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Register a new userControlled oxygen vacancy induced p-type conductivity in HfO{2-x} thin films
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We have synthesized highly oxygen deficient HfO$_{2-x}$ thin films by controlled oxygen engineering using reactive molecular beam epitaxy. Above a threshold value of oxygen vacancies, p-type conductivity sets in with up to 6 times 10^{21} charge carriers per cm3. At the same time, the band-gap is reduced continuously by more than 1 eV. We suggest an oxygen vacancy induced p-type defect band as origin of the observed behavior.
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Solid oxide oxygen ion and proton conductors are a highly important class of materials for renewable energy conversion devices like solid oxide fuel cells. Ba2In2O5 (BIO) exhibits both oxygen ion and proton conduction, in dry and humid environment, respectively. In dry environment, the brownmillerite crystal structure of BIO exhibits an ordered oxygen ion sublattice, which has been speculated to result in anisotropic oxygen ion conduction. The hydrated structure of BIO, however, resembles a perovskite and the protons in it were predicted to be ordered in layers. To complement the significant theoretical and experimental efforts recently reported on the potentially anisotropic conductive properties in BIO, we measure here the proton and oxygen ion conductivity along different crystallographic directions. Using epitaxial thin films with different crystallographic orientations the charge transport for both charge carriers is shown to be anisotropic. The anisotropy of the oxygen ion conduction can indeed be explained through the layered structure of the oxygen sublattice in brownmillerite BIO. The anisotropic proton conduction however, further supports the suggested ordering of the protonic defects in the material. The differences in proton conduction along different crystallographic directions attributed to proton ordering in BIO are of a similar extent as those observed along different crystallographic directions in materials where proton ordering is not present but where protons find preferential conduction pathways through chain-like or layered structures.
A series of electron-doped cuprate La(2-x)CexCuO4 thin films with different thicknesses have been fabricated and their annealing time are adjusted carefully to ensure the highest superconducting transition temperature. The transport measurements indicate that, with the increase of the film thickness (<100 nm), the residual resistivity increases and the Hall coefficient shifts in the negative direction. Further more, the X-ray diffraction data reveal that the c-axis lattice constant c0 increases with the decrease of film thickness. These abnormal phenomena can be attributed to the insufficient oxygen reduction in the thin films. Considering the lattice mismatching in the ab-plane between the SrTiO3 substrates and the films, the compressive stress from the substrates may be responsible for the more difficult reduction of the oxygen in the thin films.
We investigated the unoccupied part of the electronic structure of the oxygen-deficient hafnium oxide (HfO$_{sim1.8}$) using soft x-ray absorption spectroscopy at O $K$ and Hf $N_3$ edges. Band-tail states beneath the unoccupied Hf 5$d$ band are observed in the O $K$-edge spectra; combined with ultraviolet photoemission spectrum, this indicates the non-negligible occupation of Hf 5$d$ state. However, Hf $N_3$-edge magnetic circular dichroism spectrum reveals the absence of a long-range ferromagnetic spin order in the oxide. Thus the small amount of $d$ electron gained by the vacancy formation does not show inter-site correlation, contrary to a recent report [M. Venkatesan {it et al.}, Nature {bf 430}, 630 (2004)].
In oxide epitaxy, the growth temperature and background oxygen partial pressure are considered as the most critical factors that control the phase stability of an oxide thin film. Here, we report an unusual case wherein diffusion of oxygen vacancies from the substrate overpowers the growth temperature and oxygen partial pressure to deterministically influence the phase stability of $Bi_{2}WO_{6}$ thin film grown by the pulsed laser deposition technique. We show that when grown on an oxygen-deficient $SrTiO_{3}$ substrate, the $Bi_{2}WO_{6}$ film exhibits a mixture of (001) and (100)/(010)-oriented domains alongside (001)-oriented impurity $WO_{3}$ phases. The (100)/(010)-oriented $Bi_{2}WO_{6}$ phases form a self-organized 3D nanopillar-structure, yielding a very rough film surface morphology. Oxygen annealing of the substrate or using a few monolayer-thick $SrRuO_{3}$ as the blocking layer for oxygen vacancy diffusion enables growing high-quality single-crystalline $Bi_{2}WO_{6}$ (001) thin film exhibiting an atomically smooth film surface with step-terrace structure. We propose that the large oxide-ion conductivity of $Bi_{2}WO_{6}$ facilitates diffusion of oxygen vacancies from the substrate during the film growth, accelerating the evaporation of volatile Bismuth (Bi), which hinders the epitaxial growth. Our work provides a general guideline for high-quality thin film growth of Aurivillius compounds and other oxide-ion conductors containing volatile elements.
Epitaxial thin films of hexagonal ErMnO3 fabricated on Pt(111)/Al2O3(0001) and YSZ(111) substrates exhibited both ferroelectric character and magnetic ordering at low temperatures. As the temperature was reduced, the ErMnO3 films first showed antiferromagnetism. At lower temperatures, the films deposited at lower oxygen partial pressures exhibited spin glass behavior. This re-entrant spin glass behavior was attributed to competition between an antiferromagnetic interaction in the hexagonal geometry and a ferromagnetic interaction caused by a change in Mn valence induced by excess electrons from the oxygen vacancies.
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