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Operando Spectroscopic Investigation of the Valence Change Mechanism in La2NiO4+δ -Based Memristive Devices
Advanced Electronic Materials ( IF 5.3 ) Pub Date : 2024-07-04 , DOI: 10.1002/aelm.202400313 Thoai‐Khanh Khuu 1, 2 , Aleksandra Koroleva 1, 3 , Carlos Moncasi 1 , Alexander Stangl 1 , David Cooper 4 , Gauthier Lefèvre 2 , Fabrice Wilhelm 5 , Andrei Rogalev 5 , Matthieu Weber 1 , Carmen Jiménez 1 , Mónica Burriel 1
Advanced Electronic Materials ( IF 5.3 ) Pub Date : 2024-07-04 , DOI: 10.1002/aelm.202400313 Thoai‐Khanh Khuu 1, 2 , Aleksandra Koroleva 1, 3 , Carlos Moncasi 1 , Alexander Stangl 1 , David Cooper 4 , Gauthier Lefèvre 2 , Fabrice Wilhelm 5 , Andrei Rogalev 5 , Matthieu Weber 1 , Carmen Jiménez 1 , Mónica Burriel 1
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Valence change memory devices, based on redox reactions and oxygen dynamics, are considered to be one of the most promising candidates for the next generation of non-volatile memory devices and neuromorphic architectures. Devices based on La2NiO4+δ have demonstrated analog resistive switching behavior, but the underlying mechanism is not fully understood. To get a profound understanding of the device's behavior, the employment of element-selective techniques to provide direct information on oxygen migration is of paramount importance. In this work, TiN/La2NiO4+δ/Pt devices are studied using an original operando X-ray absorption near edge spectroscopy (XANES) methodology based on monitoring absorbance intensity changes at a fixed energy position which, in combination with in situ electron energy-loss spectroscopy (EELS) measurements, has provided valuable insights into the resistive switching mechanism. This approach allows to study the formation of the TiNxOy interlayer at the TiN/La2NiO4+δ interface and directly monitor oxygen migration between TiNxOy and La2NiO4+δ. An energy shift of the Ni K-edge spectra is consistently measured during the device operation as it underwent cycling in both voltage polarities, thus confirming the pivotal role of the valence change mechanism in the resistive switching behavior of these devices. Furthermore, a switching model based on the coexistence of filamentary and interfacial switching is proposed.
中文翻译：
La2NiO4+δ 忆阻器件价态变化机制的原位光谱研究
基于氧化还原反应和氧动力学的价态变化存储器件被认为是下一代非易失性存储器件和神经形态架构最有前途的候选器件之一。基于La 2 NiO 4+δ的器件已经展示了模拟电阻开关行为，但其基本机制尚不完全清楚。为了深入了解设备的行为，采用元素选择技术来提供有关氧迁移的直接信息至关重要。在这项工作中，TiN/La 2 NiO 4+δ /Pt 器件采用原始操作 X 射线吸收近边光谱 (XANES) 方法进行研究，该方法基于监测固定能量位置处的吸收强度变化，并结合原位电子能量损失光谱（EELS）测量为电阻开关机制提供了宝贵的见解。该方法可以研究TiN/La 2 NiO 4+δ界面处TiN x O y中间层的形成，并直接监测TiN x O y和La 2 NiO 4+δ之间的氧迁移。当 Ni K 边光谱在两种电压极性下经历循环时，在器件运行过程中始终测量到 Ni K 边光谱的能量变化，从而证实了价态变化机制在这些器件的电阻开关行为中的关键作用。此外，提出了一种基于丝状和界面切换共存的切换模型。
更新日期：2024-07-04
中文翻译：
La2NiO4+δ 忆阻器件价态变化机制的原位光谱研究
基于氧化还原反应和氧动力学的价态变化存储器件被认为是下一代非易失性存储器件和神经形态架构最有前途的候选器件之一。基于La 2 NiO 4+δ的器件已经展示了模拟电阻开关行为，但其基本机制尚不完全清楚。为了深入了解设备的行为，采用元素选择技术来提供有关氧迁移的直接信息至关重要。在这项工作中，TiN/La 2 NiO 4+δ /Pt 器件采用原始操作 X 射线吸收近边光谱 (XANES) 方法进行研究，该方法基于监测固定能量位置处的吸收强度变化，并结合原位电子能量损失光谱（EELS）测量为电阻开关机制提供了宝贵的见解。该方法可以研究TiN/La 2 NiO 4+δ界面处TiN x O y中间层的形成，并直接监测TiN x O y和La 2 NiO 4+δ之间的氧迁移。当 Ni K 边光谱在两种电压极性下经历循环时，在器件运行过程中始终测量到 Ni K 边光谱的能量变化，从而证实了价态变化机制在这些器件的电阻开关行为中的关键作用。此外，提出了一种基于丝状和界面切换共存的切换模型。
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