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Control 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 we explore the evolution of local disorder in ion-irradiated La$_2$Ti$_2$O$_7$ / SrTiO$_3$ thin film heterostructures using a combination of high-resolution scanning transmission electron microscopy (STEM), position-averaged convergent beam electron diffraction (PACBED), electron energy loss spectroscopy (STEM-EELS), and textit{ab initio} theory calculations. We observe highly non-uniform lattice disordering driven by asymmetric oxygen vacancy formation across the interface. Our 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.
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Order-disorder processes fundamentally determine the structure and properties of many important oxide systems for energy and computing applications. While these processes have been intensively studied in bulk materials, they are less investigated and understood for nanostructured oxides in highly non-equilibrium conditions. These systems can now be realized through a range of deposition techniques and probed at exceptional spatial and chemical resolution, leading to a greater focus on interface dynamics. Here we survey a selection of recent studies of order-disorder behavior at thin film oxide interfaces, with a particular emphasis on the emergence of order during synthesis and disorder in extreme irradiation environments. We summarize key trends and identify directions for future study in this growing research area.
Mastery of order-disorder processes in highly non-equilibrium nanostructured oxides has significant implications for the development of emerging energy technologies. However, we are presently limited in our ability to quantify and harness these processes at high spatial, chemical, and temporal resolution, particularly in extreme environments. Here we describe the percolation of disorder at the model oxide interface LaMnO$_3$ / SrTiO$_3$, which we visualize during in situ ion irradiation in the transmission electron microscope. We observe the formation of a network of disorder during the initial stages of ion irradiation and track the global progression of the system to full disorder. We couple these measurements with detailed structural and chemical probes, examining possible underlying defect mechanisms responsible for this unique percolative behavior.
Using resonant X-ray spectroscopies combined with density functional calculations, we find an asymmetric bi-axial strain-induced $d$-orbital response in ultra-thin films of the correlated metal LaNiO$_3$ which are not accessible in the bulk. The sign of the misfit strain governs the stability of an octahedral breathing distortion, which, in turn, produces an emergent charge-ordered ground state with an altered ligand-hole density and bond covalency. Control of this new mechanism opens a pathway to rational orbital engineering, providing a platform for artificially designed Mott materials.
Electroluminescence (EL) spectra from hybrid charge transfer excitons at metal oxide/organic type-II heterojunctions exhibit pronounced bias-induced spectral shifts. The reasons for this phenomenon have been discussed controversially and arguments for both electric field-induced effects as well as filling of trap states at the oxide surface have been put forward. Here, we combine the results from EL and photovoltaic measurements to eliminate the disguising effects of the series resistance. For SnOx combined with the conjugated polymer MeLPPP, we find a one-to-one correspondence between the blueshift of the EL peak and the increase of the quasi-Fermi level splitting at the hybrid heterojunction, which we unambiguously assign to state filling. Our data is resembled best by a model considering the combination an exponential density of states with a doped semiconductor.
Here we study the electronic properties of cuprate/manganite interfaces. By means of atomic resolution electron microscopy and spectroscopy, we produce a subnanometer scale map of the transition metal oxidation state profile across the interface between the high $T_c$ superconductor YBa$_2$Cu$_3$O$_{7-delta}$ and the colossal magnetoresistance compound (La,Ca)MnO$_3$. A net transfer of electrons from manganite to cuprate with a peculiar non-monotonic charge profile is observed. Model calculations rationalize the profile in terms of the competition between standard charge transfer tendencies (due to band mismatch), strong chemical bonding effects across the interface, and Cu substitution into the Mn lattice, with different characteristic length scales.
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