Abstract
AbstractControl of order–disorder phase transitions is a fundamental materials science challenge, underpinning the development of energy storage technologies such as solid oxide fuel cells and batteries, ultra‐high temperature ceramics, and durable nuclear waste forms. At present, the development of promising complex oxides for these applications is hindered by a poor understanding of how interfaces affect lattice disordering processes and defect transport. Here, the evolution of local disorder in ion‐irradiated La2Ti2O7/SrTiO3 thin film heterostructures is explored using a combination of high‐resolution scanning transmission electron microscopy, position‐averaged convergent beam electron diffraction, electron energy loss spectroscopy, and ab initio simulations. Highly non‐uniform lattice disordering driven by asymmetric oxygen vacancy formation across the interface is observed. Theory calculations indicate that this asymmetry results from differences in the polyhedral connectivity and vacancy formation energies of the two interface components, suggesting ways to manipulate lattice disorder in functional oxide heterostructures.
Highlights
Thin film oxide heterostructures have emerged as key enabling technologies for transformative advances in electronics, quantum computing, and energy production
Order-disorder phase transitions are important in A2B2O7 compounds, which have been studied for use in solid oxide fuel cells (SOFCs),[2,3,4] advanced ferroelectric sensors,[5,6] and nuclear waste forms.[7]
Several nominally 50 nm-thick epitaxial La2Ti2O7 thin films were deposited on SrTiO3 (110) substrates using pulsed laser deposition (PLD) and annealed in air,[5] as described in the Methods
Summary
Thin film oxide heterostructures have emerged as key enabling technologies for transformative advances in electronics, quantum computing, and energy production. We examine ion-irradiation-induced disordering of La2Ti2O7 (LTO) / SrTiO3 (STO) interfaces using a combination of aberration-corrected scanning transmission electron microscopy (STEM), position-averaged convergent beam electron diffraction (PACBED), and electron energy loss spectroscopy (STEM-EELS), supported by ab initio simulations.
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