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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. [ABSTRACT FROM AUTHOR]

The investigation of the structural phase transition in the vicinity of the Curie temperature Tc$T_{\text{c}}$ of LiNb1−xTaxO3$\left(\text{LiNb}\right)_{1 - x} \left(\text{Ta}\right)_{x} \left(\text{O}\right)_{3}$ crystals is motivated by the expected combination of advantageous high‐temperature properties of LiNbO3$\left(\text{LiNbO}\right)_{3}$ and LiTaO3$\left(\text{LiTaO}\right)_{3}$, including high piezoelectric modules and remarkable high‐temperature stability, respectively. Tc$T_{\text{c}}$ marks the ultimate limit for exploiting the piezoelectric properties; however, transition‐related structural modifications might impact this and other properties even below Tc$T_{\text{c}}$. Remarkably, the phase transition from the ferroelectric to the paraelectric phase, whose temperature strongly depends on the composition x, shows a significant drop in the activation energy of the electrical conductivity. The magnitude, temperature dependence, and underlying mechanisms of this drop are discussed from a microscopic perspective. Molecular dynamics calculations in the framework of the density functional theory show that substantial displacements of the cations occur below Tc$T_{\text{c}}$ for both the end compounds LiNbO3$\left(\text{LiNbO}\right)_{3}$ and LiTaO3$\left(\text{LiTaO}\right)_{3}$, and might thus affect the electrical conductivity. Above Tc$T_{\text{c}}$, the migration of lithium ions is presumably facilitated by a shortened diffusion path for the most favorable jump of the lithium ions. Electronic contributions to the conductivity, which become important above 900 K, are explained within the polaronic picture by the formation and migration of free small polarons. [ABSTRACT FROM AUTHOR]

Specific heat capacity measurements by differential scanning calorimetry (DSC) of single crystals of solid solutions of LiNbO3 and LiTaO3 are reported and compared with corresponding ab initio calculations, with the aim to investigate the variation of the ferroelectric Curie temperature as a function of composition. For this purpose, single crystals of these solid solutions were grown with Czochralski pulling along the c-axis. Elemental composition of Nb and Ta was investigated using XRF analysis, and small samples with homogeneous and well known composition were used for the DSC measurements. We observed that the ferroelectric Curie temperature decreases linearly with increasing Ta concentration in the LiNb 1 − x Ta x O3 solid solution crystals. Furthermore, the ferroelectric transition width of a mixed crystal appears to be smaller, as compared to pure LiTaO3. [ABSTRACT FROM AUTHOR]

Ceramic dielectrics with particularly low levels of dielectric loss and low permittivity are of growing interest toward millimeter‐wave applications. Based on composition and structural considerations, lithic kosmochlor is expected to meet these requirements while exhibiting low densification temperatures, allowing its integration also in co‐fired circuits. Herein, it is found that the spark plasma sintering of LiCrSi2O6 ceramics facilitates densification at temperatures more than 200 °C lower than conventionally processed materials in only a fraction of the time. A spark plasma sintering duration of 10 min is necessary in order to achieve a controllable process with a repeatable high‐performance product material exhibiting a fine‐grained microstructure. Characterization millimeter‐wave frequencies reveal that LiCrSi2O6 materials produced in this manner exhibit excellent dielectric properties (Qf = 80 700 GHz and εr = 7.5 at 134.24 GHz) following densification at only 950 °C with a relative density of 97.4%. These results represent an unprecedented combination of low dielectric losses and processing temperatures for ceramics processed without the addition of sintering aids. The materials and methods explored here present a promising pathway toward high‐performance millimeter‐wave and co‐firable systems. [ABSTRACT FROM AUTHOR]

Laser‐flash measurements of the thermal conductivity λ(hkl)$\lambda _{(hkl)}$ of Czochralski‐grown β‐Ga2O3 single crystals are reported perpendicular to four independent crystallographic lattice planes (hkl)=(2¯01)$(hkl)=(\bar{2}01)$, (010), (001), and (100) between room temperature and 1200 K. λ is represented by a symmetric tensor of rank 2 and has four independent components. Tensor components λ11=λ(100)=12.13$\lambda _{11}=\lambda _{(100)}=12.13$ W m−1 K−1 and λ22=λ(010)=24.26$\lambda _{22}=\lambda _{(010)}=24.26$ W m−1 K−1 (values for 300 K) can be directly measured. λ33=14.09$\lambda _{33}=14.09$ W m−1 K−1 and λ13=−0.992$\lambda _{13}=-0.992$ W m−1 K−1, instead, are obtained by combining λ(001)=13.53$\lambda _{(001)}=13.53$ W m−1 K and λ(2¯01)=14.33$\lambda _{(\bar{2}01)}=14.33$ W m−1 K. The crystallographic b⃗$\vec{b}$‐axis is the direction with the highest thermal conductivity, λ22. The thermal conductivity assumes its lowest value (11.73 W m−1 K−1) in a direction close to the crystallographic a⃗$\vec{a}$‐axis. However, this direction does not coincide with a⃗$\vec{a}$, and changes with temperature. [ABSTRACT FROM AUTHOR]

By differential thermal analysis, a concentration field suitable for the growth of Zr, Mg co-doped strontium hexagallate crystals was observed that corresponds well with known experimental results. It was shown that the melting point of doped crystal is ca. 60 K higher than that of undoped crystals. This higher melting points indicate hexagallate phase stabilization by Zr, Mg co-doping and increase the growth window of (Mg,Zr):SrGa12O19, compared to undoped SrGa12O19 that grows from SrO–Ga2O3 melts. [ABSTRACT FROM AUTHOR]

Iron(II) oxide, wüstite, is the iron oxide with the lowest oxygen content. Under ambient conditions it is metastable for two reasons: (1) it undergoes eutectoid decomposition to Fe and Fe3O4 below ≈570° C, and (2) depending on temperature, it is thermodynamically stable only for very low oxygen partial pressures, down to below 10−20 bar. Hence, for the growth of single crystals from the melt, the growth atmosphere must contain reducing components to keep the oxygen partial pressure on the required low level. With Ar/CO2/CO mixtures this aim can be reached. It is shown experimentally and by thermodynamic calculation, that the grown crystals contain carbon inclusions. Theoretically it is shown that wüstite crystals without carbon inclusions could be grown in humid N2/H2 mixtures. First experiments are presented in this article, but a further adjustment of experimental parameters is required. [ABSTRACT FROM AUTHOR]

Two inch diameter, highly conducting (Si-doped) bulk β-Ga2O3 single crystals with the cylinder length up to one inch were grown by the Czochralski method. The obtained crystals revealed high structural quality characterized by narrow x-ray rocking curves (FWHM ≤ 25 arc sec) and high surface smoothness (RMS < 200 pm) of the epi-ready wafers. The free electron concentration and Hall mobility at room temperature were in the range of 1.6–9 × 1018 cm−3 and 118 – 52 cm2 V−1 s−1, respectively, which are not affected by a heat treatment at temperatures up to 1000 °C in an oxidizing atmosphere. Temperature-dependent electrical properties of the crystals revealed a degenerated semiconducting state. Both high structural quality and electrical properties make the crystals well suited as substrates for homoepitaxy and electronic device fabrication in the vertical configuration. [ABSTRACT FROM AUTHOR]

Several metal oxide compounds, especially those containing metals possessing several valence states, are able to absorb or release oxygen under suitable thermodynamic conditions. Such behavior is found often in systems containing oxides of transition metals. It is important to note that the equilibrium oxidation level of those metal oxides can depend on the aggregation state, which may significantly impede crystal growth processes from the melt. If during the melt growth of such oxide crystals, the average valence state of the oxides is different in the molten and solid state, then crystallization is connected with the absorption of free oxygen from the ambient gas, or with the release of free oxygen into it. This phenomenon can be detected by simultaneous DTA/TG measurements and can deteriorate the stability of crystal growth. This holds especially if the average valence in the solid is smaller than in the melt, because oxygen release can lead to bubble formation at the crystallization front. [ABSTRACT FROM AUTHOR]

Pb2Sc2Si2O9 and Pb2In2Si2O9, respectively, the scandium and indium containing structural analogues of the mineral kentrolite are grown by spontaneous crystallization from a PbO flux. The corresponding polycrystalline powder samples are synthesized by conventional solid-state approach. The compounds are thoroughly characterized using temperature-dependent single crystal and powder X-ray diffraction, heat capacity measurements, second harmonic generation experiments and Raman spectroscopy. At ambient conditions, both compounds crystallize in the non-centrosymmetric Pna21 space group and undergo phase transitions to the centrosymmetric Pbcn space group at elevated temperatures. The Pbcn into Pna21 phase transitions are complemented by the signals of the temperature-dependent second harmonic generation. The specific heat capacity exhibits distinct cusp, supporting the λ-type second-order phase transition. The temperature dependency of some selective Raman modes further complements the findings, showing softening and hardening of the phonons across the phase transitions. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]