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    Ultra-wide bandgap, conductive, high mobility, and high quality melt-grown bulk ZnGa2O4 single crystals
    (Melville, NY : AIP Publ., 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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    Charge carrier density, mobility, and Seebeck coefficient of melt-grown bulk ZnGa2O4 single crystals
    (New York, NY : American Inst. of Physics, 2020) Boy, Johannes; Handwerg, Martin; Mitdank, Rüdiger; Galazka, Zbigniew; Fischer, Saskia F.
    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/).
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    High-temperature electromechanical loss in piezoelectric langasite and catangasite crystals
    (Melville, NY : American Inst. of Physics, 2021) Suhak, Yuriy; Fritze, Holger; Sotnikov, Andrei; Schmidt, Hagen; Johnson, Ward L.
    Temperature-dependent acoustic loss Q−1 is studied in partially disordered langasite (LGS, La3Ga5SiO14) and ordered catangasite (CTGS, Ca3TaGa3Si2O14) crystals and compared with previously reported CTGS and langatate (LGT, La3Ga5.5Ta0.5O14) data. Two independent techniques, a contactless tone-burst excitation technique and contacting resonant piezoelectric spectroscopy, are used in this study. Contributions to the measured Q−1(T) are determined through fitting to physics-based functions, and the extracted fit parameters, including the activation energies of the processes, are discussed. It is shown that losses in LGS and CTGS are caused by a superposition of several mechanisms, including intrinsic phonon–phonon loss, point-defect relaxations, and conductivity-related relaxations.
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    Cobalt as a promising dopant for producing semi-insulating β -Ga2O3crystals: Charge state transition levels from experiment and theory
    (Melville, NY : AIP Publ., 2022) Seyidov, Palvan; Varley, Joel B.; Galazka, Zbigniew; Chou, Ta-Shun; Popp, Andreas; Fiedler, Andreas; Irmscher, Klaus
    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.
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    Temperature dependence of the Seebeck coefficient of epitaxial β -Ga2O3 thin films
    (Melville, NY : AIP Publ., 2019) Boy, Johannes; Handwerg, Martin; Ahrling, Robin; Mitdank, Rüdiger; Wagner, Günter; Galazka, Zbigniew; Fischer, Saskia F.
    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).
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    Substrate-orientation dependence of β -Ga2O3 (100), (010), (001), and (2 ̄ 01) homoepitaxy by indium-mediated metal-exchange catalyzed molecular beam epitaxy (MEXCAT-MBE)
    (Melville, NY : AIP Publ., 2020) Mazzolini, P.; Falkenstein, A.; Wouters, C.; Schewski, R.; Markurt, T.; Galazka, Z.; Martin, M.; Albrecht, M.; Bierwagen, O.
    We experimentally demonstrate how In-mediated metal-exchange catalysis (MEXCAT) allows us to widen the deposition window for β-Ga2O3 homoepitaxy to conditions otherwise prohibitive for its growth via molecular beam epitaxy (e.g., substrate temperatures ≥800 °C) on the major substrate orientations, i.e., (010), (001), (2⎯⎯01), and (100) 6°-offcut. The obtained crystalline qualities, surface roughnesses, growth rates, and In-incorporation profiles are shown and compared with different experimental techniques. The growth rates, Γ, for fixed growth conditions are monotonously increasing with the surface free energy of the different orientations with the following order: Γ(010) > Γ(001) > Γ(2⎯⎯01) > Γ(100). Ga2O3 surfaces with higher surface free energy provide stronger bonds to the surface ad-atoms or ad-molecules, resulting in decreasing desorption, i.e., a higher incorporation/growth rate. The structural quality in the case of (2⎯⎯01), however, is compromised by twin domains due to the crystallography of this orientation. Notably, our study highlights β-Ga2O3 layers with high structural quality grown by MEXCAT-MBE not only in the most investigated (010) orientation but also in the (100) and (001) ones. In particular, MEXCAT on the (001) orientation results in both growth rate and structural quality comparable to the ones achievable with (010), and the limited incorporation of In associated with the MEXCAT deposition process does not change the insulating characteristics of unintentionally doped layers. The (001) surface is therefore suggested as a valuable alternative orientation for devices.
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    Step-flow growth in homoepitaxy of β-Ga2O3 (100)—The influence of the miscut direction and faceting
    (Melville, NY : AIP Publ., 2019) Schewski, R.; Lion, K.; Fiedler, A.; Wouters, C.; Popp, K.; Levchenko, S.V.; Schulz, T.; Schmidbauer, M.; Bin Anooz, S.; Grüneberg, R.; Galazka, Z.; Wagner, G.; Irmscher, K.; Scheffler, M.; Draxl, C.; Albrecht, M.
    We present a systematic study on the influence of the miscut orientation on structural and electronic properties in the homoepitaxial growth on off-oriented β-Ga2O3 (100) substrates by metalorganic chemical vapour phase epitaxy. Layers grown on (100) substrates with 6° miscut toward the [001⎯⎯] direction show high electron mobilities of about 90 cm2 V−1 s−1 at electron concentrations in the range of 1–2 × 1018 cm−3, while layers grown under identical conditions but with 6° miscut toward the [001] direction exhibit low electron mobilities of around 10 cm2 V−1 s−1. By using high-resolution scanning transmission electron microscopy and atomic force microscopy, we find significant differences in the surface morphologies of the substrates after annealing and of the layers in dependence on their miscut direction. While substrates with miscuts toward [001⎯⎯] exhibit monolayer steps terminated by (2⎯⎯01) facets, mainly bilayer steps are found for miscuts toward [001]. Epitaxial growth on both substrates occurs in step-flow mode. However, while layers on substrates with a miscut toward [001⎯⎯] are free of structural defects, those on substrates with a miscut toward [001] are completely twinned with respect to the substrate and show stacking mismatch boundaries. This twinning is promoted at step edges by transformation of the (001)-B facets into (2⎯⎯01) facets. Density functional theory calculations of stoichiometric low index surfaces show that the (2⎯⎯01) facet has the lowest surface energy following the (100) surface. We conclude that facet transformation at the step edges is driven by surface energy minimization for the two kinds of crystallographically inequivalent miscut orientations in the monoclinic lattice of β-Ga2O3.
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    Enhancement-mode Ga2O3 wrap-gate fin field-effect transistors on native (100) β-Ga2O3 substrate with high breakdown voltage
    (Melville, NY : American Inst. of Physics, 2016) Chabak, Kelson D.; Moser, Neil; Green, Andrew J.; Walker, Dennis E.; Tetlak, Stephen E.; Heller, Eric; Crespo, Antonio; Fitch, Robert; McCandless, Jonathan P.; Leedy, Kevin; Baldini, Michele; Wagner, Gunter; Galazka, Zbigniew; Li, Xiuling; Jessen, Gregg
    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.
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    Suppression of particle formation by gas-phase pre-reactions in (100) MOVPE-grown β -Ga2O3films for vertical device application
    (Melville, NY : American Inst. of Physics, 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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    Efficient suboxide sources in oxide molecular beam epitaxy using mixed metal + oxide charges: The examples of SnO and Ga2O
    (Melville, NY : AIP Publ., 2020) Hoffmann, Georg; Budde, Melanie; Mazzolini, Piero; Bierwagend, Oliver
    Sources of suboxides, providing several advantages over metal sources for the molecular beam epitaxy (MBE) of oxides, are conventionally realized by decomposing the corresponding oxide charge at extreme temperatures. By quadrupole mass spectrometry of the direct flux from an effusion cell, we compare this conventional approach to the reaction of a mixed oxide + metal charge as a source for suboxides with the examples of SnO2 + Sn → 2 SnO and Ga2O3 + 4 Ga → 3 Ga2O. The high decomposition temperatures of the pure oxide charge were found to produce a high parasitic oxygen background. In contrast, the mixed charges reacted at significantly lower temperatures, providing high suboxide fluxes without additional parasitic oxygen. For the SnO source, we found a significant fraction of Sn2O2 in the flux from the mixed charge that was basically absent in the flux from the pure oxide charge. We demonstrate the plasma-assisted MBE growth of SnO2 using the mixed Sn + SnO2 charge to require less activated oxygen and a significantly lower source temperature than the corresponding growth from a pure Sn charge. Thus, the sublimation of mixed metal + oxide charges provides an efficient suboxide source for the growth of oxides by MBE. Thermodynamic calculations predict this advantage for further oxides as well, e.g., SiO2, GeO2, Al2O3, In2O3, La2O3, and Pr2O3 © 2020 Author(s).