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.
Abstract
Homoepitaxial growth of SrTiO
3
thin films on 0.5 wt% niobium doped SrTiO
3
(100) substrates with high structural perfection was developed using liquid-delivery spin metal–organic vapor ...phase epitaxy (MOVPE). Exploiting the advantage of adjusting the partial pressures of the individual constituents independently, we tuned the Sr/Ti ratio of the gas phase for realizing, stoichiometric, as well as Sr deficient layers. Quantitative energy dispersive X-ray spectroscopy in a scanning transmission electron microscope confirm Sr deficiency of up to 20% in nominally off-stoichiometrically grown films. Our MOVPE process allows to grow such layers in phase pure state and without extended defect formation. Indications for oxygen deficiency could not be identified. Sr deficient layers exhibit an increased permittivity of
ɛ
r
= 202 and a larger vertical lattice parameter. Current–voltage characteristics (IVCs) of metal–oxide–semiconductor (Pt/SrTiO
3
/SrTiO
3
:Nb) structures reveal that Sr deficient SrTiO
3
films show an intrinsic resistive switching with on–off ratios of three orders of magnitude at RT and seven orders of magnitude at 10 K. There is strong evidence that a large deviation from stoichiometry pronounces the resistive switching behavior. IVCs conducted at 10 K indicate a defect-based mechanism instead of mass transport by ion diffusion. This is supported by in-situ STEM investigations that show filaments to form at significant higher voltages than those were resistive switching is observed in our samples.
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.
Freestanding AlN single crystals are grown in a RF-heated furnace by physical vapor transport (PVT). Three different growth regimes with growth temperatures between 2080--2200 °C result in different ...crystal habits and very high structural quality. The Rocking curves show $\mathrm{FWHM}< 21$ arcsec in the 0002 and $10\bar{1}0$ Reflection on the as-grown facets. Isometric AlN crystals with sizes up to $10\times 10\times 12$ mm 3 show a zonar structure consisting of a yellowish core area which is grown on the N-polar ($000\bar{1}$) facet and a nearly colorless edge region grown on prismatic $\{10\bar{1}0\}$ facets. In the two growth zones nearly the same C concentrations but different amounts of O and Si are measured by secondary ion mass spectrometry (SIMS). The yellowish core area show a very low defect density ($\mathrm{EPD}\leq 100$ cm -2 ) and a higher deep UV transparency compared to the edge region.
Czochralski-grown β-Ga2O3 and β-Ga2O3:Si crystals with the free electron concentrations between 2.5·1016 and 4.3·1018 cm−3 have been characterized by means of pulse height and scintillation time ...profile measurements in order to assess their basic scintillation properties. At room temperature, with increasing free electron concentration in the studied range, the scintillation yields decrease from 8920 to 1930 ph/MeV, while the mean scintillation decay times pare down from 989 to 61 ns. However, when the brightest β-Ga2O3 sample is cooled down below 100 K, its scintillation yield exceeds 20000 ph/MeV.
•Czochralski-grown β-Ga2O3 and β-Ga2O3:Si crystals have been characterized.•Scintillation yield and decay times strongly depend on free electron concentration.•Scintillation yield clearly goes up with decreasing temperature towards liquid N2.
SnO2 is a semiconductor with a wide optical bandgap (3.5 eV), which makes it an attractive transparent semiconducting oxide (TSO) for electronic and opto‐electronic applications. At elevated ...temperatures it is, however, much more unstable than other TSOs (such as ZnO, Ga2O3, or In2O3). This leads to a rapid decomposition even under very high oxygen pressures. Our experiments showed that stoichiometric SnO2 does not melt up to 2100 °C, in contradiction to earlier published data. Bulk SnO2 single crystals, that could provide substrates for epitaxial growth, have not been reported so far. Hereby we report on truly bulk SnO2 single crystals of 1 inch diameter grown by physical vapor transport (PVT). The most volatile species during SnO2 decomposition is, in addition to oxygen, SnO, which is stable in the gas phase at high temperature and reacts again with oxygen at lower temperatures to form SnO2. We identified a relatively narrow temperature window, temperature gradients and a ratio of SnO/O2 for providing the best conditions for SnO2 single crystal growth. X‐ray powder diffraction (XRD) proved the single SnO2 phase. Moreover, by selecting a suitable SnO/O2 ratio it was possible to obtain either n‐type conductivity with electron concentrations up to 2 × 1018 cm−3 and electron mobilities up to 200 cm2 V−1 s−1, or insulating behavior. The crystals exhibited an optical absorption edge located at 330–355 nm, depending on the crystal orientation, and a good transparency over visible and near infrared (NIR) spectra.
Ammonothermally grown GaN is a promising substrate for high-power optoelectronics and electronics thanks to its scalability and high structural perfection. Despite extensive research, ammonothermal ...GaN still suffers from significant concentrations of impurities. This article discusses the evolution of impurity incorporation during growth of basic ammonothermal GaN, in specific whether the impurity concentration changes temporally along the growth direction and how the autoclave influences the impurity concentration. The effect of the impurities on the structural, electrical and optical properties of the grown crystal is also discussed. The chemical analysis is carried out by time of flight secondary ion mass spectroscopy (ToF-SIMS) and laser-ablation inductively-coupled plasma mass spectroscopy (LA-ICP-MS). Strain and dislocation generation caused by impurity concentration gradients and steps are studied by synchrotron radiation x-ray topography (SR-XRT). Fourier transform infrared (FTIR) reflectivity is used to determine the effect of the impurities on the free carrier concentration, and the luminescent properties are studied by low temperature photoluminescence (PL). The influence of the autoclave is studied by growing a single boule in multiple steps in several autoclaves. LA-ICP-MS and ToF-SIMS ion intensities indicate that the impurity concentrations of several species vary between different autoclaves by over an order of magnitude. SR-XRT measurements reveal strain at the growth interfaces due to impurity concentration gradients and steps. Oxygen is determined to be the most abundant impurity species, resulting in a high free carrier concentration, as determined by FTIR. The large variation in Mn concentration dramatically affects PL intensity.
•Ammonothermal GaN was grown in several steps in several autoclaves.•Impurity incorporation varied by over an order of magnitude between autoclaves.•No dislocation generation despite strain due to inhomogeneous impurity incorporation.•High oxygen concentration resulted in a high free carrier concentration.•High manganese concentration reduced photoluminescence intensity dramatically.
In this work, we train a hybrid deep-learning model (fDNN, Forest Deep Neural Network) to predict the doping level measured from the Hall Effect measurement at room temperature and to investigate the ...doping behavior of Si dopant in both (100) and (010) β-Ga2O3 thin film grown by the metalorganic vapor phase epitaxy (MOVPE). The model reveals that a hidden parameter, the Si supplied per nm (mol/nm), has a dominant influence on the doping process compared with other process parameters. An empirical relation is concluded from this model to estimate the doping level of the grown film with the Si supplied per nm (mol/nm) as the primary variable for both (100) and (010) β-Ga2O3 thin film. The outcome of the work indicates the similarity between the doping behavior of (100) and (010) β-Ga2O3 thin film via MOVPE and the generality of the results to different deposition systems.
Low temperature thermoluminescence of β-Ga2O3, β-Ga2O3:Al and β-Ga2O3:Ce has been investigated. Glow curves have been analyzed quantitatively using a rate equations model in order to determine the ...traps parameters, such as activation energies, capture cross-sections and probabilities of recombination and retrapping.
•Undoped and doped β-Ga2O3 crystals have been grown by the Czochralski method.•Their glow curves between 10 and 350 K have been investigated.•Rate equations model has been used to determine traps parameters.