InAs/GaAs quantum dots with wide-range tunable densities by simply varying V/III ratio using metal-organic chemical vapor deposition

The complicated behaviors of InAs/GaAs quantum dots with increasing V/III ratio associated with several competing mechanisms have been described. The results demonstrate that the densities of InAs quantum dots can be tuned in a wide range from 10⁵ to 10¹⁰ cm⁻² by simply manipulating V/III ratio via metal-organic chemical vapor deposition. These results are mainly ascribed to the changes of coverage and In adatom migration length due to the increasing V/III ratio.     

The influence of temperature on the photoluminescence properties of single InAs quantum dots grown on patterned GaAs

ABSTRACT: We report the temperature-dependent photoluminescence of single site-controlled and self-assembled InAs quantum dots. We have used nanoimprint lithography for patterning GaAs(100) templates and molecular beam epitaxy for quantum dot deposition. We show that the influence of the temperature on the photoluminescence properties is similar for quantum dots on etched nanopatterns and randomly positioned quantum dots on planar surfaces. The photoluminescence properties indicate that the prepatterning does not degrade the radiative recombination rate for the site-controlled quantum dots.     

Improved photoluminescence quantum yield of CsPbBr3 quantum dots glass ceramics

We have fabricated CsPbBr₃ perovskite quantum dots (QDs) in a multi-component borate glass by melt-quenching technique. Transmission electron microscopy (TEM) reveals a cubic phase CsPbBr₃ crystal for QDs. As the treatment temperature or the treatment time duration increases, the photoluminescence (PL) peak shifts to long wavelength in the range of 510 to 525 nm, and the full width at half-maximum varies in the range of 24 to 18 nm. The absorption edge shifts to low energy side in the range of 2.54 to 2.41 eV. The different photoluminescence excitation spectra (PLE) reflect the change of microstructure for different samples. The PL peak wavelength and line-shape are independent of excitation wavelength. These results of spectra show typical exciton emission characteristics. As treatment conditions strengthens, photoluminescence quantum yield (PLQY) first increases and then decreases, having the best PLQY 86.9%. Bi-exponential fitting curves show that short lifetime τ₁ continuously decreases. Long lifetime τ₂, weight for long lifetime component, and average lifetime τ_avg first increase and then decrease. The PLQY values are affected by both τ₁ and τ₂, which are relative to the crystal quality in the interior and the surface of QDs, respectively. The high PLQY value corresponds to medium treatment condition, which is attributed to a balanced effect of crystal quality in interior and the surface of QDs.     

Suppression of dislocations by Sb spray in the vicinity of InAs/GaAs quantum dots

The effect of Sb spray prior to the capping of a GaAs layer on the structure and properties of InAs/GaAs quantum dots (QDs) grown by molecular beam epitaxy (MBE) is studied by cross-sectional high-resolution transmission electron microscopy (HRTEM). Compared to the typical GaAs-capped InAs/GaAs QDs, Sb-sprayed QDs display a more uniform lens shape with a thickness of about 3 ~ 4 nm rather than the pyramidal shape of the non-Sb-sprayed QDs. Particularly, the dislocations were observed to be passivated in the InAs/GaAs interface region and even be suppressed to a large extent. There are almost no extended dislocations in the immediate vicinity of the QDs. This result is most likely related to the formation of graded GaAsSb immediately adjacent to the InAs QDs that provides strain relief for the dot/capping layer lattice mismatch.

PACS

81.05.Ea; 81.07.-b; 81.07.Ta     

Narrow ridge waveguide high power single mode 1.3-μm InAs/InGaAs ten-layer quantum dot lasers

Ten-layer InAs/In_0.15Ga_0.85As quantum dot (QD) laser structures have been grown using molecular beam epitaxy (MBE) on GaAs (001) substrate. Using the pulsed anodic oxidation technique, narrow (2 μm) ridge waveguide (RWG) InAs QD lasers have been fabricated. Under continuous wave operation, the InAs QD laser (2 × 2,000 μm²) delivered total output power of up to 272.6 mW at 10 °C at 1.3 μm. Under pulsed operation, where the device heating is greatly minimized, the InAs QD laser (2 × 2,000 μm²) delivered extremely high output power (both facets) of up to 1.22 W at 20 °C, at high external differential quantum efficiency of 96%. Far field pattern measurement of the 2-μm RWG InAs QD lasers showed single lateral mode operation.     

Multi-scale ordering of self-assembled InAs/GaAs(001) quantum dots

Ordering phenomena related to the self-assembly of InAs quantum dots (QD) grown on GaAs(001) substrates are experimentally investigated on different length scales. On the shortest length-scale studied here, we examine the QD morphology and observe two types of QD shapes, i.e., pyramids and domes. Pyramids are elongated along the [1–10] directions and are bounded by {137} facets, while domes have a multi-facetted shape. By changing the growth rates, we are able to control the size and size homogeneity of freestanding QDs. QDs grown by using low growth rate are characterized by larger sizes and a narrower size distribution. The homogeneity of buried QDs is measured by photoluminescence spectroscopy and can be improved by low temperature overgrowth. The overgrowth induces the formation of nanostructures on the surface. The fabrication of self-assembled nanoholes, which are used as a template to induce short-range positioning of QDs, is also investigated. The growth of closely spaced QDs (QD molecules) containing 2–6 QDs per QD molecule is discussed. Finally, the long-range positioning of self-assembled QDs, which can be achieved by the growth on patterned substrates, is demonstrated. Lateral QD replication observed during growth of three-dimensional QD crystals is reported.     

In situ accurate control of 2D-3D transition parameters for growth of low-density InAs/GaAs self-assembled quantum dots

A method to improve the growth repeatability of low-density InAs/GaAs self-assembled quantum dots by molecular beam epitaxy is reported. A sacrificed InAs layer was deposited firstly to determine in situ the accurate parameters of two- to three-dimensional transitions by observation of reflection high-energy electron diffraction patterns, and then the InAs layer annealed immediately before the growth of the low-density InAs quantum dots (QDs). It is confirmed by micro-photoluminescence that control repeatability of low-density QD growth is improved averagely to about 80% which is much higher than that of the QD samples without using a sacrificed InAs layer.     

Self-assembled InAs quantum dot formation on GaAs ring-like nanostructure templates

The evolution of InAs quantum dot (QD) formation is studied on GaAs ring-like nanostructures fabricated by droplet homo-epitaxy. This growth mode, exclusively performed by a hybrid approach of droplet homo-epitaxy and Stransky-Krastanor (S-K) based QD self-assembly, enables one to form new QD morphologies that may find use in optoelectronic applications. Increased deposition of InAs on the GaAs ring first produced a QD in the hole followed by QDs around the GaAs ring and on the GaAs (100) surface. This behavior indicates that the QDs prefer to nucleate at locations of high monolayer (ML) step density.     

Boron nitride quantum dots/polyvinyl butyral nanocomposite films for the enhanced photoluminescence and UV shielding properties

The present investigation focused on the effect of boron nitride quantum dots (BNQDs) as a filler on the optical properties of polyvinyl butyral (PVB) nanocomposites. Herein, polymer nanocomposite films with advanced UV protection and high photoluminescence properties were successfully synthesized. Polymer nanocomposite films were produced by adding BNQDs to the polymer in different ratios by a simple solution forming and casting method. The films were decomposed at different UV degradation times, and their UV protective properties were tested. The structural, morphological, optical and chemical interaction of BNQDs/PVB nanocomposites was confirmed by Scanning Electron Microscope (SEM), Transmission Electron Microscope (TEM), Fourier Transform Infrared (FTIR), micro-Raman spectroscopy, ultraviolet and visible (UV–Vis), and photoluminescence (PL) analyzes. As the amount of BNQDs in the polymer increased, the intensity of the bright images separated from the polymer also increased. TEM images confirmed the good distribution of quantum dots in PVB polymer matrix. Polymer composites doped with 0.25% and 0.4% BNQDs show excellent UV-shielding properties as the transmittance in the UV region decreased about 69% and 95%, respectively. As the addition of BNQDs into the polymer increased, the PL emission of the pure PVB film, which showed almost no emission, increased significantly.     

An analysis of Hall mobility in as-grown and annealed n- and p-type modulation-doped GaInNAs/GaAs quantum wells

In this study, we investigate the effect of annealing and nitrogen amount on electronic transport properties in n- and p-type-doped Ga_0.68In_0.32N_yAs_{1 − y}/GaAs quantum well (QW) structures with y = 0%, 0.9%, 1.2%, 1.7%. The samples are thermal annealed at 700°C for 60 and 600 s, and Hall effect measurements have been performed between 10 and 300 K. Drastic decrease is observed in the electron mobility of n-type N-containing samples due to the possible N-induced scattering mechanisms and increasing effect mass of the alloy. The temperature dependence of electron mobility has an almost temperature insensitive characteristic, whereas for p-type samples hole mobility is decreased drastically at T > 120 K. As N concentration is increased, the hole mobility also increased as a reason of decreasing lattice mismatch. Screening effect of N-related alloy scattering over phonon scattering in n-type samples may be the reason of the temperature-insensitive electron mobility. At low temperature regime, hole mobility is higher than electron mobility by a factor of 3 to 4. However, at high temperatures (T > 120 K), the mobility of p-type samples is restricted by the scattering of the optical phonons. Because the valance band discontinuity is smaller compared to the conduction band, thermionic transport of holes from QW to the barrier material, GaAs, also contributes to the mobility at high temperatures that results in a decrease in mobility. The hole mobility results of as-grown samples do not show a systematic behavior, while annealed samples do, depending on N concentration. Thermal annealing does not show a significant improvement of electron mobility.     

Influence of GaAs Substrate Orientation on InAs Quantum Dots: Surface Morphology, Critical Thickness, and Optical Properties

InAs/GaAs heterostructures have been simultaneously grown by molecular beam epitaxy on GaAs (100), GaAs (100) with a 2° misorientation angle towards [01−1], and GaAs (n11)B (n = 9, 7, 5) substrates. While the substrate misorientation angle increased from 0° to 15.8°, a clear evolution from quantum dots to quantum well was evident by the surface morphology, the photoluminescence, and the time-resolved photoluminescence, respectively. This evolution revealed an increased critical thickness and a delayed formation of InAs quantum dots as the surface orientation departed from GaAs (100), which was explained by the thermal-equilibrium model due to the less efficient of strain relaxation on misoriented substrate surfaces.     

Long-lasting photoluminescence quantum yield of cesium lead halide perovskite-type quantum dots

Cesium lead halide perovskite(CsPbX₃,X=Cl,Br,I)quantum dots(QDs)and their partly Mn²⁺-substituted QDs(CsPb1–xMnxX3)attract considerable attention owing to their unique photoluminescence(PL)efficiencies.The two types of QDs,having different PL decay dynamics,needed to be further investigated in a form of aggregates to understand their solid-state-induced exciton dynamics in conjunction with their behaviors upon degradation to achieve practical applications of those promising QDs.However,thus far,these QDs have not been sufficiently investigated to obtain deep insights related to the long-term stability of their PL properties as aggregated solid-states.Therefore,in this study,we comparatively examined CsPbX₃-and CsPb1–xMnxX₃-type QDs stocked for>50 d under dark ambient conditions by using excitation wavelength-dependent PL quantum yield and time-resolved PL spectroscopy.These investigations were performed with powder samples in addition to solutions to determine the influence of the inter-QD interaction of the aged QD aggregates on their radiative decays.It turns out that the Mn²⁺-substituted QDs exhibited long-lasting PL quantum efficiencies,while the unsubstituted CsPbX₃-type QDs exhibited a drastic reduction of their PL efficiencies.And the obtained PL traces were clearly sensitive to the sample status.This is discussed with the possible interaction depending on the size and distance of the QD aggregates.     

Long-wavelength room-temperature luminescence from InAs/GaAs quantum dots with an optimized GaAsSbN capping layer

An extensive study on molecular beam epitaxy growth conditions of quaternary GaAsSbN as a capping layer (CL) for InAs/GaAs quantum dots (QD) was carried out. In particular, CL thickness, growth temperature, and growth rate were optimized. Problems related to the simultaneous presence of Sb and N, responsible for a significant degradation of photoluminescence (PL), are thereby solved allowing the achievement of room-temperature (RT) emission. A particularly strong improvement on the PL is obtained when the growth rate of the CL is increased. This is likely due to an improvement in the structural quality of the quaternary alloy that resulted from reduced strain and composition inhomogeneities. Nevertheless, a significant reduction of Sb and N incorporation was found when the growth rate was increased. Indeed, the incorporation of N is intrinsically limited to a maximum value of approximately 1.6% when the growth rate is at 2.0 ML s⁻¹. Therefore, achieving RT emission and extending it somewhat beyond 1.3 μm were possible by means of a compromise among the growth conditions. This opens the possibility of exploiting the versatility on band structure engineering offered by this QD-CL structure in devices working at RT.

PACS

81.15.Hi (molecular beam epitaxy); 78.55.Cr (III-V semiconductors); 73.21.La (quantum dots)     

Impact of N on the atomic-scale Sb distribution in quaternary GaAsSbN-capped InAs quantum dots

The use of GaAsSbN capping layers on InAs/GaAs quantum dots (QDs) has recently been proposed for micro- and optoelectronic applications for their ability to independently tailor electron and hole confinement potentials. However, there is a lack of knowledge about the structural and compositional changes associated with the process of simultaneous Sb and N incorporation. In the present work, we have characterized using transmission electron microscopy techniques the effects of adding N in the GaAsSb/InAs/GaAs QD system. Firstly, strain maps of the regions away from the InAs QDs had revealed a huge reduction of the strain fields with the N incorporation but a higher inhomogeneity, which points to a composition modulation enhancement with the presence of Sb-rich and Sb-poor regions in the range of a few nanometers. On the other hand, the average strain in the QDs and surroundings is also similar in both cases. It could be explained by the accumulation of Sb above the QDs, compensating the tensile strain induced by the N incorporation together with an In-Ga intermixing inhibition. Indeed, compositional maps of column resolution from aberration-corrected Z-contrast images confirmed that the addition of N enhances the preferential deposition of Sb above the InAs QD, giving rise to an undulation of the growth front. As an outcome, the strong redshift in the photoluminescence spectrum of the GaAsSbN sample cannot be attributed only to the N-related reduction of the conduction band offset but also to an enhancement of the effect of Sb on the QD band structure.     

Influence of substrate orientation on exciton fine structure splitting of InAs/InP nanowire quantum dots

ABSTRACT: : In this paper, we use an atomistic approach to investigate strain distributions, single particle and many body electronic properties of InAs/InP nanowire quantum dots with substrate orientation varying from [111] to high-index [119], and compared with [001] case. We show that single particle gap for high-index [11k] substrates is increased with respect to [111] and [001] cases, and oscillates with the substrate index due to faceting effects. Surprisingly, the overall shell-like structure of single particle states is preserved even for highly facetted, high-index substrates. On the contrary, we demonstrate that besides two limiting high-symmetry cases, [001] and [111], the bright exciton splitting varies strongly with substrate orientation. For [112]-oriented substrate, the fine structure splitting reaches maximum due to crystal lattice anisotropy despite fully cylindrical isotropic shape of nanowire quantum dot.     

谷氨酰胺为稳定剂制备硒化镉纳米晶及光谱性质研究

以谷氨酰胺(Gln)为稳定剂合成了硒化镉纳米晶,利用X-射线粉末衍射(XRD)和透射电镜(TEM)对纳米晶结构进行了表征,粒径约为20 nm。通过紫外-可见吸收光谱、激发光谱与发射光谱研究了纳米晶光谱特性。实验结果表明,反应温度过高、反应时间过长都会破坏谷氨酰胺(Gln)的稳定作用,使CdSe聚集,影响其荧光性质。而聚乙二醇(PEG)的加入会使纳米晶的荧光发射明显加强,而且发射峰峰形尖锐。     

CdSe量子点标记免疫球蛋白及光谱性质研究

以巯基乙酸为稳定剂合成了CdSe量子点,利用X-射线粉末衍射(XRD)和透射电镜(TEM)对量子点结构进行了表征,粒径约为5 nm。以碳二亚胺为缩合剂将量子点与免疫球蛋白共价连接,光谱实验结果表明CdSe量子点与免疫球蛋白有效结合,其荧光发射峰发生了红移,而半峰宽和发射强度没有明显变化。     

Synthesis and characterisation of functional manganese doped ZnS quantum dots for bio-imaging application

Fluorescent quantum dots (QDs) are potential candidates for bio-imaging but major problems in using them for bio-imaging applications are either bandgap lying in UV region or the cytotoxicity of the visible light-excited cadmium-based QDs. Keeping these things in mind, glutathione (GLT) functionalised Mn-doped ZnS QDs has been studied to make a desired fluorescent system for bioimaging application. XRD measurements show that grain size decreases at higher concentration of GLT capping on Mn-doped quantum dots. UV–visible studies show that the band gap shows a blue shift at higher GLT concentration. FTIR studies confirm GLT functionalisation on the surface of ZnS QDs. Both UV excited and IR excited photoluminescence spectrum of samples exhibited a tunable orange emission intensity with increase in GLT concentration however multiphoton infrared excited spectra was used to show the feasibility of GLT functionalised ZnS:Mn quantum dots for a real application in a biological window of 650–950?nm.     

氮和硫双掺杂石墨烯量子点的合成及其性能研究

以来源丰富的大豆蛋白为前体,采用水热法和乙醇沉淀的分离方法合成了氮和硫双掺杂的石墨烯量子点（N,S-GQDs）。通过红外光谱（FTIR）、X射线光电子能谱（XPS）、紫外-可见光光谱（UV-vis）、高分辨率透射电镜（HRTEM）、原子力显微镜（AFM）和荧光光谱表征了N,S-GQDs的结构,及其对铁离子的检测性能。结果表明：大豆蛋白-柠檬酸-尿素水溶液在220℃水热温度下反应10 h,获得荧光量子效率为9.23%的N,S-GQDs,其水分散液具有明亮的蓝色荧光。N, S-GQDs具有0.34 nm的石墨烯晶格并展现出清晰的快速傅里叶变换图像,其厚度为2~5 nm。N, S-GQDs对Fe³⁺的检测限为0.95 μmol/L。本工作乙醇沉淀的简便方法将是一种快速获得N,S-GQDs固体的方法。     

木质素磺酸钙-石墨烯复合量子点的制备及性能

木质素磺酸盐是造纸工业主要副产物之一,本文利用木质素磺酸钙和柠檬酸为原料通过绿色简便的原位反应制备木质素磺酸钙/石墨烯复合量子点,利用荧光光谱、紫外可见光谱和透射电镜等研究了复合量子点的光学性能、结构模型和对金属离子的选择性吸附性能,结果表明该复合量子点的荧光强度是石墨烯量子点的4倍多,并且复合量子点可以选择性识别Fe³⁺,在10～500μmol/L范围内,Fe³⁺的浓度与复合量子点溶液的荧光强度有良好的线性关系,可应用于Fe³⁺的检测。此荧光探针制备简便,成本低廉,检测铁离子速度快,准确性高,选择性好,在离子检测方面有潜在的应用价值。