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Register a new userOxygen annealing induced changes in defects within beta-Ga2O3 epitaxial films measured using photoluminescence
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In this work, we use photoluminescence spectroscopy (PL) to monitor changes in the UV, UV, blue, and green emission bands from n-type (010) Ga2O3 films grown by metalorganic vapor phase epitaxy (MOVPE) induced by annealing at different temperatures under O2 ambient. Annealing at successively higher temperatures decreases the overall PL yield and UV intensity at nearly the same rates, indicating the increase in formation of at least one non-radiative defect type. Simultaneously, the PL yield ratios of blue/UV and green/UV increase, suggesting that defects associated with these emissions increase in concentration with O2 annealing. Utilizing the different absorption coefficients of 240 and 266 nm polarization-dependent excitation, we find an overall activation energy for the generation of non-radiative defects of 0.69 eV in the bulk but 1.55 eV near the surface. We also deduce activation energies for the green emission-related defects of 0.60 eV near the surface and 0.89-0.92 eV through the films, whereas the blue-related defects have activation energy in the range 0.43-0.62 eV for all depths. Lastly, we observe hillock surface morphologies and Cr diffusion from the substrate into the film for temperatures above 1050 oC. These observations are consistent with the formation and diffusion of VGa and its complexes as a dominant process during O2 annealing, but further work will be necessary to determine which defects and complexes provide radiative and non-radiative recombination channels and the detailed kinetic processes occurring at surfaces and in bulk amongst defect populations.
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The ability to manipulate oxygen anion defects rather than metal cations in complex oxides can facilitate creating new functionalities critical for emerging energy and device technologies. However, the difficulty in activating oxygen at reduced temperatures hinders the deliberate control of important defects, oxygen vacancies. Here, strontium cobaltite (SrCoOx) is used to demonstrate that epitaxial strain is a powerful tool for manipulating the oxygen vacancy concentration even under highly oxidizing environments and at annealing temperatures as low as 300 C. By applying a small biaxial tensile strain (2%), the oxygen activation energy barrier decreases by ~30%, resulting in a tunable oxygen deficient steady-state under conditions that would normally fully oxidize unstrained cobaltite. These strain-induced changes in oxygen stoichiometry drive the cobaltite from a ferromagnetic metal towards an antiferromagnetic insulator. The ability to decouple the oxygen vacancy concentration from its typical dependence on the operational environment is useful for effectively designing oxides materials with a specific oxygen stoichiometry.
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.
We report on the non-destructive measurement of Youngs modulus of thin-film single crystal beta gallium oxide (beta-Ga2O3) out of its nanoscale mechanical structures by measuring their fundamental mode resonance frequencies. From the measurements, we extract Youngs modulus in (100) plane, EY,(100) = 261.4+/-20.6 GPa, for beta-Ga2O3 nanoflakes synthesized by low-pressure chemical vapor deposition (LPCVD), and Youngs modulus in [010] direction, EY,[010] = 245.8+/-9.2 GPa, for beta-Ga2O3 nanobelts mechanically cleaved from bulk beta-Ga2O3 crystal grown by edge-defined film-fed growth (EFG) method. The Youngs moduli extracted directly on nanomechanical resonant device platforms are comparable to theoretical values from first-principle calculations and experimentally extracted values from bulk crystal. This study yields important quantitative nanomechanical properties of beta-Ga2O3 crystals, and helps pave the way for further engineering of beta-Ga2O3 micro/nanoelectromechanical systems (M/NEMS) and transducers.
The effects of hydrogen incorporation into beta-Ga2O3 thin films have been investigated by chemical, electrical and optical characterization techniques. Hydrogen incorporation was achieved by remote plasma doping without any structural alterations of the film; however, X-ray photoemission reveals major changes in the oxygen chemical environment. Depth-resolved cathodoluminescence (CL) reveals that the near-surface region of the H-doped Ga2O3 film exhibits a distinct red luminescence (RL) band at 1.9 eV. The emergence of the H-related RL band is accompanied by an enhancement in the electrical conductivity of the film by an order of magnitude. Temperature-resolved CL points to the formation of abundant H-related donors with a binding energy of 28 +/- 4 meV. The RL emission is attributed to shallow donor-deep acceptor pair recombination, where the acceptor is a VGa-H complex and the shallow donor is interstitial H. The binding energy of the VGa-H complex, based on our experimental considerations, is consistent with the computational results by Varley et al [J. Phys.: Condens. Matter, 23, 334212, 2011].
The interrelation between the epitaxial strain and oxygen deficiency in La0.7Ca0.3MnO3-{delta} thin films was studied in terms of structural and functional properties. The films with a thickness of 1000{AA} were prepared using a PLD system equipped with a RHEED facility and a pyrometric film temperature control. The epitaxial strain and the oxygen deficiency in the samples were systematically modified using three different substrates: SrTiO3, (LaAlO3)0.3-(Sr2AlTaO6)0.7 and LaSrAlO4, and four different oxygen pressures during film growth ranging from 0.27mbar to 0.1mbar. It could be demonstrated that the oxygen incorporation depends on the epitaxial strain: oxygen vacancies were induced to accommodate tensile strain whereas the compressive strain suppressed the generation of oxygen vacancies.
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