Reversible redox reactions in an epitaxially stabilized SrCoO(x) oxygen sponge.

Fast, reversible redox reactions in solids at low temperatures without thermomechanical degradation are a promising strategy for enhancing the overall performance and lifetime of many energy materials and devices. However, the robust nature of the cation's oxidation state and the high thermodynamic barrier have hindered the realization of fast catalysis and bulk diffusion at low temperatures. Here, we report a significant lowering of the redox temperature by epitaxial stabilization of strontium cobaltites (SrCoO(x)) grown directly as one of two distinct crystalline phases, either the perovskite SrCoO(3-δ) or the brownmillerite SrCoO(2.5). Importantly, these two phases can be reversibly switched at a remarkably reduced temperature (200-300 °C) in a considerably short time (< 1 min) without destroying the parent framework. The fast, low-temperature redox activity in SrCoO(3-δ) is attributed to a small Gibbs free-energy difference between two topotatic phases. Our findings thus provide useful information for developing highly sensitive electrochemical sensors and low-temperature cathode materials.

Spontaneous vortex nanodomain arrays at ferroelectric heterointerfaces.

The polarization of the ferroelectric BiFeO(3) sub-jected to different electrical boundary conditions by heterointerfaces is imaged with atomic resolution using a spherical aberration-corrected transmission electron microscope. Unusual triangular-shaped nanodomains are seen, and their role in providing polarization closure is understood through phase-field simulations. Heterointerfaces are key to the performance of ferroelectric devices, and this first observation of spontaneous vortex nanodomain arrays at ferroelectric heterointerfaces reveals properties unlike the surrounding film including mixed Ising-Néel domain walls, which will affect switching behavior, and a drastic increase of in-plane polarization. The importance of magnetization closure has long been appreciated in multidomain ferromagnetic systems; imaging this analogous effect with atomic resolution at ferroelectric heterointerfaces provides the ability to see device-relevant interface issues. Extension of this technique to visualize domain dynamics is envisioned.

Sketched oxide single-electron transistor.

Devices that confine and process single electrons represent an important scaling limit of electronics. Such devices have been realized in a variety of materials and exhibit remarkable electronic, optical and spintronic properties. Here, we use an atomic force microscope tip to reversibly 'sketch' single-electron transistors by controlling a metal-insulator transition at the interface of two oxides. In these devices, single electrons tunnel resonantly between source and drain electrodes through a conducting oxide island with a diameter of ∼1.5 nm. We demonstrate control over the number of electrons on the island using bottom- and side-gate electrodes, and observe hysteresis in electron occupation that is attributed to ferroelectricity within the oxide heterostructure. These single-electron devices may find use as ultradense non-volatile memories, nanoscale hybrid piezoelectric and charge sensors, as well as building blocks in quantum information processing and simulation platforms.

Domain dynamics during ferroelectric switching.

The utility of ferroelectric materials stems from the ability to nucleate and move polarized domains using an electric field. To understand the mechanisms of polarization switching, structural characterization at the nanoscale is required. We used aberration-corrected transmission electron microscopy to follow the kinetics and dynamics of ferroelectric switching at millisecond temporal and subangstrom spatial resolution in an epitaxial bilayer of an antiferromagnetic ferroelectric (BiFeO(3)) on a ferromagnetic electrode (La(0.7)Sr(0.3)MnO(3)). We observed localized nucleation events at the electrode interface, domain wall pinning on point defects, and the formation of ferroelectric domains localized to the ferroelectric and ferromagnetic interface. These results show how defects and interfaces impede full ferroelectric switching of a thin film.