB-SEM原位偏置及成分实验与计算，揭示a-LLTO因Ti还原形成双导电态并产生导电细丝，在-3.5至3.5 V窗口实现三个数量级稳定阻变。
摘要：
探索新型阻变开关材料引起了人们的关注，其目的是取代传统的硅基晶体管，并实现能够在物联网（IoT）时代超越当前冯·诺依曼计算限制的神经形态计算。先前用于电池的材料已经证明，由于电偏置引起的成分变化，它们会在电偏置下发生金属-绝缘体转变。这一特性正是未来阻变开关器件所需要的。非晶锂镧钛氧化物（a-LLTO）最初是作为固态电解质开发的，在氧化物型固态电解质中具有相对较高的锂离子电导率和较低的电子电导率。然而，已有研究表明，a-LLTO的电导率会随氧含量而变化。在本工作中，通过采用一系列电压扫描技术对a-LLTO的开关行为进行了研究，最终在-3.5 V至3.5 V的电压窗口内建立了稳定且最佳的工作条件。该电压范围有效地平衡了实现三个数量级显著电阻变化的理想特性与避免LLTO分解的必要要求。这种开关行为还通过聚焦离子束/扫描电子显微镜（FIB-SEM）中的原位偏置，在Ni/LLTO/Ni纳米器件上得到证实。针对不同LLTO成分的实验和计算表明，由于Ti的还原，LLTO具有两种不同的导电态。本文使用简化的二元模型讨论了这两种状态的分布，暗示低阻态期间存在导电细丝生长。因此，我们的研究加深了对LLTO电子性质的理解，并推动了电池材料在阻变开关器件中的跨学科应用。
英文摘要：
Exploration of novel resistive switching materials attracts attention to replace conventional Si-based transistors and to achieve neuromorphic computing that can surpass the limit of the current Von-Neumann computing for the time of Internet of Things (IoT). Materials priorly used to serve in batteries have demonstrated metal-insulator transitions upon an electrical biasing due to resulting compositional change. This property is desirable for future resistive switching devices. Amorphous lithium lanthanum titanate (a-LLTO) was originally developed as a solid-state electrolyte with relatively high lithium ionic conductivity and low electronic conductivity among oxide-type solid electrolytes. However, it has been suggested that electric conductivity of a-LLTO changes depending on oxygen content. In this work, the investigation of switching behavior of a-LLTO was conducted by employing a range of voltage sweep techniques, ultimately establishing a stable and optimal operating condition within the voltage window of -3.5 V to 3.5 V. This voltage range effectively balances the desirable trait of a substantial resistance change by three orders of magnitude with the imperative avoidance of LLTO decomposition. This switching behavior is also confirmed at nanodevice of Ni/LLTO/Ni through in-situ biasing inside focused-ion beam/scanning electron microscope (FIB-SEM). Experiment and computation with different LLTO composition shows that LLTO has two distinct conductivity states due to Ti reduction. The distribution of these two states is discussed using simplified binary model, implying the conductive filament growth during low resistance state. Consequently, our study deepens understanding of LLTO electronic properties and encourages the interdisciplinary application of battery materials for resistive switching devices.
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