Stacking of multilayer InAs quantum dots with combination capping of InAlGaAs and high temperature grown GaAs

We are reporting the growth of multilayer stacks of quantum dots (10 periods) with a combination capping of In_0.21Al_0.21Ga_0.58As (30 Å) and GaAs (70–180 Å) grown by solid source molecular beam epitaxy (MBE). Reflection high energy electron diffraction (RHEED) has been used for the insitu monitoring of quantum dot (QD) formation in heterostructure samples. The samples were also characterized by other exsitu techniques like cross sectional transmission electron microscopy (XTEM) and photoluminescence measurements (PL). For a heterostructure sample with thin barrier thickness (<100 Å), an XTEM image showed the stacking of QDs only up to the 5th layer and in the upper layers there was hardly any formation of dots. We presume the stoppage of dot formation is due to the uneven surface of the InAlGaAs alloy overgrown on the InAs QDs, as a result of the local compositional deviations of the Group-III atoms. Samples grown with thicker barriers (>100 Å of GaAs) showed good stacking of islands until the tenth layer. The thick GaAs layer overgrown on the InAlGaAs at 590 ^°C is believed to remove the surface modifications of the quaternary layer thereby creating a smoother surface front for the growth of subsequent QD layers.     

Time-resolved photoluminescence spectroscopy of InAs quantum dots on InP with various InAlGaAs barrier thicknesses

The Optical characteristics of InAs quantum dots (QDs) embeded in InAlGaAs on InP have been investigated by photoluminescence (PL) spectroscopy and time-resolved PL. Four different QD samples are grown by using molecular beam epitaxy, and all the QD samples have five-stacked InAs quantum dot layers with a different InAlGaAs barrier thickness. The PL yield from InAs QDs was increased with an increase in the thickness of the InAlGaAs barrier, and the emission peak positions of all InAs QD samples were measured around 1.5 μm at room temperature. The decay time of the carrier in InAs QDs is decreased abruptly in the QD sample with the 5 nm InAlGaAs barrier. This feature is explained by the tunneling and coupling effect in the vertical direction and probably defect generation.     

Intrinsic and Mn doped InAs quantum dots studied at the atomic scale by cross-sectional scanning tunneling microscopy

Cross-sectional Scanning Tunneling Microscopy (X-STM) is an ideal tool to study the structural properties of semiconductor nanostructures, such as InAs self-assembled quantum dots (QDs) and the properties of individual doping atoms at the atomic scale. The technique allows for a precise determination of the size, shape and composition of overgrown semiconductor nanostructures which can be part of a (complex) multilayer structure. In this paper we discuss our recent results on InAs QD structures that were capped by various methods in order to control their size and shape. We will show that the capping process does strongly affect the final QD structure and thus forms a very important step in the dot formation process. Recently people have started to investigate magnetically doped QDs. We have used our X-STM technique to study the incorporation of single Mn-impurities in InAs/GaAs QDs.     

The emission wavelength tuning of InAs/InP quantum dots with thin GaAs, InGaAs, InP capping layers by MOCVD

InAs quantum dots (QDs) were grown on InP substrates by metalorganic chemical vapor deposition. The width and height of the dots were 50 and 5.8 nm, respectively on the average and an areal density of 3.0×10¹⁰ cm⁻² was observed by atomic force microscopy before the capping process. The influences of GaAs, In_0.53Ga_0.47As, and InP capping layers (5–10 ML thickness) on the InAs/InP QDs were studied. Insertion of a thin GaAs capping layer on the QDs led to a blue shift of up to 146 meV of the photoluminescence (PL) peak and an InGaAs capping layer on the QDs led to a red shift of 64 meV relative to the case when a conventional InP capping layer was used. We were able to tune the emission wavelength of the InAs QDs from 1.43 to 1.89 μm by using the GaAs and InGaAs capping layers. In addition, the full-width at half-maximum of the PL peak decreased from 79 to 26 meV by inserting a 7.5 ML GaAs layer. It is believed that this technique is useful in tailoring the optical properties of the InAs QDs at mid-infrared regime.     

The improvement of InAs/GaAs quantum dot properties capped by Graphene

InAs self‐assembled quantum dots (QDs) were grown by molecular beam epitaxy on (001) GaAs substrate. Uncapped and capped QDs with GaAs and graphene layers were studied using atomic force microscopy and Raman spectroscopy. Graphene multi‐layer was grown by chemical vapor deposition and transferred on InAs/GaAs QDs. It is well known that the presence of a cap layer modifies the size, shape, and density of the QDs. According to the atomic force microscopy study, in contrast to the GaAs capped sample, which induce a dramatic decrease of the density and height of dots, graphene cap layer sample presents a slight influence on the surface morphology and the density of the islands compared with the uncapped one. The difference shown in the Raman spectra of the samples is due to change of strain and alloy disorder effects on the QDs. Residuals strain and the relaxation coefficients have been investigated. All results confirm the best crystalline quality of the graphene cap layer dots sample relative to the GaAs capped one. So graphene can be used to replace GaAs in capping InAs/GaAs dots. To our knowledge, such study has not been carried out until now. Copyright © 2013 John Wiley & Sons, Ltd.     

Size-shrinkage effect of InAs quantum dots during a GaAs capping growth

The modification of the InAs quantum dots (QDs) by the GaAs capping growth was studied by using cross-sectional STEM and atomic force microscopy. In case of the GaAs capping growth at 450 °C, it was found that the lateral size of the InAs QDs significantly decreases rather than the height and that this size-shrinkage effect is enhanced for the large QDs. The shrinkage behavior is mainly attributed to the indium surface segregation, strongly depending on the surface strain of the QDs. The growth process of the GaAs capping layer plays an important role for achieving the size ordering of the embedded QDs.     

Inhibition of emission wavelength blueshift in annealed InAs/GaAs quantum dot stacks: an important observation for their potential application in photovoltaic devices

We have investigated the effect of post growth rapid thermal annealing on self-assembled InAs/GaAs multilayer QDs (MQD) overgrown with a combination barrier of InAlGaAs and GaAs for their possible use in photovoltaic device application. The samples were characterized by transmission electron microscopy and photoluminescence measurements. We noticed a thermally induced material interdiffusion between the QDs and the wetting layer in the MQD sample up to a certain annealing temperature. The QD heterostructure exhibited a thermal stability in the emission peak wavelength on annealing up to 700 ^°C temperature. A phenomenological model has been proposed for this stability of the emission peak. The model considers the effect of the strain field, propagating from the underlying QD layer to the upper layers of the multilayer QD and the effect of indium atom gradient in the combination barrier layer due to the presence of a quaternary InAlGaAs layer.     

Effects of Si-doped GaAs layer on optical properties of InAs quantum dots

We have investigated the optical properties of InAs self-assembled quantum dots (SAQDs) with the Si-doped GaAs barrier layer. Two types of samples are fabricated according to the position of the Si-doped GaAs layer. For type A samples the Si-doped GaAs layer is grown below the QDs, whereas for type B samples the Si-doped GaAs layer is grown above the QDs. For both types of samples the excited-state emissions caused by state filling are observed in photoluminescence (PL) spectra at high excitation power densities. The bandgap renormalization of QDs can be found from the shift of the PL peak energy. Particularly, for type A samples the Si atoms act as nucleation centers during the growth of InAs QDs on the Si-doped GaAs layer and affect the density and the size of the QDs. The Si-doped GaAs layer in type A samples has more effects on the properties of QDs, such as state filling and bandgap renormalization than those of type B samples.     

带有InGaAs覆盖层的InAs量子点红外探测器材料的发光与光电响应

利用分子束外延技术(MBE),在GaAs(001)衬底上自组织生长了不同结构的InAs量子点样品,并制备了量子点红外探测器件。利用原子力显微镜(AFM)和光致发光(PL)光谱研究了量子点的表面结构、形貌和光学性质。渐变InGaAs层的插入有效地释放了InAs量子点所受的应力,抑制了量子点中In组分的偏析,提高了外延层的生长质量,降低了势垒高度,使InAs量子点荧光波长红移。伏安特性曲线和光电流(PC)谱结果表明,生长条件的优化提高了器件的红外响应,具有组分渐变的InGaAs层的探测器响应波长发生明显红移。     

Comparison of single-layer and bilayer InAs/GaAs quantum dots with a higher InAs coverage

Epitaxially grown self-assembled InAs quantum dots (QDs) have found applications in optoelectronics. Efforts are being made to obtain efficient quantum-dot lasers operating at longer telecommunication wavelengths, specifically 1.3 μm and 1.55 μm. This requires narrow emission linewidth from the quantum dots at these wavelengths. In InAs/GaAs single layer quantum dot (SQD) structure, higher InAs monolayer coverage for the QDs gives rise to larger dots emitting at longer wavelengths but results in inhomogeneous dot-size distribution. The bilayer quantum dot (BQD) can be used as an alternative to SQDs, which can emit at longer wavelengths (1.229 μm at 8 K) with significantly narrow linewidth (∼16.7 meV). Here, we compare the properties of single layer and bilayer quantum dots grown with higher InAs monolayer coverage. In the BQD structure, only the top QD layer is covered with increased (3.2 ML) InAs monolayer coverage. The emission line width of our BQD sample is found to be insensitive towards post growth treatments.     

Formation process for and strain effect in InAs quantum dots grown on GaAs substrates by using molecular beam epitaxy

Reflection high-energy electron diffraction (RHEED) and atomic force microscopy (AFM) measurements were used to investigate the dependences of the formation process and the strain on the As/In ratio and the substrate temperature of InAs quantum dots (QDs) grown on GaAs substrates by using molecular beam epitaxy. The thickness of the InAs wetting layer and the shape and the size of the InAs QDs were significantly affected by the As/In ratio and the substrate temperature. The strains in the InAs layer and the GaAs substrate were studied by using RHEED patterns. The magnitude in strain of the InAs QDs formed at a low substrate temperature was larger than that in InAs QDs grown at high substrate temperature. The present results can help to improve the understanding of the formation process and the strain effect in InAs QDs.     

Thermal stability of quaternary alloy (InAlGaAs)-capped InAs/GaAs multilayer quantum dot heterostructures with variation in growth rate, barrier thickness, seed quantum dot monolayer coverage, and post-growth annealing

Strain-driven influences on the structural and optoelectronic properties of self-assembled InAs/GaAs multilayer quantum dot (MQD) heterostructures prompted our research into the growth of thermally stable MQD samples that were functional in an emission range technically favorable for communication lasers and intermediate band gap solar cells. We also studied parameter optimization by varying growth rate, capping layer thickness, seed quantum dot (QD) monolayer coverage, and post-growth annealing. A capping combination of InAlGaAs and i-GaAs was used. This combination helps in strain compensation, favors growth of multiple QD layers, functions as a strain-driven phase separation alloy, and helps increase QD stability. Photoluminescence results showed MQD sample emissions in the technologically significant range of 1.1–1.3 μm. Post-growth annealing at high temperatures led to inter-diffusion of the constituent QD materials, generation of low minimum energy states, and greater carrier involvement in intermediate band gap structures, thereby showing that annealing is a suitable method for post-growth manipulation. For one MQD sample, the annealing temperature was found to affect structural and optoelectronic properties as well as the presence of intermediate energy states. Heterostructure stability at annealing temperatures up to 750 ^°C was found for the other samples. Transmission electron microscopy and photoluminescence results supported these findings.     

Tuning vertically stacked InAs/GaAs quantum dot properties under spacer thickness effects for 1.3 μm emission

Coherent InAs islands separated by GaAs spacer (d) layers are shown to exhibit self-organized growth along the vertical direction. A vertically stacked layer structure is useful for controlling the size distribution of quantum dots. The thickness of the GaAs spacer has been varied to study its influence on the structural and optical properties. The structural and optical properties of multilayer InAs/GaAs quantum dots (QDs) have been investigated by atomic force microscopy (AFM), transmission electron microscopy (TEM), and photoluminescence (PL) measurements. The PL full width at half maximum (FWHM), reflecting the size distribution of the QDs, was found to reach a minimum for an inter-dots GaAs spacer layer thickness of 30 monolayers (ML). For the optimized structure, the TEM image shows that multilayer QDs align vertically in stacks with no observation of apparent structural defects. Furthermore, AFM images showed an improvement of the size uniformity of the QDs in the last layer of QDs with respect to the first one. The effect of growth interruption on the optical properties of the optimized sample (E30) was investigated by PL. The observed red shift is attributed to the evolution of the InAs islands during the growth interruption. We show the possibility of increasing the size of the QDs approaching the strategically important 1.3 m wavelength range (at room temperature) with growth interruption after InAs QD deposition.     

不同组分InxGa1-xAs(0≤x≤0.3)覆盖层对自组织InAs量子点的影响

研究了不同In组分的In_xGa_1-xAs(0≤x≤0.3)覆盖层对自组织InAs量子点的结构及发光特性的影响.透射电子显微镜和原子力显微镜表明,InAs量子点在InGaAs做盖层时所受应力较GaAs盖层时有所减小,并且x＝0.3时,InGaAs在InAs量子点上继续成岛.随x值的增大,量子点的光荧光峰红移,但随温度的变化发光峰峰位变化不明显.理论分析表明InAs量子点所受应力及其均匀性的变化分别是导致上述现象的主要原因. 关键词： 量子点 盖层 应力 红移     

Surface processes during growth of InAs/GaAs quantum dot structures monitored by reflectance anisotropy spectroscopy

The time resolved reflectance anisotropy spectroscopy (RAS) measurement at 4.2 eV was used for the optimization of technological parameters for Stranski–Krastanow quantum dot (QD) formation. TMIn dosage and waiting time following InAs deposition during which QD formation takes place were optimized.RAS measurement helps us to study the MOVPE surface processes such as QD formation, dissolution of In from InAs QDs during the growth of GaAs capping layer or recovery of epitaxial surface from As deficiency, when As partial pressure is increased. We have shown, that the recovery of epitaxial surface from As deficiency is rather a slow process of the order of tens of seconds.We have for the first time observed in situ the mechanism of In atoms migration from QDs during GaAs capping layer growth. First the GaAs layer is formed and then the In migration from QDs follows. These two processes do not start at the same time, the In dissolution is delayed. Conclusions extracted from RAS measurement are in agreement with photoluminescence results.     

Grid-pattern aligned InAs self-assembled quantum dots grown on InP substrate

We present a method to control the nucleation sites of InAs self-assembled quantum dots (QDs). Tensile-strained material, such as GaAs used here, was grown on InP substrates before InAs deposition. This thin GaAs layer can provide a surface with grid-pattern trenches which have the same function as atomic-steps and are promising for the formation of QDs with controlled nucleation sites. Atom force microscopy (AFM) measurement was performed and the AFM images indicate that the InAs islands grown with our technique are grid-pattern aligned and have good homogeneity and low size fluctuation. In addition, another kind of three-dimensional structure with larger size would coexist with normal QDs if a 30nm thick GaAs layer was deposited. This revised version was published online in June 2006 with corrections to the Cover Date.     

Self-organized formation of shell-like InAs/GaAs quantum dot ensembles

Formation of a multimodal quantum dot (QD) ensemble by strained layer epitaxy of InAs on GaAs near the critical value for the onset of the 2D-3D transition is studied. Reflection anisotropy spectroscopy is employed to confirm that a smooth surface is maintained during strained layer growth prior to QD formation. Instantaneous capping after deposition leads to InAs quantum wells with some thickness flucuations. Multimodal QD InAs ensembles form after an at least short growth interruption prior to cap layer deposition. The QDs consist of pure InAs with heights varying in steps of complete InAs monolayers. Related exciton energies indicate a simultaneous increase of both height and lateral extension, i.e. a shell-like increase of sizes. The formation of the multimodal QD ensemble is described by a kinetic approach. A growth scenario is presented where QDs having initially shorter base length stop vertical growth at a smaller height, accounting for the experimentally observed shell-like sub-ensemble structure.     

Sb-mediated growth of high-density InAs quantum dots and GaAsSb embedding growth by MBE

Self-assembled InAs quantum dots (QDs) with high-density were grown on GaAs(0 0 1) substrates by antimony (Sb)-mediated molecular beam epitaxy technique using GaAsSb/GaAs buffer layer and InAsSb wetting layer (WL). In this Sb-mediated growth, many two-dimensional (2D) small islands were formed on those WL surfaces. These 2D islands provide high step density and suppress surface migration. As the results, high-density InAs QDs were achieved, and photoluminescence (PL) intensity increased. Furthermore, by introducing GaAsSb capping layer (CL), higher PL intensity at room temperature was obtained as compared with that InGaAs CL.     

Effects of thermal annealing on the interband transitions of single and vertically stacked InAs/GaAs self-assembled quantum dots

Photoluminescence (PL) measurements have been carried out to investigate the annealing effects in one-period and three-periods of InAs/GaAs self-assembled quantum dots (QDs) grown on GaAs substrates by using molecular beam epitaxy. After annealing, the PL spectra for the annealed InAs/GaAs QDs showed dramatic blue shifts and significant linewidth narrowing of the PL peaks compared with the as-grown samples. The variations in the PL peak position and the full width at half-maximum of the PL peak are attributed to changes in the composition of the InAs QDs resulting from the interdiffusion between the InAs QDs and the GaAs barrier and to the size homogeneity of the QDs. These results indicate that the optical properties and the crystal qualities of InAs/GaAs QDs are dramatically changed by thermal treatment.     

Optical transitions of InAs/In0.36Ga0.64As/GaAs(311B) surface quantum dots clearly identified by the piezoreflectance technique

The bilayer InAs/In_0.36Ga_0.64As/GaAs(311B) quantum dots (QDs), including one InAs buried quantum dot (BQD) layer and the other InAs surface quantum dot (SQD) layer, have been grown by molecular beam epitaxy (MBE). The optical properties of these three samples have been studied by the piezoreflectance (PzR) spectroscopy. The PzR spectra do not exhibit only the optical transitions originated from the InAs BQDs, but the features originated from the InAs SQDs. After the InAs SQDs have been removed chemically, those optical transitions from InAs SQDs have been demonstrated clearly by investigating the PzR spectra of the residual InAs BQDs in these samples. The great redshift of these interband transitions of InAs SQDs has been well discussed. Due to the suitable InAs SQD sizes and the thickness of In_0.36Ga_0.64As layer, the interband transition of InAs SQDs has been shifted to ∼1.55 μm at 77 K.