Lithium lanthanum titanate (LLTO) is a promising solid state electrolyte for solid state batteries due to its demonstrated high bulk ionic conductivity. However, crystalline LLTO has a relatively low grain boundary conductivity, limiting the overall material conductivity. In this work, we investigate amorphous LLTO (a-LLTO) thin films grown by pulsed laser deposition (PLD). By controlling the background pressure and temperature we are able to optimize the ionic conductivity to 3 × 10 −4 S/cm and electronic conductivity to 5 × 10 −11 S/cm. XRD, TEM, and STEM/EELS analysis confirm that the films are amorphous and indicate that oxygen background gas is necessary during the PLD process to decrease the oxygen vacancy concentration, decreasing the electrical conductivity. Amorphous LLTO is deposited onto high voltage LiNi 0. Next generation lithium-ion batteries will require a broad range of energies to meet the challenges of portable electronic storage from electric vehicles to microelectromechanical systems (MEMS). The cost per Watt-hour of commercial batteries have shown incremental improvement due to better manufacturing design, but drastic increases in energy and power density are needed to satisfy projected demand. 1 Solid-state electrolytes are researched heavily because they have the potential to improve capacity loss, cycle lifetime, operation temperature, and safety. Lithium Phosphorous Oxynitride (LiPON) based thin-film solid-state batteries have excellent cycle life and are currently commercialized.2,3 However, LiPON has a relatively low ionic conductivity (1 × 10 −6 S/cm) and other solid electrolytes have demonstrated conductivity several orders of magnitude higher. 4,5 Lithium lanthanum titanate (LLTO) is a promising solid-state electrolyte due to its high bulk ionic conductivity (∼10 −3 S/cm) at room temperature, negligible electronic conductivity, and high voltage, atmospheric, and temperature stabilities.6-8 Extensive fundamental studies have been carried out to demonstrate this high ionic conductivity, elucidate the crystal structure, and determine the mechanism of lithium ion conduction.9-12 However, there are fundamental impediments to the implementation of crystalline LLTO into an actual device. One key issue is that crystalline LLTO has a relatively low grain boundary ionic conductivity (<10 −5 S/cm), lowering the effective material ionic conductivity. 6 In addition, crystalline LLTO is unstable in contact with lithium metal because lithium will easily insert reducing Ti 4+ to Ti 3+ , thus increasing electronic conductivity.
13,14Fortunately, amorphous LLTO has not only been shown to overcome these barriers, the lower energy constraints of fabricating amorphous LLTO opens up numerous thin film synthesis techniques. Amorphous LLTO thin films have been synthesized by pulsed laser deposition (PLD), RF magnetron sputtering, E-beam evaporation, atomic layer deposition, chemical solution deposition and sol-gel synthesis. [15][16][17][18][19][20][21][22][23][24] Furusawa et al. demonstrated amorphous LL...