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Ultra-wide bandgap, conductive, high mobility, and high quality melt-grown bulk ZnGa2O4 single crystals
Truly bulk ZnGa2O4 single crystals were obtained directly from the melt. High melting point of 1900 ± 20 °C and highly incongruent evaporation of the Zn- and Ga-containing species impose restrictions on growth conditions. The obtained crystals are characterized by a stoichiometric or near-stoichiometric composition with a normal spinel structure at room temperature and by a narrow full width at half maximum of the rocking curve of the 400 peak of (100)-oriented samples of 23 arcsec. ZnGa2O4 is a single crystalline spinel phase with the Ga/Zn atomic ratio up to about 2.17. Melt-grown ZnGa2O4 single crystals are thermally stable up to 1100 and 700 °C when subjected to annealing for 10 h in oxidizing and reducing atmospheres, respectively. The obtained ZnGa2O4 single crystals were either electrical insulators or n-type semiconductors/degenerate semiconductors depending on growth conditions and starting material composition. The as-grown semiconducting crystals had the resistivity, free electron concentration, and maximum Hall mobility of 0.002–0.1 Ωcm, 3 × 1018–9 × 1019 cm−3, and 107 cm2 V−1 s−1, respectively. The semiconducting crystals could be switched into the electrically insulating state by annealing in the presence of oxygen at temperatures ≥700 °C for at least several hours. The optical absorption edge is steep and originates at 275 nm, followed by full transparency in the visible and near infrared spectral regions. The optical bandgap gathered from the absorption coefficient is direct with a value of about 4.6 eV, close to that of β-Ga2O3. Additionally, with a lattice constant of a = 8.3336 Å, ZnGa2O4 may serve as a good lattice-matched substrate for magnetic Fe-based spinel films.
Melt Growth and Physical Properties of Bulk LaInO3 Single Crystals
Large bulk LaInO3 single crystals are grown from the melt contained within iridium crucibles by the vertical gradient freeze (VGF) method. The obtained crystals are undoped or intentionally doped with Ba or Ce, and enabled wafer fabrication of size 10 × 10 mm2. High melting point of LaInO3 (≈1880 °C) and thermal instability at high temperatures require specific conditions for bulk crystal growth. The crystals do not undergo any phase transition up to 1300 °C, above which a noticeable thermal decomposition takes place. The good structural quality of the crystals makes them suitable for epitaxy. The onset of strong optical absorption shows orientation-dependent behavior due to the orthorhombic symmetry of the LaInO3 crystals. Assuming direct transitions, optical bandgaps of 4.35 and 4.39 eV are obtained for polarizations along the [010] and the [100], [001] crystallographic directions, respectively. There is an additional weak absorption in the range between 2.8 and 4 eV due to oxygen vacancies. Density-functional-theory calculations support the interpretation of the optical absorption data. Cathodoluminescence spectra show a broad, structured emission band peaking at ≈2.2 eV. All bulk crystals are electrically insulating. The relative static dielectric constant is determined at a value of 24.6 along the [001] direction.
High-mobility 4 μm MOVPE-grown (100) β-Ga2O3 film by parasitic particles suppression
In this work, we comprehensively investigate the development of unwanted parasitic particles in the MOVPE chamber while growing μm level films. The density of the parasitic particles is found to be pronounced at film thicknesses starting from >1.5 to 2 μm. These particles seem to induce structural defects such as twin lamellae, thereby harming the electrical properties of the grown film. The origin of the parasitic particle is attributed to the parasitic reactions within the chamber triggered by the promoted gas-phase reactions during the growth process, which can be largely reduced by increasing the total gas flow and decreasing the showerhead distance to the susceptor. A film thickness of up to 4 μm has been achieved after minimizing the density of parasitic particles. Thereby, RT Hall measurements reveal carrier mobilities of 160 cm2V−1s−1 at carrier concentrations of 5.7 × 1016cm−3
Enhancement-mode Ga2O3 wrap-gate fin field-effect transistors on native (100) β-Ga2O3 substrate with high breakdown voltage
Sn-doped gallium oxide (Ga2O3) wrap-gate fin-array field-effect transistors (finFETs) were formed by top-down BCl3 plasma etching on a native semi-insulating Mg-doped (100) β-Ga2O3 substrate. The fin channels have a triangular cross-section and are approximately 300 nm wide and 200 nm tall. FinFETs, with 20 nm Al2O3 gate dielectric and ∼2 μm wrap-gate, demonstrate normally-off operation with a threshold voltage between 0 and +1 V during high-voltage operation. The ION/IOFF ratio is greater than 105 and is mainly limited by high on-resistance that can be significantly improved. At VG = 0, a finFET with 21 μm gate-drain spacing achieved a three-terminal breakdown voltage exceeding 600 V without a field-plate.
Charge carrier density, mobility, and Seebeck coefficient of melt-grown bulk ZnGa2O4 single crystals
The temperature dependence of the charge carrier density, mobility, and Seebeck coefficient of melt-grown, bulk ZnGa2O4 single crystals was measured between 10 K and 310 K. The electrical conductivity at room temperature is about σ = 286 S/cm due to a high electron concentration of n = 3.26 × 1019 cm−3 caused by unintentional doping. The mobility at room temperature is μ = 55 cm2/V s, whereas the scattering on ionized impurities limits the mobility to μ = 62 cm2/Vs for temperatures lower than 180 K. The Seebeck coefficient relative to aluminum at room temperature is SZnGa2O4−Al = (−125 ± 2) μV/K and shows a temperature dependence as expected for degenerate semiconductors. At low temperatures, around 60 K, we observed the maximum Seebeck coefficient due to the phonon drag effect. © 2020 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).
Experimental Hall electron mobility of bulk single crystals of transparent semiconducting oxides
We provide a comparative study of basic electrical properties of bulk single crystals of transparent semiconducting oxides (TSOs) obtained directly from the melt (9 compounds) and from the gas phase (1 compound), including binary (β-Ga2O3, In2O3, ZnO, SnO2), ternary (ZnSnO3, BaSnO3, MgGa2O4, ZnGa2O4), and quaternary (Zn1−xMgxGa2O4, InGaZnO4) systems. Experimental outcome, covering over 200 samples measured at room temperature, revealed n-type conductivity of all TSOs with free electron concentrations (ne) between 5 × 1015 and 5 × 1020 cm−3 and Hall electron mobilities (μH) up to 240 cm2 V−1 s−1. The widest range of ne values was achieved for β-Ga2O3 and In2O3. The most electrically conducting bulk crystals are InGaZnO4 and ZnSnO3 with ne > 1020 cm−3 and μH > 100 cm2 V−1 s−1. The highest μH values > 200 cm2 V−1 s−1 were measured for SnO2, followed by BaSnO3 and In2O3 single crystals. In2O3, ZnO, ZnSnO3, and InGaZnO4 crystals were always conducting, while others could be turned into electrical insulators.
Cobalt as a promising dopant for producing semi-insulating β -Ga2O3crystals: Charge state transition levels from experiment and theory
Optical absorption and photoconductivity measurements of Co-doped β-Ga2O3 crystals reveal the photon energies of optically excited charge transfer between the Co related deep levels and the conduction or valence band. The corresponding photoionization cross sections are fitted by a phenomenological model considering electron-phonon coupling. The obtained fitting parameters: thermal ionization (zero-phonon transition) energy, Franck-Condon shift, and effective phonon energy are compared with corresponding values predicted by first principle calculations based on density functional theory. A (+/0) donor level ∼0.85 eV above the valence band maximum and a (0/-) acceptor level ∼2.1 eV below the conduction band minimum are consistently derived. Temperature-dependent electrical resistivity measurement at elevated temperatures (up to 1000 K) yields a thermal activation energy of 2.1 ± 0.1 eV, consistent with the position of the Co acceptor level. Furthermore, the results show that Co doping is promising for producing semi-insulating β-Ga2O3 crystals.
Numerical modelling of the czochralski growth of β-Ga2O3
Our numerical modelling of the Czochralski growth of single crystalline β-Ga2O3 crystals (monoclinic symmetry) starts at the 2D heat transport analysis within the crystal growth furnace, proceeds with the 3D heat transport and fluid flow analysis in the crystal-melt-crucible arrangement and targets the 3D thermal stress analysis within the β-Ga2O3 crystal. In order to perform the stress analysis, we measured the thermal expansion coefficients and the elastic stiffness coefficients in two samples of a β-Ga2O3 crystal grown at IKZ. Additionally, we analyse published data of β-Ga2O3 material properties and use data from literature for comparative calculations. The computations were performed by the software packages CrysMAS, CGsim, Ansys-cfx and comsol Multiphysics. By the hand of two different thermal expansion data sets and two different crystal orientations, we analyse the elastic stresses in terms of the von-Mises stress.
Bulk single crystals and physical properties of β-(AlxGa1-x)2O3(x = 0-0.35) grown by the Czochralski method
We have systematically studied the growth, by the Czochralski method, and basic physical properties of a 2 cm and 2 in. diameter bulk β-(AlxGa1-x)2O3 single crystal with [Al] = 0-35 mol. % in the melt in 5 mol. % steps. The segregation coefficient of Al in the Ga2O3 melt of 1.1-1.2 results in a higher Al content in the crystals than in the melt. The crystals were also co-doped with Si or Mg. [Al] = 30 mol. % in the melt (33-36 mol. % in the crystals) seems to be a limit for obtaining bulk single crystals of high structural quality suitable for homoepitaxy. The crystals were either semiconducting (no intentional co-dopants with [Al] = 0-30 mol. % and Si-doped with [Al] = 15-20 mol. %), degenerately semiconducting (Si-doped with [Al] ≤ 15 mol. %), or semi-insulating ([Al] ≥ 25 mol. % and/or Mg-doped). The full width at half maximum of the rocking curve was 30-50 arcsec. The crystals showed a linear but anisotropic decrease in all lattice constants and a linear increase in the optical bandgap (5.6 eV for [Al] = 30 mol. %). The room temperature electron mobility at similar free electron concentrations gradually decreases with [Al], presumably due to enhanced scattering at phonons as the result of a larger lattice distortion. In Si co-doped crystals, the scattering is enhanced by ionized impurities. Measured electron mobilities and bandgaps enabled to estimate the Baliga figure of merit for electronic devices.
Temperature dependence of the Seebeck coefficient of epitaxial β -Ga2O3 thin films
The temperature dependence of the Seebeck coefficient of homoepitaxial metal organic vapor phase grown, silicon doped β-Ga 2 O 3 thin films was measured relative to aluminum. For room temperature, we found the relative Seebeck coefficient of Sβ-Ga2O3-Al=(-300±20) μV/K. At high bath temperatures T > 240 K, the scattering is determined by electron-phonon-interaction. At lower bath temperatures between T = 100 K and T = 300 K, an increase in the magnitude of the Seebeck coefficient is explained in the frame of Stratton's formula. The influence of different scattering mechanisms on the magnitude of the Seebeck coefficient is discussed and compared with Hall measurement results. © 2019 Author(s).