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  1. Free, publicly-accessible full text available July 1, 2024
  2. Vertically aligned nanocomposite (VAN) thin films have shown strong potential in oxide nanoionics but are yet to be explored in detail in solid-state battery systems. Their 3D architectures are attractive because they may allow enhancements in capacity, current, and power densities. In addition, owing to their large interfacial surface areas, the VAN could serve as models to study interfaces and solid-electrolyte interphase formation. Here, we have deposited highly crystalline and epitaxial vertically aligned nanocomposite films composed of a Li x La 0.32±0.05 (Nb 0.7±0.1 Ti 0.32±0.05 )O 3±δ -Ti 0.8±0.1 Nb 0.17±0.03 O 2±δ -anatase [herein referred to as LL(Nb, Ti)O-(Ti, Nb)O 2 ] electrolyte/anode system, the first anode VAN battery system reported. This system has an order of magnitude increased Li + ionic conductivity over that in bulk Li 3x La 1/3−x NbO 3 and is comparable with the best available Li 3x La 2/3−x TiO 3 pulsed laser deposition films. Furthermore, the ionic conducting/electrically insulating LL(Nb, Ti)O and electrically conducting (Ti, Nb)O 2 phases are a prerequisite for an interdigitated electrolyte/anode system. This work opens up the possibility of incorporating VAN films into an all solid-state battery, either as electrodes or electrolytes, by the pairing of suitable materials. 
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    Here, in ionically conducting Na 0.5 Bi 0.5 TiO 3 (NBT), we explore the link between growth parameters, stoichiometry and resistive switching behavior and show NBT to be a highly tunable system. We show that the combination of oxygen ionic vacancies and low-level electronic conduction is important for controlling Schottky barrier interfacial switching. We achieve a large ON/OFF ratio for high resistance/low resistance ( R HRS / R LRS ), enabled by an almost constant R HRS of ∼10 9 Ω, and composition-tunable R LRS value modulated by growth temperature. R HRS / R LRS ratios of up to 10 4 and pronounced resistive switching at low voltages (SET voltage of <1.2 V without high-voltage electroforming), strong endurance (no change in resistance states after several 10 3 cycles), uniformity, stable switching and fast switching speed are achieved. Of particular interest is that the best performance is achieved at the lowest growth temperature studied (600 °C), which is opposite to the case of most other perovskite oxides for memristors, where higher growth temperatures are required for optimum performance. This is understood based on the oxygen vacancy control of interfacial switching in NBT, whereas a range of other mechanisms (including filamentary switching) occur in other perovskites. The study of NBT has enabled us to determine key parameters for achieving high performance memristors. 
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