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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.
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).
The electronic structure of ϵ-Ga2O3
The electronic structure of ε-Ga2O3 thin films has been investigated by ab initio calculations and photoemission spectroscopy with UV, soft, and hard X-rays to probe the surface and bulk properties. The latter measurements reveal a peculiar satellite structure in the Ga 2p core level spectrum, absent at the surface, and a core-level broadening that can be attributed to photoelectron recoil. The photoemission experiments indicate that the energy separation between the valence band and the Fermi level is about 4.4 eV, a valence band maximum at the Γ point and an effective mass of the highest lying bands of – 4.2 free electron masses. The value of the bandgap compares well with that obtained by optical experiments and with that obtained by calculations performed using a hybrid density-functional, which also reproduce well the dispersion and density of states.
Static Dielectric Constant of β-Ga2O3 Perpendicular to the Principal Planes (100), (010), and (001)
The relative static dielectric constant ℇr of β-Ga2O3 perpendicular to the planes (100), (010), and (001) is determined in the temperature range from 25 K to 500 K by measuring the AC capacitance of correspondingly oriented plate capacitor structures using test frequencies of up to 1 MHz. This allows a direct quantification of the static dielectric constant and a unique direction assignment of the obtained values. At room temperature, ℇr perpendicular to the planes (100), (010), and (001) amounts to 10.2 ± 0.2, 10.87 ± 0.08, and 12.4 ± 0.4, respectively, which clearly evidence the anisotropy expected for β-Ga2O3 due to its monoclinic crystal structure. An increase of ℇr by about 0.5 with increasing temperature from 25 K to 450 K was found for all orientations. Our ℇr data resolve the inconsistencies in the previously available literature data with regard to absolute values and their directional assignment and therefore provide a reliable basis for the simulation and design of devices. © The Author(s) 2019.
Femtosecond laser-assisted fabrication of chalcopyrite micro-concentrator photovoltaics
Micro-concentrator solar cells offer an attractive way to further enhance the efficiency of planar-cell technologies while saving absorber material. Here, two laser-based bottom-up processes for the fabrication of regular arrays of CuInSe2 and Cu(In,Ga)Se2 microabsorber islands are presented, namely one approach based on nucleation and one based on laser-induced forward transfer. Additionally, a procedure for processing these microabsorbers to functioning micro solar cells connected in parallel is demonstrated. The resulting cells show up to 2.9% efficiency and a significant efficiency enhancement under concentrated illumination.
Adsorption-controlled growth of La-doped BaSnO3 by molecular-beam epitaxy
Epitaxial La-doped BaSnO3 films were grown in an adsorption-controlled regime by molecular-beam epitaxy, where the excess volatile SnOx desorbs from the film surface. A film grown on a (001) DyScO3 substrate exhibited a mobility of 183 cm2 V-1 s-1 at room temperature and 400 cm2 V-1 s-1 at 10 K despite the high concentration (1.2 × 1011 cm-2) of threading dislocations present. In comparison to other reports, we observe a much lower concentration of (BaO)2 Ruddlesden-Popper crystallographic shear faults. This suggests that in addition to threading dislocations, other defects - possibly (BaO)2 crystallographic shear defects or point defects - significantly reduce the electron mobility.
Structural and chemical investigations of adapted Siemens feed rods for an optimized float zone process
The optimization of the float zone process for industrial application is a promising way to crystallize high purity silicon for high efficiency solar cells with reduced process costs. We investigated two differently produced Siemens rods which should be used as feed material for the float zone process. The aim is to identify and to improve material properties of the feed rods which have a high impact to the float zone process. We show here microstructural and chemical analysis comparing feed rods manufactured under standard conditions and under float zone adapted conditions. To resolve the growth behavior of the grains SEM/EBSD mappings are performed at different positions. TEM analyses are used to investigate the interface region between the mono- and the multicrystalline silicon within the Siemens feed rod. Additionally, drilled cores are cut out from the feed rods containing the region of the slim rod. Afterwards, the drilled cores are crystallized with the float zone process. Finally, carbon and oxygen measurements with FT-IR spectrometry on different positions of the crystallized drilled cores of the Siemens feed rods show the influence of the slim rod material to the float zone process.
Lithium metal penetration induced by electrodeposition through solid electrolytes: Example in single-crystal Li6La3ZrTaO12 garnet
Solid electrolytes potentially enable rechargeable batteries with lithium metal anodes possessing higher energy densities than today’s lithium ion batteries. To do so the solid electrolyte must suppress instabilities that lead to poor coulombic efficiency and short circuits. In this work, lithium electrodeposition was performed on single-crystal Li6La3ZrTaO12 garnets to investigate factors governing lithium penetration through brittle electrolytes. In single crystals, grain boundaries are excluded as paths for lithium metal propagation. Vickers microindentation was used to introduce surface flaws of known size. However, operando optical microscopy revealed that lithium metal penetration propagates preferentially from a different, second class of flaws. At the perimeter of surface current collectors smaller in size than the lithium source electrode, an enhanced electrodeposition current density causes lithium filled cracks to initiate and grow to penetration, even when large Vickers defects are in proximity. Modeling the electric field distribution in the experimental cell revealed that a 5-fold enhancement in field occurs within 10 micrometers of the electrode edge and generates high local electrochemomechanical stress. This may determine the initiation sites for lithium propagation, overriding the presence of larger defects elsewhere.
Step-flow growth in homoepitaxy of β-Ga2O3 (100)—The influence of the miscut direction and faceting
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.
Influence of slim rod material properties to the Siemens feed rod and the float zone process
The identification and understanding of material properties influencing the float zone process is important to crystallize high purity silicon for high efficiency solar cells. Also the knowledge of minimal requirements to crystallize monocrystalline silicon with the float zone process is of interest from an economic point of view. In the present study, feed rods for the float zone process composed of a central slim rod and the deposited silicon from the Siemens process are investigated. Previous studies have shown that the slim rod has a significant impact on the purity and suitability for further crystallization processes. In particular, contaminations like substitutional carbon and the presence of precipitates as well as the formation of oxide layers play an important role and are investigated in detail. For this purpose different slim rod materials were used in deposition and float zone crystallization experiments. Samples were prepared by cross sectioning and core drilling of Siemens rods, which were recrystallized with the float zone process. Recrystallized drilled cores are analyzed with FT-IR spectrometry concerning the carbon and oxygen content. To estimate the grain growth behavior on the slim rod surface in dependence of the used slim rod material, EBSD mappings inside a SEM are performed on squared and circular slim rods. TEM analysis was used to investigate the presence of an oxide layer at the interface between slim rod and deposited polycrystalline silicon. Additionally the influence of a nitrogen-containing gas atmosphere during the slim rod pulling is investigated by IR microscopy and ToF-SIMS regarding Si3N4 precipitation.