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Ultra-wide bandgap, conductive, high mobility, and high quality melt-grown bulk ZnGa2O4 single crystals

2019, Galazka, Zbigniew, Ganschow, Steffen, Schewski, Robert, Irmscher, Klaus, Klimm, Detlef, Kwasniewski, Albert, Pietsch, Mike, Fiedler, Andreas, Schulze-Jonack, Isabelle, Albrecht, Martin, Schröder, Thomas, Bickermann, Matthias

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.

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Bulk single crystals and physical properties of β-(AlxGa1-x)2O3(x = 0-0.35) grown by the Czochralski method

2023, Galazka, Zbigniew, Fiedler, Andreas, Popp, Andreas, Ganschow, Steffen, Kwasniewski, Albert, Seyidov, Palvan, Pietsch, Mike, Dittmar, Andrea, Anooz, Saud Bin, Irmscher, Klaus, Suendermann, Manuela, Klimm, Detlef, Chou, Ta-Shun, Rehm, Jana, Schroeder, Thomas, Bickermann, Matthias

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.

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Melt Growth and Physical Properties of Bulk LaInO3 Single Crystals

2021, Galazka, Zbigniew, Irmscher, Klaus, Ganschow, Steffen, Zupancic, Martina, Aggoune, Wahib, Draxl, Claudia, Albrecht, Martin, Klimm, Detlef, Kwasniewski, Albert, Schulz, Tobias, Pietsch, Mike, Dittmar, Andrea, Grueneberg, Raimund, Juda, Uta, Schewski, Robert, Bergmann, Sabine, Cho, Hyeongmin, Char, Kookrin, Schroeder, Thomas, Bickermann, Matthias

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.

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Suppression of particle formation by gas-phase pre-reactions in (100) MOVPE-grown β -Ga2O3films for vertical device application

2023, Chou, Ta-Shun, Seyidov, Palvan, Bin Anooz, Saud, Grüneberg, Raimund, Pietsch, Mike, Rehm, Jana, Tran, Thi Thuy Vi, Tetzner, Kornelius, Galazka, Zbigniew, Albrecht, Martin, Irmscher, Klaus, Fiedler, Andreas, Popp, Andreas

This work investigated the metalorganic vapor-phase epitaxy (MOVPE) of (100) β-Ga2O3 films with the aim of meeting the requirements to act as drift layers for high-power electronic devices. A height-adjustable showerhead achieving a close distance to the susceptor (1.5 cm) was demonstrated to be a critical factor in increasing the stability of the Ga wetting layer (or Ga adlayer) on the surface and reducing parasitic particles. A film thickness of up to 3 μm has been achieved while keeping the root mean square below 0.7 nm. Record carrier mobilities of 155 cm2 V-1 s-1 (2.2 μm) and 163 cm2 V-1 s-1 (3 μm) at room temperature were measured for (100) β-Ga2O3 films with carrier concentrations of 5.7 × 1016 and 7.1 × 1016 cm-3, respectively. Analysis of temperature-dependent Hall mobility and carrier concentration data revealed a low background compensating acceptor concentration of 4 × 1015 cm-3.

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Experimental Hall electron mobility of bulk single crystals of transparent semiconducting oxides

2021, Galazka, Zbigniew, Irmscher, Klaus, Pietsch, Mike, Ganschow, Steffen, Schulz, Detlev, Klimm, Detlef, Hanke, Isabelle M., Schroeder, Thomas, Bickermann, Matthias

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.

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Quasi-monocrystalline silicon for low-noise end mirrors in cryogenic gravitational-wave detectors

2022, Kiessling, Frank M., Murray, Peter G., Kinley-Hanlon, Maya, Buchovska, Iryna, Ervik, Torunn K., Graham, Victoria, Hough, Jim, Johnston, Ross, Pietsch, Mike, Rowan, Sheila, Schnabel, Roman, Tait, Simon C., Steinlechner, Jessica, Martin, Iain W.

Mirrors made of silicon have been proposed for use in future cryogenic gravitational-wave detectors, which will be significantly more sensitive than current room-temperature detectors. These mirrors are planned to have diameters of ≈50 cm and a mass of ≈200 kg. While single-crystalline float-zone silicon meets the requirements of low optical absorption and low mechanical loss, the production of this type of material is restricted to sizes much smaller than required. Here we present studies of silicon produced by directional solidification. This material can be grown as quasi-monocrystalline ingots in sizes larger than currently required. We present measurements of a low room-temperature and cryogenic mechanical loss comparable with float-zone silicon. While the optical absorption of our test sample is significantly higher than required, the low mechanical loss motivates research into further absorption reduction in the future. While it is unclear if material pure enough for the transmissive detector input mirrors can be achieved, an absorption level suitable for the highly reflective coated end mirrors seems realistic. Together with the potential to produce samples much larger than ≈50 cm, this material may be of great benefit for realizing silicon-based gravitational-wave detectors.