Structural and optical investigation of InGaN/GaN multiple quantum well structures with various indium compositions

We have studied the influence of indium (In) composition on the structural and optical properties of In_x Ga_1−xN/GaN multiple quantum wells (MQWs) with In compositions of more than 25% by means of high-resolution x-ray diffraction (HRXRD), photoluminescence (PL), and transmission electron microscopy (TEM). With increasing the In composition, structural quality deterioration is observed from the broadening of the full width athalf maximum of the HRXRD superlattice peak, the broad multiple emission peaks oflow temperature PL, and the increase of defect density in GaN capping layers and InGaN/GaN MQWs. V-defects, dislocations, and two types of tetragonal shape defects are observed within the MQW with 33% In composition by high resolution TEM. In addition, we found that V-defects result in different growth rates of the GaN barriers according to the degree of the bending of InGaN well layers, which changes the period thickness of the superlattice and might be the source of the multiple emission peaks observed in the In_xGa_1−xN/GaN MQWs with high in compositions.     

渐变In组分InGaN/GaN多量子阱结构中的相分凝及其对提高量子效率的作用研究

利用光荧光、阴极荧光以及时间分辨荧光光谱技术研究了具有不同In组分的渐变InGaN/GaN多量子阱结构中的相分凝现象。在10 K的荧光光谱中,所有的三个样品中除了主发光峰位外,在其高能及低能位置处还出现了另外两个发光峰,表现出了明显的相分凝现象。三个样品阴极荧光结果中呈现出了明显的强度对比,证明了相分凝现象随着量子阱中In组分的增加而加剧。在15 K的时间分辨荧光光谱中,随着In组分的增加,谱线的上升时间得到了延迟,这表明了载流子在由于相分凝而造成的低、高In组分结构中的输运。     

Investigation of microstructure and V-defect formation in In<Subscript>x</Subscript>Ga<Subscript>1−x</Subscript>N/GaN MQW grown using temperature-gradient metalorganic chemical vapor deposition

Temperature-gradient metalorganic chemical vapor deposition (MOCVD) was used to deposit In_xGa_1−xN/GaN multiple quantum well (MQW) structures with a concentration gradient of indium across the wafer. These MQW structures were deposited on low defect density (2×10⁸ cm⁻²) GaN template layers for investigation of microstructural properties and V-defect (pinhole) formation. Room temperature (RT) photoluminescence (PL) and photomodulated transmission (PT) were used for optical characterization, which show a systematic decrease in emission energy for a decrease in growth temperature. Triple-axis x-ray diffraction (XRD), scanning electron microscopy, and cross-sectional transmission electron microscopy were used to obtain microstructural properties of different regions across the wafer. Results show that there is a decrease in crystal quality and an increase in V-defect formation with increasing indium concentration. A direct correlation was found between V-defect density and growth temperature due to increased strain and indium segregation for increasing indium concentration.     

Characterization of MOVPE-grown (Al, In, Ga) N heterostructures by quantitative analytical electron microscopy

The low pressure metalorganic vapor phase epitaxy growth of wurzite (Al, In, Ga)N heterostructures on sapphire substrates is investigated by quantitative analytical scanning transmission electron microscopy techniques like atomic number (Z-) contrast imaging and convergent beam electron diffraction (CBED). Especially (In, Ga)N quantum wells of different thicknesses as well as superlattices were analyzed with respect to defects, chemical composition variations, interface abruptness and strain (relaxation) effects. The interfaces in In_0.12Ga_0.88N/GaN quantum wells appear to be asymmetric. Additionally, we found composition variations of Δx_In≥0.03 within the InGaN quantum wells. The application of electron diffraction techniques (CBED) yields quantitative information on strain and relaxation effects. For the case of 17 nm thick InGaN quantum wells, we observed relaxation effects which are not present in the investigated thin quantum wells of 2 nm thickness. The experimentally obtained diffraction patterns were compared to simulations in order to get values for strain within the quantum wells. Additionally, the influence of dislocations on the digression of superlattices is investigated.     

In<Subscript>0.8</Subscript>Ga<Subscript>0.2</Subscript>As Quantum Dots for GaAs Solar Cells: Metal-Organic Vapor-Phase Epitaxy Growth Peculiarities and Properties

The growth peculiarities of In_0.8Ga_0.2As quantum dots and their arrays on GaAs surface by metalorganic vapor-phase epitaxy are investigated. The bimodal size distribution of In_0.8Ga_0.2As quantum dots is established from the photoluminescence spectra recorded at different temperatures. The growth parameters were determined at which the stacking of 20 In_0.8Ga_0.2As quantum-dot layers in the active area of a GaAs solar cell makes it possible to enhance the photogenerated current by 0.97 and 0.77 mA/cm² for space and terrestrial solar spectra, respectively, with the high quality of the p–n junction retained. The photogenerated current in a solar cell with quantum dots is higher than in the reference GaAs structure by ~1% with regard to nonradiative-recombination loss originating from stresses induced by the quantum-dot array.     

Ultrafast Dynamics of Photoexcited Charge Carriers in In<Subscript>0.53</Subscript>Ga<Subscript>0.47</Subscript>As/In<Subscript>0.52</Subscript>Al<Subscript>0.48</Subscript>As Superlattices under Femtosecond Laser Excitation

The results of experimental studies of the time dynamics of photoexcited charge carriers in In_0.53Ga_0.47As/In_0.52Al_0.48As superlattices grown by molecular-beam epitaxy on a GaAs substrate with a metamorphic buffer are reported. On the basis of the results of the numerical simulation of band diagrams, the optimal thickness of the In_0.52Al_0.48As barrier layer (4 nm) is chosen. At this thickness, the electron wave functions in In_0.53Ga_0.47As substantially overlap the In_0.52Al_0.48As barriers. This makes it possible to attain a short lifetime of photoexcited charge carriers (τ ~ 3.4 ps) at the wavelength λ = 800 nm and the pumping power 50 mW without doping of the In_0.53Ga_0.47As layer with beryllium. It is shown that an increase in the wavelength to λ = 930 nm (at the same pumping power) yields a decrease in the lifetime of photoexcited charge carriers to τ ~ 2 ps. This effect is attributed to an increase in the capture cross section of trapping states for electrons with lower energies and to a decrease in the occupancy of traps at lower excitation densities.     

Thermoelectric Properties of In<Subscript>0.3</Subscript>Ga<Subscript>0.7</Subscript>N Alloys

We report on the experimental investigation of the potential of InGaN alloys as thermoelectric (TE) materials. We have grown undoped and Si-doped In_0.3Ga_0.7N alloys by metalorganic chemical vapor deposition and measured the Seebeck coefficient and electrical conductivity of the grown films with the aim of maximizing the power factor (P). It was found that P decreases as electron concentration (n) increases. The maximum value for P was found to be 7.3 × 10⁻⁴ W/m K² at 750 K in an undoped sample with corresponding values of Seebeck coefficient and electrical conductivity of 280 μV/K and 93␣(Ω cm)⁻¹, respectively. Further enhancement in P is expected by improving the InGaN material quality and conductivity control by reducing background electron concentration.     

Optical properties of InAs<Subscript>1−x</Subscript>N<Subscript>x</Subscript>/In<Subscript>0.53</Subscript>Ga<Subscript>0.47</Subscript>As single quantum wells grown by gas source molecular beam epitaxy

Optical properties of InAs_1−xN_x/In_0.53Ga_0.47As (hereafter, abbreviated as InAsN/InGaAs) single quantum wells (SQWs) grown on InP substrates by gas source molecular-beam epitaxy are studied using photoluminescence (PL) measurements. By comparing the low-temperature PL spectra of InAs/InGaAs and InAsN/InGaAs SQWs, InAs and InAsN phases are found to coexist in the InAsN layer. Such serious alloy inhomogeneities result in obvious exciton localization by potential irregularities. The blue shift of the PL peak after rapid thermal annealing (RTA) is found to originate mainly from As-N interdiffusion inside the well layer. According to the temperature-dependent PL results, uniformity of the InAsN layer can be effectively improved by RTA, and the exciton localization is, thus, relieved. Comparison of luminescence quenching and excitation-power-dependent PL behavior between the QWs with and without nitrogen content suggests that the quality of the QW is degraded by the introduction of nitrogen, and the degradation can only be partially recovered by post-growth RTA.     

Preparation and structure of ultra-thin GaN (0001) layers on In0.11Ga0.89N-single quantum wells

Multiple surface reconstructions have been observed on ultra-thin GaN (0001) layers of 1–10 nm thickness, covering a 3 nm thick In_0.11Ga_0.89N single quantum well in a GaN matrix. Low energy electron diffraction patterns show (2×2) and (√3×√3)-R30° symmetries for samples annealed in nitrogen plasma, and (2×2), (3×3), (4×4), and (6×6) symmetries for samples overgrown with an additional monolayer-thin GaN film by molecular beam epitaxy under Ga-rich growth conditions. Photoelectron spectroscopy shows that the InGaN quantum wells and capping layers are stable for growth temperatures up to 760 °C, and do not show formation of indium or gallium droplets on the surface. The photoluminescence emission from the buried InGaN SQWs remains unchanged by the preparation process, demonstrating that the SQWs do not undergo any significant modification.     

Room-temperature photoluminescence of Ga<Subscript>0.96</Subscript>In<Subscript>0.04</Subscript>As<Subscript>0.11</Subscript>Sb<Subscript>0.89</Subscript> lattice matched to InAs

Photoluminescence (PL) has been observed at room temperature from a Ga_0.96In_0.04As_0.11Sb_0.89 quaternary solid solution for the first time. High-quality epitaxial layers of n-type (Te-doped) Ga_0.96In_0.04As_0.11Sb_0.89 with low In content were grown by liquid phase epitaxy (LPE) lattice-matched to InAs(100) substrates from a Ga-rich melt. The PL properties of the material were investigated over a wide temperature range, and the principal radiative transitions were identified. In the temperature range <150 K, donor-acceptor recombination involving the first and second ionization state of native antisite defects was the dominant radiative-recombination process, whereas interband recombination was found to dominate at room temperature.     

Bimodality in Arrays of In<Subscript>0.4</Subscript>Ga<Subscript>0.6</Subscript>As Hybrid Quantum-Confined Heterostructures Grown on GaAs Substrates

Hybrid quantum-confined heterostructures grown by metal-organic vapor-phase epitaxy (MOVPE) via the deposition of In_0.4Ga_0.6As layers with various nominal thicknesses onto vicinal GaAs substrates are studied by photoluminescence spectroscopy and transmission electron microscopy. The photoluminescence spectra of these structures show the superposition of two spectral lines, which is indicative of the bimodal distribution of the size and/or shape of light-emitting objects in an array. The dominant spectral line is attributed to the luminescence of hybrid “quantum well–dot” nanostructures in the form of a dense array of relatively small quantum dots (QDs) with weak electron and hole localization. The second, lower intensity line is attributed to luminescence from a less dense array of comparatively larger QDs. Analysis of the behavior of the spectral line intensities at various temperatures showed that the density of larger QDs grows with increasing thickness of the InGaAs layer.     

Time and temperature dependence on rapid thermal annealing of molecular beam epitaxy grown Ga<Subscript>0.8</Subscript>In<Subscript>0.2</Subscript>N<Subscript>0.01</Subscript>As<Subscript>0.99</Subscript> quantum wells analyzed using photoluminescence

GaInNAs has received a great deal of attention among the scientific community, owing to its ability to be grown pseudomorphically on GaAs substrates and, thus, to extend the possibility of using GaAs based materials for technologically important wavelengths such as 1.3 μm. Annealing was found to be a very useful tool in improving the optical characteristics of as-grown GaInNAs films. This work presents a systematic statistical analysis of two annealing parameters, time and temperature, for Ga_0.8In_0.2N_0.01As_0.99 quantum wells. Annealing, in general, has resulted in decreasing the emission wavelength by at most 0.08 μm, narrowing the peaks by at most ∼25 meV and increasing the intensity by at most 90 times. However, from the statistical analysis, it is observed that the temperature is the dominant factor among time and temperature in recovering the optical properties.     

Measurement of the absorption coefficient for light laterally propagating in light-emitting diode structures with In<Subscript>0.2</Subscript>Ga<Subscript>0.8</Subscript>N/GaN quantum wells

A procedure for measuring the absorption coefficient for light propagating parallel to the surface of a GaN-based light emitting diode chip on a sapphire substrate is suggested. The procedure implies the study of emission from one end face of the chip as the opposite end face is illuminated with a light emitting diode. The absorption coefficient is calculated from the ratio between the intensities of emission emerging from the end faces of the sapphire substrate and the epitaxial layer. From the measurements for chips based on p-GaN/In_0.2Ga_0.8N/n-GaN structures, the lateral absorption coefficient is determined at a level of (23 ± 3)cm^?1 at a wavelength of 465 nm. Possible causes for the discrepancy between the absorption coefficients determined in the study and those reported previously are analyzed.     

X-ray diffraction analysis and scanning micro-Raman spectroscopy of structural irregularities and strains deep inside the multilayered InGaN/GaN heterostructure

High-resolution X-ray diffraction analysis and scanning confocal Raman spectroscopy are used to study the spatial distribution of strains in the In _x Ga_{1 − x} N/GaN layers and structural quality of these layers in a multilayered light-emitting diode structure produced by metal-organic chemical vapor deposition onto (0001)-oriented sapphire substrates. It is shown that elastic strains almost completely relax at the heterointerface between the thick GaN buffer layer and In _x Ga_{1 − x} N/GaN buffer superlattice. It is established that the GaN layers in the superlattice are in a stretched state, whereas the alloy layers are in a compressed state. In magnitude, the stretching strains in the GaN layers are lower than the compressive strains in the InGaN layers. It is shown that, as compared to the buffer layers, the layers of the superlattice contain a smaller number of dislocations and the distribution of dislocations is more randomly disordered. In micro-Raman studies on scanning through the thickness of the multilayered structure, direct evidence is obtained for the asymmetric gradient distributions of strains and crystal imperfections of the epitaxial nitride layers along the direction of growth. It is shown that the emission intensity of the In _x Ga_{1 − x} N quantum well is considerably (more than 30 times) higher than the emission intensity of the GaN barrier layers, suggesting the high efficiency of trapping of charge carriers by the quantum well.     

Photosensitive structures based on In<Subscript>2</Subscript>S<Subscript>3</Subscript> crystals

Crystals of the compound In₂S₃ were grown by planar crystallization of the melt. The composition, structure, and electrical characteristics of the crystals obtained were determined. Photosensitive structures based on the grown In₂S₃ crystals were fabricated for the first time; spectral dependences of photoconversion quantum efficiency for H₂O/In₂S₃ cells were measured. The features of the band-to-band absorption are discussed; energies of the direct and indirect optical transitions for In₂S₃ crystals are estimated. It is stated that In₂S₃ crystals can be used in wide-range (1.5–3.5 eV) photoconverters of nonpolarized radiation (in particular, in solar cells).     

Mechanisms of photocurrent generation in In<Subscript>2</Subscript>O<Subscript>3</Subscript>-InSe heterojunctions

Spectral and integral characteristics of In₂O₃-InSe heterojunctions fabricated by oxidation of indium monoselenide substrates were studied. It was established that the photocurrent is determined by photo-generation of carriers in the space charge region of the structure via isolated deep levels.     

Very Low Pressure Magnetron Reactive Ion Etching of GaN and Al<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>Ga<Subscript>1−<Emphasis Type="Italic">x</Emphasis></Subscript>N Using Dichlorofluoromethane (Halocarbon 12)

In this work we report on the magnetron reactive ion etch (MRIE) technology for gallium nitride (GaN) and aluminum gallium nitride (Al _x Ga_1−x N) using dichlorodifluoromethane (CCl₂F₂), commonly known as halocarbon 12, with etch rates greater than 1,000 and 840 ?/min, respectively. Magnetic confinement of a very low pressure (10⁻⁴ Torr range) radio frequency (RF) discharge generates high-density plasmas, with low sheath voltages at the bounding surfaces, and very high dissociation of the source gas. Furthermore, the very low pressure of the etch process is characterized by long mean free paths so that sputtering contamination is reduced. MRIE chemistry has been monitored in situ by means of mass spectroscopy. Finally, we report on the successful fabrication of an indium gallium nitride (In _x Ga_1−x N) blue light emitting diode (LED), whose fabrication sequence included the MRIE etching of GaN in CCl₂F₂.     

Two Distinct Origins of Highly Localized Luminescent Centers within InGaN/GaN Quantum‐Well Light‐Emitting Diodes

The high light‐output efficiencies of In_xGa_1‐xN quantum‐well (QW)‐based light‐emitting diodes (LEDs) even in presence of a large number of nonradiative recombination centers (such as dislocations) has been explained by localization of carriers in radiative potential traps, the origins of which still remain unclear. To provide insights on the highly efficient radiative traps, spectrally resolved photoluminescence (PL) microscopy has been performed on green‐light‐emitting In_0.22Ga_0.78N QW LEDs, by selectively generating carriers in the alloy layers. PL imaging shows the presence of numerous inhomogeneously distributed low‐band‐gap traps with diverse radiative intensities. PL spectroscopy of a statistically relevant number of individual traps reveals a clear bimodal distribution in terms of both band‐gap energies and radiative recombination efficiencies, indicating the presence of two distinct classes of carrier localization centers within the same QW sample. Disparity in their relative surface coverage and photoemission “blinking” characteristics suggests that the deep traps originate from local compositional fluctuations of indium within the alloy, while the shallow traps arise from nanometer‐scale thickness variations of the active layers. This is further supported by Poisson–Schrödinger self‐consistent calculations and implies that radiative traps formed due to both local indium content and interface‐morphology‐related heterogeneities can coexist within the same QW sample.     

Microstructure and optical properties of In<Subscript>2</Subscript>S<Subscript>3</Subscript> films produced by thermal evaporation

The data on the influence of the microstructure of In₂S₃ films produced by thermal evaporation upon their optical properties in relation to the film’s thickness are reported. The atomic force spectroscopy data for the layers that are produced in identical technological conditions, but exhibit different spectral positions of the optical absorption edge are presented and discussed. Variations in the optical band gap from 2.0 to 3.6 eV under variations in the thickness of the In₂S₃ films from 800–450 nm to 50–30 nm are observed. The variations are interpreted as a result of variations in the content of grains, specific in dimensions and microstructure.     

Strain relaxation in InGaAs lattice engineered substrates

Strain relaxation of hypercritical thickness In_xGa_1−xAs layers has been observed during lateral oxidation of underlying AlAs layers. Strain relaxation of In_xGa_1−xAs layers was studied as a function of indium composition and the AlAs oxidation temperature. It is proposed that the enhanced strain relaxation is due to two factors. The first is enhanced motion of threading dislocations due to stresses generated during the lateral oxidation process. The second is the porous nature of the In_xGa_1−xAs/Al₂O₃ interface that minimizes the interaction of threading dislocations with existing misfit dislocation segments. The extent of strain relaxation increases with increasing oxidation temperature, whereas the efficiency of strain relaxation was found to decrease with increasing indium composition. The efficiency of strain relaxation upon oxidation can be improved by reducing the misfit dislocation density at the In_xGa_1−xAs/AlAs interface prior to oxidation and by changing the nature of the In_xGa_1−xAs/Al₂O₃ interface.