论文标题
带有垂直离子传输通道的单晶T-NB2O5薄膜中的Li Iontronics
Li iontronics in single-crystalline T-Nb2O5 thin films with vertical ionic transport channels
论文作者
论文摘要
氧化物多晶型T-NB2O5已经以其大量形式进行了广泛的研究,尤其是用于快速充电电池和电化学(伪)电容器的应用。它的晶体结构具有二维(2D)层具有非常低的空间障碍,可以快速锂离子迁移。但是,自1941年发现以来,单晶薄膜及其电子应用的生长尚未实现,这可能是由于其较大的原晶晶胞以及许多多晶型物的存在。在这里,我们证明了单晶T-NB2O5薄膜的外延生长,对垂直于膜表面的离子传输通道进行了严格的态度。这些垂直的2D通道使我们表明的快速锂离子迁移能够产生巨大的绝缘体 - 金属过渡,其中电阻率由于电子最初空的NB 4D0状态的种群而下降了11个数量级。此外,我们通过全面的原位实验和理论计算揭示了多个未开发的相变,它们在广泛的锂离子浓度上具有不同的晶体和电子结构,从而允许对这些相及其独特的电子特性进行可逆且可重复的操纵。这项工作为使用离子通道及其潜在应用探索新型薄膜铺平了道路。
The niobium oxide polymorph T-Nb2O5 has been extensively investigated in its bulk form especially for applications in fast-charging batteries and electrochemical (pseudo)capacitors. Its crystal structure that has two-dimensional (2D) layers with very low steric hindrance allows for fast Li-ion migration. However, since its discovery in 1941, the growth of single-crystalline thin films and its electronic applications have not yet been realized, likely due to its large orthorhombic unit cell along with the existence of many polymorphs. Here we demonstrate the epitaxial growth of single-crystalline T-Nb2O5 thin films, critically with the ionic transport channels oriented perpendicular to the film's surface. These vertical 2D channels enable fast Li-ion migration which we show gives rise to a colossal insulator-metal transition where the resistivity drops by eleven orders of magnitude due to the population of the initially empty Nb 4d0 states by electrons. Moreover, we reveal multiple unexplored phase transitions with distinct crystal and electronic structures over a wide range of Li-ion concentrations by comprehensive in situ experiments and theoretical calculations, that allow for the reversible and repeatable manipulation of these phases and their distinct electronic properties. This work paves the way to the exploration of novel thin films with ionic channels and their potential applications.