Electron microscopy of GaAs-based structures with InAs and As quantum dots separated by an AlAs barrier

Electron microscopy studies of GaAs-based structures grown by molecular beam epitaxy and containing arrays of semiconductor InAs quantum dots and metal As quantum dots are performed. The array of InAs quantum dots is formed by the Stranski-Krastanov mechanism and consists of vertically coupled pairs of quantum dots separated by a GaAs spacer 10 nm thick. To separate the arrays of semiconductor and metal quantum dots and to prevent diffusion-induced mixing, the array of InAs quantum dots is overgrown with an AlAs barrier layer 5 or 10 nm thick, after which a GaAs layer is grown at a comparatively low temperature (180°C). The array of As quantum dots is formed in an As-enriched layer of the low-temperature GaAs by means of post-growth annealing at 400–760°C for 15 min. It is established that the AlAs barrier layer has a surface profile corresponding to that of a subbarrier layer with InAs quantum dots. The presence of such a profile causes the formation of V-shaped structural defects upon subsequent overgrowth with the GaAs layer. Besides, it was obtained that AlAs layer is thinned over the InAs quantum dots tops. It is shown that the AlAs barrier layer in the regions between the InAs quantum dots effectively prevents the starting diffusion of excess As at annealing temperatures up to 600°C. However, the concentration of mechanical stresses and the reduced thickness of the AlAs barrier layer near the tops of the InAs quantum dots lead to local barrier breakthroughs and the diffusion of As quantum dots into the region of coupled pairs of InAs quantum dots at higher annealing temperatures.     

GaAs structures with InAs and As quantum dots produced in a single molecular beam epitaxy process

Epitaxial GaAs layers containing InAs semiconductor quantum dots and As metal quantum dots are grown by molecular beam epitaxy. The InAs quantum dots are formed by the Stranskii-Krastanow mechanism, whereas the As quantum dots are self-assembled in the GaAs layer grown at low temperature with a large As excess. The microstructure of the samples is studied by transmission electron microscopy. It is established that the As metal quantum dots formed in the immediate vicinity of the InAs semiconductor quantum dots are larger in size than the As quantum dots formed far from the InAs quantum dots. This is apparently due to the effect of strain fields of the InAs quantum dots upon the self-assembling of As quantum dots. Another phenomenon apparently associated with local strains around the InAs quantum dots is the formation of V-like defects (stacking faults) during the overgrowth of the InAs quantum dots with the GaAs layer by low-temperature molecular beam epitaxy. Such defects have a profound effect on the self-assembling of As quantum dots. Specifically, on high-temperature annealing needed for the formation of large-sized As quantum dots by Ostwald ripening, the V-like defects bring about the dissolution of the As quantum dots in the vicinity of the defects. In this case, excess arsenic most probably diffuses towards the open surface of the sample via the channels of accelerated diffusion in the planes of stacking faults.     

Electron microscopy of GaAs Structures with InAs and as quantum dots

An electron-microscopy study of GaAs structures, grown by molecular-beam epitaxy, containing two coupled layers of InAs semiconductor quantum dots (QDs) overgrown with a thin buffer GaAs layer and a layer of low-temperature-grown gallium arsenide has been performed. In subsequent annealing, an array of As nanoinclusions (metallic QDs) was formed in the low-temperature-grown GaAs layer. The variation in the microstructure of the samples during temperature and annealing conditions was examined. It was found that, at comparatively low annealing temperatures (400–500°C), the formation of the As metallic QDs array weakly depends on whether InAs semiconductor QDs are present in the preceding layers or not. In this case, the As metallic QDs have a characteristic size of about 2–3 nm upon annealing at 400°C and 4–5 nm upon annealing at 500°C for 15 min. Annealing at 600°C for 15 min in the growth setup leads to a coarsening of the As metallic QDs to 8–9 nm and to the formation of groups of such QDs in the area of the low-temperature-grown GaAs which is directly adjacent to the buffer layer separating the InAs semiconductor QDs. A more prolonged annealing at an elevated temperature (760°C) in an atmosphere of hydrogen causes a further increase in the As metallic QDs’ size to 20–25 nm and their spatial displacement into the region between the coupled InAs semiconductor QDs.     

Effect of a low-temperature-grown GaAs layer on InAs quantum-dot photoluminescence

The photoluminescence of InAs semiconductor quantum dots overgrown by GaAs in the low-temperature mode (LT-GaAs) using various spacer layers or without them is studied. Spacer layers are thin GaAs or AlAs layers grown at temperatures normal for molecular-beam epitaxy (MBE). Direct overgrowth leads to photoluminescence disappearance. When using a thin GaAs spacer layer, the photoluminescence from InAs quantum dots is partially recovered; however, its intensity appears lower by two orders of magnitude than in the reference sample in which the quantum-dot array is overgrown at normal temperature. The use of wider-gap AlAs as a spacer-layer material leads to the enhancement of photoluminescence from InAs quantum dots, but it is still more than ten times lower than that of reference-sample emission. A model taking into account carrier generation by light, diffusion and tunneling from quantum dots to the LT-GaAs layer is constructed.     

Molecular beam epitaxy of AlGaAs/Zn(Mn)Se hybrid nanostructures with InAs/AlGaAs quantum dots near the heterovalent interface

Features of the growth of InAs quantum dots in an Al_0.35Ga_0.65As matrix by molecular beam epitaxy at different substrate temperatures, deposition rates, and amounts of deposited InAs are studied. The optimum conditions for growing an array of low-density (≤2 × 10¹⁰ cm^?2) small (height of no more than 4 nm) self-organized quantum dots are determined. The possibility of the formation of optically active InAs quantum dots emitting in the energy range 1.3–1.4 eV at a distance of no more than 10 nm from the coherent heterovalent GaAs/ZnSe interface is demonstrated. It is established that inserting an optically inactive 5-nm GaAs quantum well resonantly coupled with InAs quantum dots into the upper AlGaAs barrier layer enhances the photoluminescence efficiency of the quantum-dot array in hybrid heterostructures.     

Formation of a step-free InAs quantum well selectively grown on a GaAs (111)B substrate

We investigated the possibility of forming a step-free quantum well structure. A step-free InAs monolayer was grown on a selectively grown mesa by controlling surface phases with in-situ monitoring of surface photo-absorption. We selectively grew a GaAs buffer at 800°C and cooled the sample keeping the (2×2)-like As stabilized surface. Atomic force microscopy (AFM) observation demonstrated that fully step-free surfaces were formed on the 8 μm wide mesa. Then, a monolayer-thick InAs was formed on this step-free surface and this InAs layer was capped by GaAs under the (2×2)-like condition. The quantum level of the step-free InAs layer was evaluated by spatially resolved photoluminescence (μPL) measurement. Uniform PL intensity and the lack of a double layer peak indicated the formation of a step-free InAs quantum well, which was in good agreement with AFM observation.     

The sandwich InGaAs/GaAs quantum dot structure for IR photoelectric detectors

A new possibility for growing InAs/GaAs quantum dot heterostructures for infrared photoelectric detectors by metal-organic vapor-phase epitaxy is discussed. The specific features of the technological process are the prolonged time of growth of quantum dots and the alternation of the low-and high-temperature modes of overgrowing the quantum dots with GaAs barrier layers. During overgrowth, large-sized quantum dots are partially dissolved, and the secondary InGaAs quantum well is formed of the material of the dissolved large islands. In this case, a sandwich structure is formed. In this structure, quantum dots are arranged between two thin layers with an increased content of indium, namely, between the wetting InAs layer and the secondary InGaAs layer. The height of the quantum dots depends on the thickness of the GaAs layer grown at a comparatively low temperature. The structures exhibit intraband photoconductivity at a wavelength around 4.5 μm at temperatures up to 200 K. At 90 K, the photosensitivity is 0.5 A/W, and the detectivity is 3 × 10⁹ cm Hz^1/2W^?1.     

The influence of heat treatment conditions on the evaporation of defect regions in structures with InGaAs quantum dots in the GaAs matrix

Structures with In(Ga)As quantum dots in the GaAs matrix obtained using molecular-beam epitaxy are investigated using photoluminescence (PL) measurements and transmission electron microscopy. The structures were subjected in situ to the procedure of the selective thermal elimination of defect regions. Based on the results of the analysis of luminescence properties, a method for evaluating the crystalline quality of structures using the measurements of PL intensity for the GaAs matrix at high temperatures (as high as 400 K) is suggested. Procedures for the elimination of defects are investigated, namely, the single-stage selective elimination of InAs defect islands at 600°C and a two-stage procedure. The latter procedure additionally includes selective overgrowth with a thin AlAs layer and high-temperature (650–700°C) heat treatment. The optimal conditions of the process, which permit the obtaining of structures with a relatively low defect density without a considerable decrease in the density of coherent quantum dots, are found.     

Capacitance spectroscopy of deep states in InAs/GaAs quantum dot heterostructures

The results of a study of a structure with a single array of InAs quantum dots in a GaAs matrix using capacitance-voltage measurements, deep-level transient spectroscopy (DLTS), photoluminescence spectroscopy, and transmission electron microscopy are reported. Clusters of interacting bistable defects are discovered in GaAs layers grown at low temperature. Controllable and reversible metastable populating of quantum-dot energy states and monoenergetic surface states, which depends on the temperature and conditions of a preliminary isochronal anneal, is observed. This effect is associated with the presence of bistable traps with self-trapped holes. The DLTS measurements reveal variation of the energy for the thermal ionization of holes from surface states of the InAs/GaAs heterointerface and the wetting layer as the reverse bias voltage is increased. It is theorized that these changes are caused by the built-in electric field of a dipole, which can be formed either by wetting-layer holes or by ionized levels located near the heterointerface. Fiz. Tekh. Poluprovodn. 33, 184–193 (February 1999)     

Optimization of the temperature mode of metal-organic chemical vapor deposition of the InAs(N) quantum dots on GaAs (001) with intense photoluminescence at 1.3 μm

The growth of the InAs(N) quantum dots on GaAs in a reduced-pressure reactor of metal-organic chemical vapor deposition (MOCVD) is studied. As the nitrogen source, dimethylhydrazine is used. It is currently well-known that the growth temperature of the InGaAs quantum dots should be limited in order to avoid undesirable In and Ga interdiffusion as well as reevaporation of In. However, thick GaAs barrier layers should be grown at the elevated temperature because of the pronounced effect of the growth temperature on the optical quality of the structure. An increase in the temperature of the substrate holder by 100°C requires interrupting the process in the MOCVD reactor for approximately 2 min. The time of this interruption for the temperature rise can come at various stages of the process, namely, (i) after growing the quantum dots and prior to growing the InGaAs coating layer, (ii) during the growth of the coating layer, (iii) after growing the coating layer and before growing the GaAs barrier layer, and (iv) during the growth of the GaAs barrier layer. It is shown that the last variant is the most appropriate for the structures with intense photoluminescence at 1.3 μm. In this case, the thin initial part of the barrier layer is grown under reduced temperature.     

Formation of dislocation defects in the process of burying of InAs quantum dots into GaAs

Evidence given by electron microscopy of dislocation relaxation of stresses near InAs quantum dots buried into GaAs is presented. It was found that dislocation defects not emerging to the film surface are formed in some buried quantum dots. This suggests that stress relaxation occurs in the buried state of the quantum dot, rather than at the stage of the formation and growth of an InAs island on the GaAs surface. Models of internal dislocation relaxation of buried quantum dots are presented.     

The effects of quantum dot coverage in InAs/(In)GaAs nanostructures for long wavelength emission

We present a study on the effects of quantum dot coverage on the properties of InAs dots embedded in GaAs and in metamorphic In_0.15Ga_0.85As confining layers grown by molecular beam epitaxy on GaAs substrates. We show that redshifted emission wavelengths exceeding 1.3 μm at room temperature were obtained by the combined use of InGaAs confining layers and high quantum dot coverage. The use of high InAs coverage, however, leads to detrimental effects on the optical and electrical properties of the structures. We relate such behaviour to the formation of extended structural defects originating from relaxed large-sized quantum dots that nucleate in accordance to thermodynamic equilibrium theories predicting the quantum dot ripening. The effect of the reduced lattice-mismatch of InGaAs metamorphic layers on quantum dot ripening is discussed in comparison with the InAs/GaAs system.     

The effect of misorientation of the GaAs substrate on the properties of InAs quantum dots grown by low-temperature molecular beam epitaxy

The structural and optical properties of arrays of InAs quantum dots grown on GaAs substrates at relatively low temperatures (250 and 350°C) and with various degrees of misorientation of the surface are studied. It is shown that low-temperature growth is accompanied by the formation of quantum dot clusters along the dislocation loops on the singular surface and along the steps caused by the surface vicinality on the misoriented surface. The formation of quantum dot clusters leads to the appearance of a new long-wavelength band in the exciton photoluminescence (PL) spectra. It is found that the degrees of polarization of the PL spectral band for clusters of various shapes are different.     

Study of multilayer structures with InAs nanoobjects in a silicon matrix

MBE-grown multilayer structures with InAs quantum dots embedded in a crystalline silicon matrix were studied by high resolution transmission electron microscopy. The properties of the grown structures depend critically on the substrate temperature, growth cycle sequence, and layer thicknesses. It is shown that the silicon matrix can “accommodate” only a limited volume of InAs in the form of coherent clusters about 3 nm in size. With an increasing amount of deposited InAs, large dislocated InAs clusters are formed during Si overgrowth, accumulating excess InAs.     

GaAs基上的InAs量子环制备

在分子束外延系统中,利用3nmGaAs薄盖层将InAs自组装量子点部分覆盖,然后在500°C以及As2气氛中退火一分钟,制成纳米尺度的InAs量子环。这一形成敏感地依赖于退火时的生长条件和生长InAs自组装量子点时的淀积量。InAs在GaAs表面的扩散以及同时发生的In-Ga互混控制着InAs量子环的形成。     

Optoelectronic properties of heteronanostructures with combined layers of In(Ga)As/GaAs quantum wells and dots

The effect of the incorporation of an InGaAs quantum well into structures with InAs/GaAs quantum dots grown by gas-phase epitaxy on their optoelectronic properties is analyzed in the mode with increased growth-interruption time. It is established that the quantum-dot energy spectrum is weakly sensitive to variations in the thickness and composition of the double InGaAs/GaAs coating layer. The deposition of a quantum well onto a layer of quantum dots decreases the emission-barrier effective height in them. The conditions under which the quantum well can be used for protecting the quantum-dot active layer against penetration by defects generated during structure-surface anodic oxidation are determined.     

自组织生长单层InAs量子点结构中浸润层与量子点发光的时间分辨谱研究

在GaAs(100)的衬底上，采用MBE自组织方法生长了单层层厚分别为2和2．5ML的InAs层。通过原子力显微镜(AFM)观察，证实已在InAs层中形成量子点。采用光致发光谱及时间分辨谱对InAs量子点及浸润层开展研究和对比，分析了单层InAs量子点和浸润层中的载流子迁移过程，较好地解释了实验结果。     

Localization of holes in an InAs/GaAs quantum-dot molecule

Deep-level transient spectroscopy is used to study the emission of holes from the states of a vertically coupled system of InAs quantum dots in p-n InAs/GaAs heterostructures. This emission was considered in relation to the thickness of a GaAs interlayer between two layers of InAs quantum dots and to the reversebias voltage U_r. It is established that hole localization at one of the quantum dots is observed for a quantum-dot molecule composed of two vertically coupled self-organized quantum dots in an InAS/GaAs heterostructure that has a 20-Å-thick or 40-Å-thick GaAs interlayer between two layers of InAs quantum dots. For a thickness of the GaAs interlayer equal to 100 Å, it is found that the two layers of quantum dots are incompletely coupled, which results in a redistribution of the hole localization between the upper and lower quantum dots as the voltage U_r applied to the structure is varied. The studied structures with vertically coupled quantum dots were grown by molecular-beam epitaxy using self-organization effects.     

Photoluminescence up to 1.6 μm of quantum dots with an increased effective thickness of the InAs layer

Multilayered InAs/GaAs quantum dot (QD) heterostructures are produced by metal-organic gas phase epitaxy. The structures exhibit photoluminescence around 1.55 μm at 300 K. The specific feature of the technology is the growth of an InAs layer with an increased effective thickness d _eff to form QDs, in combination with low-temperature overgrowth of the QDs with a thin (6-nm) GaAs layer and with the annelaing of defects. By X-ray diffraction analysis and PL studies, it is shown that, in a structure with the increased thickness d _eff, a secondary wetting InGaAs layer is produced on top of the QD layer from the growing relaxed large-sized InAs clusters on annealing. A new mechanism of formation of large-sized QDs characterized by a large “aspect ratio” is suggested. The mechanism involves the 2D–3D transformation of the secondary InGaAs layer in the field of elastic strains in previously formed QDs. The specific feature of the array of QDs is the coexistence of three populations of different-sized QDs responsible for the multimode photoluminescence in the range from 1 to 1.6 μm. The potentialities of such structures for infrared photoelectric detectors operating in the range from 1–2.5 μm at room temperature are analyzed.     

自组织量子点的优化生长

在不同生长条件下,生长低组分InGaAs/GaAs自组织量子点并且使用接触式AFM进行测量.通过对生长条件的优化,得到高密度、高均匀性的量子点MBE生长条件,这对于自组织量子点在器件方面的应用,比如量子点红外探测器和量子点激光器,是非常重要的.同时,还与优化的InAs/GaAs生长条件进行了比较.