Low-temperature/high-temperature AlN superlattice buffer layers for high-quality AlxGa1−xN on Si (1 1 1)

We present MOVPE-grown, high-quality Al_xGa_1−x N layers with Al content up to x=0.65 on Si (1 1 1) substrates. Crack-free layers with smooth surface and low defect density are obtained with optimized AlN-based seeding and buffer layers. High-temperature AlN seeding layers and (low temperature (LT)/high temperature (HT)) AlN-based superlattices (SLs) as buffer layers are efficient in reducing the dislocation density and in-plane residual strain. The crystalline quality of Al_xGa_1−xN was characterized by high-resolution X-ray diffraction (XRD). With optimized AlN-based seeding and SL buffer layers, best ω-FWHMs of the (0 0 0 2) reflection of 540 and 1400 arcsec for the (1 0 1¯ 0) reflection were achieved for a ∼1-μm-thick Al_0.1Ga_0.9N layer and 1010 and 1560 arcsec for the (0 0 0 2) and (1 0 1¯ 0) reflection of a ∼500-nm-thick Al_0.65Ga_0.35N layer. AFM and FE-SEM measurements were used to study the surface morphology and TEM cross-section measurements to determine the dislocation behaviour. With a high crystalline quality and good optical properties, Al_xGa_1−x N layers can be applied to grow electronic and optoelectronic device structures on silicon substrates in further investigations.     

Growth of InxGa1−xN quantum dots by nitridation of nano-alloyed droplet method using MOCVD

In_xGa_1−xN quantum dots (QDs) were grown on GaN/sapphire (0 0 0 1) substrates by employing nitridation of nano-alloyed droplet (NNAD) method using metal-organic chemical vapor deposition (MOCVD). In+Ga alloy droplets were initially formed by flowing the precursors TMIn and TMGa. Density of the In+Ga alloy droplets was increased with increasing precursors flow rate; however, the droplet size was scarcely changed in the range of about 100–200 nm. Two cases of In_xGa_1−xN QDs growth were investigated by varying the nitridation time and the growth temperature. It was observed that the In_xGa_1−xN QDs size can be easily changed by controlling the nitridation process at the temperature between 680 and 700 °C for the time of 5–30 min. Self-assembled In_xGa_1−xN QDs were successfully grown by employing NNAD method.     

Thermodynamics of the Al–Ga–N2 system

The thermodynamic properties of the Al–Ga–N₂ system under high N₂ pressure up to 10 kbar and 1800 °C are investigated. On the basis of the experimental p–T growth conditions for (Al,Ga)N crystals, the standard Gibbs free energy as well as the standard enthalpy and entropy of formation of the Al_xGa_1−xN crystals as a function of composition x were calculated. The a_N2–T and x–T phase diagrams for (Al,Ga)N are presented.     

AlxGa1−xN bulk crystal growth: Crystallographic properties and p–T phase diagram

The recent results on the growth of the Al_xGa_1−xN bulk single crystals (0.22≤x≤0.91) from solution in liquid Ga under high nitrogen pressure are discussed. We focus on the influence of temperature and the choice of the Al source on the crystal growth. The experiments involving different sources of aluminum such as Al metal, pre-reacted polycrystalline Al_yGa_1−yN and AlN powder are compared. The best results were achieved using pre-reacted polycrystalline Al_yGa_1−yN or/and AlN. Single-crystal structure refinement data of these Al_xGa_1−xN crystals are presented. We also update the p–T phase diagram of (Al,Ga)N compound at high N₂ pressure for various Al content, which is the basis for (Al,Ga)N synthesis.     

Calculation of phase diagrams in AlxIn1−xAs/InP,AsxSb1−xAl/InP and AlxIn1−xSb/InSb nano-film systems

The models for calculation of phase diagrams of semiconductor thin films with different substrates were proposed by considering the contributions of strain energy, the self-energy of misfit dislocations and surface energy to Gibbs free energy. The phase diagrams of the Al_xIn_1−xAs and As_xSb_1−xAl thin films grown on the InP (1 0 0) substrate, and the Al_xIn_1−xSb thin films grown on the InSb (1 0 0) substrate at various thicknesses were calculated. The calculated results indicate that when the thickness of film is less than 1 μm, the strain-induced zinc-blende phase appears, the region of this phase extends with decreasing of the layer thickness, and there is small effect of surface energies of liquid and solid phases on the phase diagrams.     

Digitally alloyed modulated precursor flow epitaxial growth of AlxGa1−xN layers with AlN and AlyGa1−yN monolayers

We propose a new growth scheme of digitally alloyed modulated precursor flow epitaxial growth (DA-MPEG) using metalorganic and hydride precursors for the growth of Al_xGa_1−xN layers with high-Al content at relatively low temperatures. The growth of high-quality, high-Al content Al_xGa_1−xN layers (x_Al>50%) that are composed of AlN and Al_yGa_1−yN monolayers on AlN/sapphire template/substrates by DA-MPEG was demonstrated. The overall composition of the ternary Al_xGa_1−xN material by DA-MPEG can be controlled continuously by adjusting the Column III mole fraction of the atomic Al_yGa_1−yN sub-layer. X-ray diffraction and optical transmittance results show that the AlGaN materials have good crystalline quality. The surface morphology of DA-MPEG AlGaN samples measured by atomic force microscopy are comparable to high-temperature-grown AlGaN and are free from surface features such as nano-pits.     

Relaxation and recovery processes of AlxGa1−xN grown on AlN underlying layer

The processes as in title of relaxation of the lattice mismatch and the recovery of crystalline quality in thick Al_xGa_1−xN on high-temperature-grown AlN were investigated. When x=0.3, rapid lattice relaxation occurred over a few microns, then the crystalline quality gradually recovered over 10 μm. In contrast, when x=0.7, relaxation of the lattice mismatch gradually occurred over 5 μm.     

Pseudomorphic growth of thick n-type AlxGa1−xN layers on low-defect-density bulk AlN substrates for UV LED applications

Recently it has been discovered that when growing Al_xGa_1−xN on low-defect-density bulk AlN substrates pseudomorphic layers can be achieved with a thickness far exceeding the critical thickness as given by the Matthews and Blakeslee model. For instance, the critical thickness of an Al_xGa_1−xN layer (with x=0.6) is about 40 nm thick. However we have been able to grow layers with this composition that are pseudomorphic with a thickness exceeding the critical thickness by more than an order of magnitude. This work defines the limits of pseudomorphic growth on low defect density, bulk AlN substrates to obtain low defect density, high-power UV LEDs.     

The effect of annealing on the surface morphology of strained and unstrained InxAl1−xN thin films

In_xAl_1−xN is a particularly useful group-III nitride alloy because by adjusting its composition it can be lattice matched to GaN. Such lattice-matched layers may find application in distributed Bragg reflectors (DBRs) and high electron mobility transistors (HEMTs). However, compared with other semiconducting nitride alloys, In_xAl_1-xN has not been researched extensively. In this study, thin In_xAl_1−xN epilayers were grown by metal-organic vapour phase epitaxy (MOVPE) on GaN and Al_yGa_1−yN layers. Samples were subjected to annealing at their growth temperature of 790 °C for varying lengths of time, or alternatively to a temperature ramp to 1000 °C. Their subsequent surface morphologies were analysed by atomic force microscopy (AFM). For both unstrained In_xAl_1−xN epilayers grown on GaN and compressively strained epilayers grown on Al_yGa_1−yN, surface features and fissures were seen to develop as a consequence of thermal treatment, resulting in surface roughening. It is possible that these features are caused by the loss of In-rich material formed on spinodal decomposition. Additionally, trends seen in the strained In_xAl_1−xN layers may suggest that the presence of biaxial strain stabilises the alloy by suppressing the spinode and shifting it to higher indium compositions.     

Structure and dynamics of liquid Al1−xSix alloys by ab initio molecular dynamics simulations

First-principles molecular dynamics (MD) simulations are performed to study the structure and dynamics of liquid Al_1−xSi_x (x = 0.0, 0.12, 0.2, 0.4, 0.6, 0.8) at the temperature of 1573 K. The composition dependence of static structure factors, pair correlation functions, and diffusion constants are investigated. We found that the structure of the liquid Al_1−xSi_x alloys is strongly dependent on the composition. From our simulation and analysis, we can see that although liquid Al_1−xSi_x is metallic, there are some degrees of covalent tetrahedral short-range order in the liquid. The degree of tetrahedral short-range order increases linearly as the Si concentration in the liquid increased. The diffusion coefficients of both Al and Si atoms in liquid Al_1−xSi_x alloys at 1573 K are not very sensitive to the composition.     

Optical properties of MOVPE-grown a-plane GaN and AlGaN

a-Plane GaN and AlGaN were grown on r-plane sapphire by low-pressure metal-organic vapor epitaxy (LP-MOVPE), and the effects of reactor pressure (from 40 to 500 Torr) and growth temperature (from 1020 to 1100 °C) on the crystalline quality and surface morphology of a-plane GaN were studied. The a-plane GaN grown under 40 Torr had a smooth-surface morphology but a poor crystalline quality; however, the a-plane GaN grown under 500 Torr had higher crystalline quality and optical properties, whose full-width at half-maximum of the X-ray rocking curve (XRC-FWHM) and intensity of yellow luminescence (YL) were smaller. Furthermore, the optical properties of a-plane GaN were investigated by photoluminescence (PL) in detail. We also studied the emission properties of a-plane Al_0.35Ga_0.65N grown at room temperature.     

Metamorphic growth of tensile strained GaInP on GaAs substrate

Optical and structural properties of tensile strained graded Ga_xIn_1−xP buffers grown on GaAs substrate have been studied by photoluminescence, X-ray diffraction, atomic force microscopy, and scanning electron microscopy measurements. The Ga composition in the graded buffer layers was varied from x=0.51 (lattice matched to GaAs) to x=0.66 (1% lattice mismatch to GaAs). The optimal growth temperature for the graded buffer layer was found to be about 80–100 °C lower than that for the lattice matched GaInP growth. The photoluminescence intensity and surface smoothness of the Ga_0.66In_0.34P layer grown on top of the graded buffer were strongly enhanced by temperature optimization. The relaxation of tensile GaInP was found to be highly anisotropic. A 1.5 μm thick graded buffer led to a 92% average relaxation and a room temperature photoluminescence peak wavelength of 596 nm.     

AlGaAs/InGaP interfaces in structures prepared by MOVPE

Al_0.3Ga_0.7As/In_1−xGa_xP structures were prepared by low-pressure MOVPE. Lattice matched and strained ones with top In_1−xGa_xP layers as well as reverse ones with top Al_0,3Ga_0,7As layers were examined. The structures were studied by photoluminescence, X-ray and atomic force microscope (AFM) methods. An additional photoluminescence peak from the Al_0.3Ga_0.7As/In_1−xGa_xP interface was observed in our samples and it was attributed to a type-II band offset. A conduction band offset of 0.121 eV was measured in the Al_0.3Ga_0.7As/In_0.485Ga_0.515P lattice-matched structure and a linear dependence of the conduction band offset on In_1−xGa_xP composition, with a zero offset in the Al_0.3Ga_0.7As/In_0.315Ga_0.685P structure, was determined. The valence band discontinuity had a nearly constant value of 0.152 eV.     

Mg doping behavior of MOVPE InxGa1−xN (x∼0.4)

The Mg doping behavior of MOVPE indium gallium nitride (InGaN), such as secondary ion mass spectrometry (SIMS) Mg profile, crystalline quality and n–p conversion of the films are described and discussed in this paper. The SIMS analysis reveals that the memory effect of Cp₂Mg as a doping source deteriorates the controllability of Mg doping level and profile, especially for thin (−0.4 μm) InGaN. The high residual donors (10¹⁹–10²⁰ cm⁻³) in InGaN with In content from 0.05 to 0.37 can be compensated by Mg doping and p-type conduction is obtained for those with In content up to 0.2. It is found that a higher Cp₂Mg flow rate is needed to get p-type conduction in InGaN with a higher In content x; for example, Cp₂Mg/(TEG+TMI)≈0.5% for x=0 (GaN), ≈2% for x=0.05 and ≈4% for x=0.2. Such a high Cp₂Mg flow rate is needed due to the high residual donor concentration (10¹⁹–10²⁰ cm⁻³) of InGaN films and the low activation efficiency of Mg. The crystalline quality of InGaN is deteriorated with increasing In content as well as Mg doping level. To achieve a p-type InGaN with a lower Mg doping, it is essential to improve the crystalline quality of non-doped InGaN. For this purpose, the use of a thicker GaN interlayer is effective.     

Crystal growth and luminescent properties of Pr-doped K(Y,Lu)3F10 single crystal for scintillator application

Pr1%:K(Y_1−xLu_x)₃F₁₀ (x=0, 0.2, 0.4) single crystals were grown by the μ-PD method. All the grown crystals were greenish and perfectly transparent without any inclusions or cracks. Radioluminescence spectra and decay kinetics of the Pr1%:K(Y,Lu)₃F₁₀ crystals were measured. Emission from the Pr³⁺ 5d–4f transition, peaking around 260 nm and of the decay time of around 22 ns were observed. The 5d–4f emission intensities of the Pr1%:K(Y,Lu)₃F₁₀ crystals were higher than that of the standard BGO scintillator.     

Thermal treatment-dependent chemical composition of ternary CdS1−xSex nanocrystals grown in borosilicate glass

Variation of the chemical composition of ternary CdS_1−xSe_x nanocrystals grown in borosilicate glass depending on the thermal treatment is studied by resonant Raman spectroscopy. It is shown that only for the nanocrystals with roughly equal content of substitutive S and Se chalcogen atoms (0.4<x<0.6) the nanocrystal composition is independent of the thermal treatment parameters. In other cases an increase of the thermal treatment temperature (625–700 °C) and duration (2–12 h) results in a considerable increase of the predominant chalcogen content in the nanocrystals.     

A sharp thermally reversing window in As45Te55−xIx chalcohalide glasses revealed by alternating differential scanning calorimetry and photo thermal deflection studies

The composition dependence of different thermal parameters such as glass transition temperature, non-reversing enthalpy, thermal diffusivity etc., of bulk As₄₅Te_55−xI_x chalcohalide glasses (3 ? x ? 10), has been evaluated using the temperature modulated Alternating Differential Scanning Calorimetry (ADSC) and Photo Thermal Deflection (PTD) studies. It is found that there is not much variation in the glass transition temperature of As₄₅Te_55−xI_x glasses, even though there is a wide variation in the average coordination number . This observation has been understood on the basis that the variation in glass transition temperature of network glasses is dictated by the variation in average bond energy rather than . Further, it is found that both the non-reversing enthalpy (ΔH_nr) and the thermal diffusivity (α) exhibit a sharp minimum at a composition x = 6. A broad hump is also seen in glass transition and crystallization temperatures in the composition range 5 ? x ? 7. The results obtained clearly indicate a sharp thermally reversing window in As₄₅Te_55−xI_x chalcohalide glasses around the composition x = 6.     

On the Bridgman growth of lead–tin selenide crystals with uniform tin distribution

The application of T–x–y phase diagram for the control of the crystal composition of alloy crystals during Bridgman growth is illustrated using (Pb_1−xSn_x)_1−δSe_1+δ solid solutions as an example. Within the framework of the proposed approach, the axial segregation can be minimised if the feed composition is chosen in the regions of phase diagram where the iso-mole-fraction lines are perpendicular to isotherms. For the system Pb–Sn–Se the component distribution in crystals grown from a melt with δ=0, a Se-rich melt (δ>0) and a metal-rich melt (δ<0) are discussed. Uniform crystals with x=(0.03–0.15)±0.01 can be obtained from Se-rich melt (Se enrichment is 12–5 at%Se, T=1280–1200 K). The use of metal-rich melt allows obtaining crystals with moderate segregation of 3–5 mol% SnSe for x=0.13–0.23 at 3–9 at% of metal enrichment and T=1270–1200 K and for x=0.35–0.45 at 25–35 at% of metal enrichment and T=1120–1050 K.     

A study on structural formation and optical property of wide band-gap Be0.2Zn0.8O layers grown by RF magnetron co-sputtering system

Wide band-gap BeZnO layers were grown on Al₂O₃ (0 0 0 1) substrate using radio-frequency magnetron co-sputtering. The rate of Be_xZn_1−xO crystallized as a hexagonal structure was x=0.2. From the X-ray photoelectron spectroscopy measurement, the O–Zn bonds relating the crystal structure and the Be–O bonds related to the deviation of the stoichiometry in the BeZnO layer were caught at 530.4 and 531.7 eV in the O 1s spectrum, respectively. Thus, the observance on the Be 1s peak of 113.2 eV associated with the bonding Be–O indicates that the sputtered Be atoms are substituted for the host-lattice site in ZnO. This Be–O bonding shows a relatively low intense and broadening spectrum caused by large fluctuation of Be content in the BeZnO layer. From the photoluminescence and transmittance measurement, the free exciton and the neutral donor-bound exciton (D⁰, X) emissions were observed at 3.7692 and 3.7313 eV, respectively, and an average transmittance rate over 95% was achieved in a wide ultraviolet (UV)–visible region. Also, the binding energy for the (D⁰, X) emission was extracted to be 37.9 meV. Through the wide band-gap material BeZnO, we may open some possibilities for fabricating a ZnO-based UV light-emitting diode to be utilized as a barrier layer comprised of the ZnO/BeZnO quantum well structure and/or an UV light emitting material itself.     

Crystal growth and characterization of two-leg spin ladder compounds: Sr14Cu24O41 and Sr2Ca12Cu24O41

Single crystals of Sr_14−xCa_xCu₂₄O₄₁ (x=0 and 12) are grown by the travelling solvent floating zone technique using an image furnace. The grown crystals are characterized for their single crystallinity by the X-ray and Neutron Laue method. The magnetic susceptibility measurements in Sr₁₄Cu₂₄O₄₁ show considerable anisotropy along the main crystallographic axes. Low-temperature specific heat measurement and DC susceptibility measurement in Ca-doped crystal showed antiferromagnetic ordering at 2.8 K at ambient pressure. High-pressure AC susceptibility measurement on Ca-doped crystal showed a sharp superconducting transition at 2 K under 40 kbars. T_c onset reached a maximum value of 9.9 K at 54 kbars. The bulk superconductivity of the sample is confirmed by the high-pressure AC calorimetry with T_c max=9.4 K and T_N=5 K at 56 kbars.