Single-dot Spectroscopy of GaAs Quantum Dots Fabricated by Filling of Self-assembled Nanoholes

We study the optical emission of single GaAs quantum dots (QDs). The QDs are fabricated by filling of nanoholes in AlGaAs and AlAs which are generated in a self-assembled fashion by local droplet etching with Al droplets. Using suitable process parameters, we create either uniform QDs in partially filled deep holes or QDs with very broad size distribution in completely filled shallow holes. Micro photoluminescence measurements of single QDs of both types establish sharp excitonic peaks. We measure a fine-structure splitting in the range of 22–40μeV and no dependence on QD size. Furthermore, we find a decrease in exciton–biexciton splitting with increasing QD size.     

Change in properties of coated cadmium-tellurium quantum dots after heat treatment

The effects of heat treatment using an electronic furnace on the morphology of thin-film CdTe quantum dots (QDs) grown on glass substrates was investigated. The photoluminescence properties of CdTe QDs were found to depend on the size of QDs; photoemission was found to deteriorate, and sometimes, get completely lost with the change in QD size. Generally during the synthesis, QD size can be controlled by controlling the reflux time. However, since reflux temperature could not be increased beyond 100°C, we focused on heat treatment after synthesis. Therefore, the properties of fabricated QD solutions could be changed with additional heat treatment.     

Selective area epitaxy of ultra-high density InGaN quantum dots by diblock copolymer lithography

Highly uniform InGaN-based quantum dots (QDs) grown on a nanopatterned dielectric layer defined by self-assembled diblock copolymer were performed by metal-organic chemical vapor deposition. The cylindrical-shaped nanopatterns were created on SiN _x layers deposited on a GaN template, which provided the nanopatterning for the epitaxy of ultra-high density QD with uniform size and distribution. Scanning electron microscopy and atomic force microscopy measurements were conducted to investigate the QDs morphology. The InGaN/GaN QDs with density up to 8 × 10¹⁰ cm^-2 are realized, which represents ultra-high dot density for highly uniform and well-controlled, nitride-based QDs, with QD diameter of approximately 22-25 nm. The photoluminescence (PL) studies indicated the importance of NH₃ annealing and GaN spacer layer growth for improving the PL intensity of the SiN _x -treated GaN surface, to achieve high optical-quality QDs applicable for photonics devices.     

Self-assembled GaInNAs/GaAsN quantum dot lasers: solid source molecular beam epitaxy growth and high-temperature operation

Self-assembled GaInNAs quantum dots (QDs) were grown on GaAs (001) substrate using solid-source molecular-beam epitaxy (SSMBE) equipped with a radio-frequency nitrogen plasma source. The GaInNAs QD growth characteristics were extensively investigated using atomic-force microscopy (AFM), photoluminescence (PL), and transmission electron microscopy (TEM) measurements. Self-assembled GaInNAs/GaAsN single layer QD lasers grown using SSMBE have been fabricated and characterized. The laser worked under continuous wave (CW) operation at room temperature (RT) with emission wavelength of 1175.86 nm. Temperature-dependent measurements have been carried out on the GaInNAs QD lasers. The lowest obtained threshold current density in this work is ∼1.05 kA/cm² from a GaInNAs QD laser (50 × 1,700 μm²) at 10 °C. High-temperature operation up to 65 °C was demonstrated from an unbonded GaInNAs QD laser (50 × 1,060 μm²), with high characteristic temperature of 79.4 K in the temperature range of 10–60 °C.     

Submonolayer Quantum Dots for High Speed Surface Emitting Lasers

We report on progress in growth and applications of submonolayer (SML) quantum dots (QDs) in high-speed vertical-cavity surface-emitting lasers (VCSELs). SML deposition enables controlled formation of high density QD arrays with good size and shape uniformity. Further increase in excitonic absorption and gain is possible with vertical stacking of SML QDs using ultrathin spacer layers. Vertically correlated, tilted or anticorrelated arrangements of the SML islands are realized and allow QD strain and wavefunction engineering. Respectively, both TE and TM polarizations of the luminescence can be achieved in the edge-emission using the same constituting materials. SML QDs provide ultrahigh modal gain, reduced temperature depletion and gain saturation effects when used in active media in laser diodes. Temperature robustness up to 100 °C for 0.98 μm range vertical-cavity surface-emitting lasers (VCSELs) is realized in the continuous wave regime. An open eye 20 Gb/s operation with bit error rates better than 10⁻¹² has been achieved in a temperature range 25–85 °C without current adjustment. Relaxation oscillations up to ∼30 GHz have been realized indicating feasibility of 40 Gb/s signal transmission. A. V. Savel’ev—on leave from the Abraham Ioffe Physical Technical Institute, Politekhnicheskaya 26, 194021, St. Petersburg, Russia.     

Interaction and Cooperative Nucleation of InAsSbP Quantum Dots and Pits on InAs(100) Substrate

An example of InAsSbP quaternary quantum dots (QDs), pits and dots–pits cooperative structures’ growth on InAs(100) substrates by liquid phase epitaxy (LPE) is reported. The interaction and surface morphology of the dots–pits combinations are investigated by the high-resolution scanning electron microscope. Bimodal growth mechanism for the both QDs and pits nucleation is observed. Cooperative structures consist of the QDs banded by pits, as well as the “large” pits banded by the quantum wires are detected. The composition of the islands and the pits edges is found to be quaternary, enriched by antimony and phosphorus, respectively. This repartition is caused by dissociation of the wetting layer, followed by migration (surface diffusion) of the Sb and P atoms in opposite directions. The “small” QDs average density ranges from 0.8 to 2 × 10⁹ cm⁻², with heights and widths dimensions from 2 to 20 nm and 5 to 45 nm, respectively. The average density of the “small” pits is equal to (6–10) × 10⁹ cm⁻² with dimensions of 5–40 nm in width and depth. Lifshits–Slezov-like distribution for the amount and surface density of both “small” QDs and pits versus their average diameter is experimentally detected. A displacement of the absorption edge toward the long wavelength region and enlargement toward the short wavelength region is detected by the Fourier transform infrared spectrometry.     

InGaN/GaN multilayer quantum dots yellow-green light-emitting diode with optimized GaN barriers

InGaN/GaN multilayer quantum dot (QD) structure is a potential type of active regions for yellow-green light-emitting diodes (LEDs). The surface morphologies and crystalline quality of GaN barriers are critical to the uniformity of InGaN QD layers. While GaN barriers were grown in multi-QD layers, we used improved growth parameters by increasing the growth temperature and switching the carrier gas from N₂ to H₂ in the metal organic vapor phase epitaxy. As a result, a 10-layer InGaN/GaN QD LED is demonstrated successfully. The transmission electron microscopy image shows the uniform multilayer InGaN QDs clearly. As the injection current increases from 5 to 50 mA, the electroluminescence peak wavelength shifts from 574 to 537 nm.     

Growth of PbSe Quantum Dots Within High‐Index Lead‐Phosphate Glass for Infrared Saturable Absorbers

PbSe quantum dots (QDs) were grown in high‐refractive‐index low‐melting‐temperature lead‐phosphate glass. The lowest energy exciton transition of the QDs was tuned over a wide range within the infrared spectral region (0.93–2.75 μm) by a controlled heat treatment. The measured QD radius ranged between 2 and 5.3 nm, with a time (t) dependence of t^0.29 for long dwelling times during the heat treatment, indicating that the QD growth mechanism tends to follow Lifshitz‐Slyozov‐Wagner theory. The QD saturable absorber behavior at 1.2 μm had a measured saturation fluence of ~2.1 μJ/cm².     

The effect of thin gap insertion layer on InP nanostructure grown by metal–organic vapour phase epitaxys

The effect of thin GaP insertion layers on the structural and optical properties of InP/In_0.49Ga_0.51P self‐assembled quantum dots (SAQDs) on GaAs (001) substrate grown by metal–organic vapour phase epitaxy has been reported. The properties of InP/In_0.49Ga_0.51P SAQDs are modified when a thin (1–4 ML) GaP layer is inserted underneath the InP quantum dots (QDs). Deposition of the GaP insertion layer affects the dot dimension and improves the size uniformity. The density, dimension and uniformity of InP QDs strongly depend on the GaP insertion layer thickness. This variation in QD size is a result of a material nucleation effect caused by atomic intermixing between the InP QDs and underlying GaP insertion layer and surface energy. The insertion of GaP layer led to tuning the emission wavelength and narrowing of full width at half maximum (FWHM) when they are characterised by PL measurements at room temperature. © 2012 Canadian Society for Chemical Engineering     

Optical properties of as-grown and annealed InAs quantum dots on InGaAs cross-hatch patterns

InAs quantum dots (QDs) grown on InGaAs cross-hatch pattern (CHP) by molecular beam epitaxy are characterized by photoluminescence (PL) at 20 K. In contrast to QDs grown on flat GaAs substrates, those grown on CHPs exhibit rich optical features which comprise as many as five ground-state emissions from [1-10]- and [110]-aligned QDs, two wetting layers (WLs), and the CHP. When subject to in situ annealing at 700°C, the PL signals rapidly degrades due to the deterioration of the CHP which sets the upper limit of overgrowth temperature. Ex situ hydrogen annealing at a much lower temperature of 350°C, however, results in an overall PL intensity increase with a significant narrowing and a small blueshift of the high-energy WL emission due to hydrogen bonding which neutralizes defects and relieves associated strains.     

Influence of hole shape/size on the growth of site-selective quantum dots

The number of quantum dots which nucleate at a certain place has to be controllable for device integration. It was shown that the number of quantum dots per nucleation site depends on the size of the hole in the substrate, but other dimensions of the nucleation site are vague. We report on the influence of hole shape on site-selectively grown InAs quantum dots (QDs) by molecular beam epitaxy. Dry etching of the GaAs wafers was used because of its high anisotropic etching characteristic. Therefore, it was possible to verify the influence of several hole shape parameters on the subsequent QD growth independently. We show that the nucleation of these QDs depends on several properties of the hole, namely its surface area, aspect ratio of the surface area, and depth. Especially, the aspect ratio shows a big influence on the number of nucleating QDs per site. With knowledge of these dependencies, it is possible to influence the number of QDs per site and also its distribution.     

Linear and nonlinear optical characteristics of CsPbBr3 perovskite quantum dots-doped borosilicate glasses

CsPbBr₃ perovskite QDs are precipitated in a borosilicate glass matrix, while protects efficiently the QD from photo-induced and chemical degradation. We show that the CsPbBr₃ QD doped glasses exhibit strong visible photoluminescence (PL), which is dependence on the concentration that can be controlled by heat treatment conditions. Due to the stabilization by the glass matrix, we are able to determine the nonlinear optical (NLO) properties with a Z-scan technique. We observe a cross-over from saturated absorption (SA) to reverse saturated absorption (RSA) by either increase the pumping intensity or the QD size, reminiscent of quantum size effect in the NLO response. The RSA is associated with two-photon absorption (TPA) that induces strong upconversion luminescence of QD doped glass samples. Our results imply that the glasses containing CsPbBr₃ QDs may find potential applications from solid state lighting to ultrafast optical switches.     

Enhanced photoluminescence of multilayer Ge quantum dots on Si(001) substrates by increased overgrowth temperature

Four-bilayer Ge quantum dots (QDs) with Si spacers were grown on Si(001) substrates by ultrahigh vacuum chemical vapor deposition. In three samples, all Ge QDs were grown at 520 °C, while Si spacers were grown at various temperatures (520 °C, 550 °C, and 580 °C). Enhancement and redshift of room temperature photoluminescence (PL) were observed from the samples in which Si spacers were grown at a higher temperature. The enhancement of PL is explained by higher effective electrons capturing in the larger size Ge QDs. Quantum confinement of the Ge QDs is responsible for the redshift of PL spectra. The Ge QDs’ size and content were investigated by atomic force microscopy and Raman scattering measurements.     

Improving the emission efficiency of MBE-grown GaN/AlN QDs by strain control

ABSTRACT: The quantum-confined stark effect induced by polarization has significant effects on the optical properties of nitride heterostructures. In order to improve the emission efficiency of GaN/AlN quantum dots [QDs], a novel epitaxial structure is proposed: a partially relaxed GaN layer followed by an AlN spacer layer is inserted before the growth of GaN QDs. GaN/AlN QD samples with the proposed structure are grown by molecular beam epitaxy. The results show that by choosing a proper AlN spacer thickness to control the strain in GaN QDs, the internal quantum efficiencies have been improved from 30.7% to 66.5% and from 5.8% to 13.5% for QDs emitting violet and green lights, respectively.     

Miniband-related 1.4–1.8 μm luminescence of Ge/Si quantum dot superlattices

The luminescence properties of highly strained, Sb-doped Ge/Si multi-layer heterostructures with incorporated Ge quantum dots (QDs) are studied. Calculations of the electronic band structure and luminescence measurements prove the existence of an electron miniband within the columns of the QDs. Miniband formation results in a conversion of the indirect to a quasi-direct excitons takes place. The optical transitions between electron states within the miniband and hole states within QDs are responsible for an intense luminescence in the 1.4–1.8 μm range, which is maintained up to room temperature. At 300 K, a light emitting diode based on such Ge/Si QD superlattices demonstrates an external quantum efficiency of 0.04% at a wavelength of 1.55 μm.     

One-Pot Synthesis of Biocompatible CdSe/CdS Quantum Dots and Their Applications as Fluorescent Biological Labels

We developed a novel one-pot polyol approach for the synthesis of biocompatible CdSe quantum dots (QDs) using poly(acrylic acid) (PAA) as a capping ligand at 240°C. The morphological and structural characterization confirmed the formation of biocompatible and monodisperse CdSe QDs with several nanometers in size. The encapsulation of CdS thin layers on the surface of CdSe QDs (CdSe/CdS core–shell QDs) was used for passivating the defect emission (650 nm) and enhancing the fluorescent quantum yields up to 30% of band-to-band emission (530–600 nm). Moreover, the PL emission peak of CdSe/CdS core–shell QDs could be tuned from 530 to 600 nm by the size of CdSe core. The as-prepared CdSe/CdS core–shell QDs with small size, well water solubility, good monodispersity, and bright PL emission showed high performance as fluorescent cell labels in vitro. The viability of QDs-labeled 293T cells was evaluated using a 3-(4,5-dimethylthiazol)-2-diphenyltertrazolium bromide (MTT) assay. The results showed the satisfactory (>80%) biocompatibility of as-synthesized PAA-capped QDs at the Cd concentration of 15 μg/ml.     

Synthesis and Properties of Water-Soluble Silica-Coated ZnSe/ZnS Semiconductor Quantum Dots

Silica encapsulated ZnSe/ZnS quantum dots (QDs) are prepared via a sol–gel method by hydrolyzing tetraethyl orthosilicate (TEOS) on the surface of the QDs. The photoluminescence (PL) intensity of ZnS coated ZnSe QDs is more than three times that of ZnSe QDs. By partial interchange of the capping ligand from thioglycolic acid (TGA) to 3-mercaptopropyltri-methoxysilane (MPS) on the QDs, initial PL efficiency of the QDs in water was retained. The average size and morphology of the multicore-shell structured ZnSe/ZnS@SiO₂ can be controlled by varying MPS and TEOS concentration.     

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.     

Design of semiconductor ternary quantum dots with optimal optoelectronic function

The function of nanometer‐size quantum dots (QDs) of ternary compound semiconductors, such as In_xGa_1?xAs and ZnSe_1?xTe_x, used in the fabrication of optoelectronic and photovoltaic devices can be optimized by precise tuning of their electronic band gap through control of the QD composition (x) and diameter. Results on compositional distributions in ternary QDs and how they affect the QDs' electronic band gap are reported. A hierarchical modeling approach is followed that combines first‐principles density functional theory calculations and classical Monte Carlo simulations with a continuum model of species transport in spherical nanocrystals. In certain cases, the model predicts the formation of core/shell‐like structures with shell regions rich in the surface segregating species. A systematic parametric analysis generates a database of transport properties, which can be used to design post‐growth thermal annealing processes that enable the development of thermodynamically stable QDs with optimal electronic properties grown through simple one‐step colloidal synthesis techniques. © 2013 American Institute of Chemical Engineers AIChE J, 59: 3223–3236, 2013     

Growth of InAs Quantum Dots on Germanium Substrate Using Metal Organic Chemical Vapor Deposition Technique

Self-assembled InAs quantum dots (QDs) were grown on germanium substrates by metal organic chemical vapor deposition technique. Effects of growth temperature and InAs coverage on the size, density, and height of quantum dots were investigated. Growth temperature was varied from 400 to 450 °C and InAs coverage was varied between 1.40 and 2.35 monolayers (MLs). The surface morphology and structural characteristics of the quantum dots analyzed by atomic force microscope revealed that the density of the InAs quantum dots first increased and then decreased with the amount of InAs coverage; whereas density decreased with increase in growth temperature. It was observed that the size and height of InAs quantum dots increased with increase in both temperature and InAs coverage. The density of QDs was effectively controlled by growth temperature and InAs coverage on GaAs buffer layer.