Studies of ambient-pressure and high-pressure behaviour of photoluminescence (PL) as well as the phase transition pressure from wurtzite to cubic structure for a series of Zn1-xMgxO alloys as a function of the Mg-content x (0 <= x <= 0.34) are presented. The measured PL peak energy is shown to increase approximately linearly with increasing magnesium content from 3.36 eV to 4.11 eV, and the phase transition pressure from wurtzite to cubic structure decreases with increasing x from 12.6 GPa to 5.9 GPa. The phase transition is accompanied by a strong decrease of the near band-gap PL intensity. The value of the PL peak pressure coefficient dE(PL)/dp changes non-monotonically. It varies between 18.6 meV/GPa and 25.2 meV/GPa, and seems to depend on the layer thickness rather than on the layer composition, exhibiting strong scattering for several alloys with similar magnesium content. This behaviour can be due to the stabilizing influence of sapphire substrate, as is indicated both by the pressure coefficients and by the values of pressure of phase transition from wurtzite to rock salt structure in Zn1-xMgxO layers with the same or similar composition and different layer thicknesses. (C) 2016 Elsevier B.V. All rights reserved.
The self-assembled formation of ordered, vertically stacked rocksalt/wurtzite MgxZn1−xO heterostructures by planar phase separation is shown. These heterostructures form quasi “natural” two-dimensional hetero-interfaces between the different phases upon annealing of MgO-oversaturated wurtzite MgxZn1−xO layers grown by plasma-assisted molecular beam epitaxy on c-plane sapphire substrates. The optical absorption spectra show a red shift simultaneous with the appearance of a cubic phase upon annealing at temperatures between 900 °C and 1000 °C. Transmission electron microscopy reveals that these effects are caused by phase separation leading to the formation of a vertically ordered rock salt/wurtzite heterostructures. To explain these observations, we suggest a phase separation epitaxy model that considers this process being initiated by the formation of a cubic (Mg,Zn)Al2O4 spinel layer at the interface to the sapphire substrate, acting as a planar seed for the epitaxial precipitation of rock salt MgxZn1−xO. The equilibrium fraction x of magnesium in the resulting wurtzite (rock salt) layers is approximately 0.15 (0.85), independent of the MgO content of the as-grown layer and determined by the annealing temperature. This model is confirmed by photoluminescence analysis of the resulting layer systems after different annealing temperatures. In addition, we show that the thermal annealing process results in a significant reduction in the density of edge- and screw-type dislocations, providing the possibility to fabricate high quality templates for quasi-homoepitaxial growth.
In this work, simulations of the electronic band structure of a p-GaN/n-ZnO heterointerface are presented. In contrast to homojunctions, an additional energy barrier due to the type-II band alignment hinders the flow of majority charge carriers in this heterojunction. Spontaneous polarization and piezoelectricity are shown to additionally affect the band structure and the location of the recombination region. Proposed as potential UV-LEDs and laser diodes, p-GaN/n-ZnO heterojunction nanowires were fabricated by plasma-assisted molecular beam epitaxy (PAMBE). Atomic resolution annular bright field scanning transmission electron microscopy (STEM) studies reveal an abrupt and defect-free heterointerface with a polarity inversion from N-polar GaN to Zn-polar ZnO. Photoluminescence measurements show strong excitonic UV emission originating from the ZnO-side of the interface as well as stimulated emission in the case of optical pumping above a threshold of 55 kW/cm(2).
Zn1–xMgxO epitaxial films with Mg concentrations 0≤x≤0.3 were grown by plasma-assisted molecular beam epitaxy on a-plane sapphire substrates. Precise determination of the Mg concentration x was performed by elastic recoil detection analysis. The bandgap energy was extracted from absorption measurements with high accuracy taking electron-hole interaction and exciton-phonon complexes into account. From these results a linear relationship between bandgap energy and Mg concentration is established for x≤0.3. Due to alloy disorder, the increase of the photoluminescence emission energy with Mg concentration is less pronounced. An analysis of the lattice parameters reveals that the epitaxial films grow biaxially strained on a-plane sapphire.
Contactless electroreflectance (CER) has been applied to study optical transitions in Zn1-xMgxO layers with magnesium concentration ≤44%. CER resonances related to free exciton and band-to-band transitions were clearly observed at room temperature. For ZnO the two transitions are separated by the energy of ∼65 meV, which is attributed to the free exciton binding energy in ZnO. Due to magnesium incorporation, the CER resonances broaden and shift to blue. The energy separation between excitonic and band-to-band transitions increases up to ∼100 meV when the magnesium concentration reaches 22%. For larger magnesium concentrations, CER resonances are significantly broadened and the excitonic transition is no longer resolved in the CER spectrum.
We investigate the carrier relaxation from (ZnMg)O barrier layers into a ZnO quantum well (QW) by following the dynamic screening of its built-in electric fields. The respective emission lines shift in energy as the carriers populate the QW, spectrally shifting the time-resolved photoluminescence. At low temperatures, the carrier capture into the QW is found to occur on the same or an even faster time scale than the carrier-trapping processes within the barriers. DOI: 10.1103/PhysRevB.87.035309
ZnO/Zn1−xMgxO single quantum wells (SQWs) were grown by plasma-assisted molecular beam epitaxy on c-plane sapphire substrates. Compositional grading allows the application of optimized growth conditions for the fabrication of Zn1−xMgxO barriers with high crystalline quality and a maximum Mg content of x = 0.23. High resolution x-ray diffraction reveals partial relaxation of the graded barriers. Due to exciton localization, the SQW emission is found to consist of contributions from donor-bound and free excitons. While for narrow SQWs with well width dW≤2.5nm, the observed increase of the exciton binding energy is caused by quantum confinement, the drop of the photoluminescence emission below the ZnO bulk value found for wide SQWs is attributed to the quantum-confined Stark effect. For a Mg content of x = 0.23, a built-in electric field of 630 kV/cm is extracted, giving rise to a decrease of the exciton binding energy and rapid thermal quenching of the SQW emission characterized by an activation energy of (24 ± 4) meV for dW = 8.3 nm.
Nonpolar Zn1-xMgxO epitaxial films were grown by plasma-assisted molecular beam epitaxy on a-plane ZnO substrates. A smooth surface morphology was accomplished under oxygen-rich growth conditions. The benefits of the use of ZnO substrates on the structural properties are reflected by a low-density of threading dislocations. Furthermore, no indications for the generation of basal plane stacking faults are found. The pseudomorphic growth on a-plane ZnO substrates efficiently locks the epitaxial Zn1-xMgxO films to the wurtzite structure up to x=0.25. The Mg concentration is not constant and increases with larger thickness. The optical properties reflect the influence of alloy disorder. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4754076]
ZnO/Zn1 − xMgxO single quantum well (SQW) structures with well widths dW between 1.1 nm and 10.4 nm were grown by plasma-assisted molecular beam epitaxy both heteroepitaxially on c-plane sapphire and homoepitaxially on (0001¯)-oriented bulk ZnO. A significantly reduced Mg incorporation in the top barrier related to the generation of stacking faults is observed for heteroepitaxial samples. Exciton localization is observed for both types of samples, while an enhancement of the exciton binding energy compared to bulk ZnO is only found for homoepitaxial SQWs for 2 nm ≤ dW ≤ 4 nm. Consistently, for homoepitaxial samples, the carrier dynamics are mainly governed by radiative recombination and carrier cooling processes at temperatures below 170 K, whereas thermally activated non-radiative recombination dominates in heteroepitaxial samples. The effects of polarization-induced electric fields are concealed for Mg concentrations x < 0.1 due to the reduction of the exciton binding energy, the screening by residual carriers as well as the asymmetric barrier structure in heteroepitaxial wells.
The characteristics of the excitonic absorption and emission around the fundamental bandgap of wurtzite MgxZn1−xO grown on c-plane sapphire substrates by plasma assisted molecular beam epitaxy with Mg contents between x = 0 and x = 0.23 are studied using spectroscopic ellipsometry and photoluminescence (PL) measurements. The ellipsometric data were analyzed using a multilayer model yielding the dielectric function (DF). The imaginary part of the DF for the alloys exhibits a pronounced feature which is attributed to exciton-phonon coupling (EPC) similar to the previously reported results for ZnO. Thus, in order to determine reliable transition energies, the spectral dependence is analyzed by a model which includes free excitonic lines, the exciton continuum, and the enhanced absorption due to EPC. A line shape analysis of the temperature-dependent PL spectra yielded in particular the emission-related free excitonic transition energies, which are compared to the results from the DF line-shape analysis. The PL linewidth is discussed within the framework of an alloy disorder model.
The temperature and carrier-density dependent excitonic relaxation in bulk ZnO is studied by means of time-resolved photoluminescence. A rate-equation model is used to analyze the population dynamics and the transitions between different exciton states. Intra-excitonic (n = 1) to (n = 2) relaxation is clearly identified at low excitation densities and lattice temperatures with a characteristic time constant of 6 ± 0.5 ps.
Carrier recombination dynamics in Zn1-xMgxO alloys were studied by time-resolved photoluminescence as function of Mg concentration and lattice temperature for different emission and excitation energies. Disorder and carrier localization effects are found to play a significant role, becoming increasingly important for lower temperatures and higher Mg concentrations.Emission energy dependent dynamics were analyzed by the application of a theoretical model, yielding a characteristic localization energy of 60 +/- 15meV for the sample with the highest Mg concentration of x = 0.21. (C) 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
The influence of the Mg concentration and lattice temperature on the carrier recombination dynamics in Zn1−xMgxO alloys has been studied by time-resolved photoluminescence for different emission and excitation energies. Carrier localization effects are found to play a significant role, becoming increasingly important for lower temperatures and higher Mg concentrations. Emission energy dependent dynamics were analyzed by the application of the theoretical model, yielding a characteristic localization energy of 60±15meV for the sample with the highest Mg concentration of x=0.21.
Zn1−xMgxO thin films with a Mg content x between 0 and 0.42 grown by plasma-assisted molecular beam epitaxy on c-plane sapphire substrates were investigated by electron spin resonance at 5 K. Above band gap illumination induces a persistent resonance signal, which is attributed to free conduction band electrons. The g-factors of the Zn1−xMgxO epitaxial layers and their anisotropy were determined experimentally and an increase from g∥=1.957 for x=0 to g∥=1.970 for x=0.42 was found, accompanied by a decrease in anisotropy. A comparison with g-factors of the AlxGa1−xN system is also given.
Wurtzite Zn1−xMgxO thin films with Mg contents between x=0 and x=0.37 were grown on c-plane sapphire substrates by plasma assisted molecular beam epitaxy using a MgO/ZnMgO buffer layer. The a-lattice parameter is independent from the Mg concentration, whereas the c-lattice parameter decreases from 5.20 Å for x=0 to 5.17 Å for x=0.37, indicating pseudomorphic growth. The near band edge photoluminescence shows a blueshift with increasing Mg concentration to an emission energy of 4.11 eV for x=0.37. Simultaneously, the energetic position of the deep defect luminescence shows a linear shift from 2.2 to 2.8 eV. Low temperature transmission measurements reveal strong excitonic features for the investigated composition range and alloy broadening effects for higher Mg contents. The Stokes shift as well as the Urbach energy is increased to values of up to 125 and 54 meV for x=0.37, respectively, indicating exciton localization due to alloy fluctuations.