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Register a new userPercolation of Ion-Irradiation-Induced Disorder in Complex Oxide Interfaces
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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.
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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.
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.
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.
A precisely selected elastic strain can be introduced in submicron-thick single-crystal SrTiO3 sheets using a silicon nitride stressor layer. A conformal stressor layer deposited using plasma-enhanced chemical vapor deposition produces an elastic strain in the sheet consistent with the magnitude of the nitride residual stress. Synchrotron x-ray nanodiffraction reveals that the strain introduced in the SrTiO3 sheets is on the order of 10 4, matching the predictions of an elastic model. This approach to elastic strain sharing in complex oxides allows the strain to be selected within a wide and continuous range of values, an effect not achievable in heteroepitaxy on rigid substrates.
Magneto-ionic control of magnetic properties through ionic migration has shown promise in enabling new functionalities in energy-efficient spintronic devices. In this work, we demonstrate the effect of helium ion irradiation and oxygen implantation on magneto-ionically induced exchange bias effect in Gd/Ni$_{0.33}$Co$_{0.67}$O heterostructures. Irradiation using $He^+$ leads to an expansion of the Ni$_{0.33}$Co$_{0.67}$O lattice due to strain relaxation. At low He+ fluence ($leq$ 2$times$10$^{14}$ ions cm$^{-2}$), the redox-induced interfacial magnetic moment initially increases, owing to enhanced oxygen migration. At higher fluence, the exchange bias is suppressed due to reduction of pinned uncompensated interfacial Ni$_{0.33}$Co$_{0.67}$O spins. For oxygen implanted samples, an initial lattice expansion below a dose of 5$times$10$^{15}$ cm$^{-2}$ is subsequently dominated at higher dose by a lattice contraction and phase segregation into NiO and CoO-rich phases, which in turn alters the exchange bias. These results highlight the possibility of ion irradiation and implantation as an effective means to tailor magneto-ionic effects.
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