Size Distribution Of Quantum Dots Research Articles

Determination of the particle size distribution of cube-shaped colloidal perovskite quantum dots from photoluminescence spectra: A combined theoretical-experimental approach.

A theoretical-experimental approach is proposed to convert the photoluminescence spectra of colloidal perovskite quantum dot ensembles into accurate estimates for their intrinsic particle size distribution functions. Two main problems were addressed and properly correlated: the size dependence of the first excitonic transition in a single cube-shaped quantum dot and the inhomogeneous broadening of the fluorescence line shape due to the size nonuniformity of the chemically prepared quantum dot suspension in addition to the single-dot homogeneous broadening. By applying the reported methodology to CsPbBr3 quantum dot samples belonging to the strong and intermediate confinement regimes, the calculated size distributions exhibited close agreement with those obtained from transmission electron microscopy, with precise estimates for the average particle size and standard deviation. Specifically for strongly confined ultrasmall CsPbBr3 quantum dots, the presented spectroscopic model for size distribution computation is based on a new analytical expression for the size-dependent bandgap, which was developed within the framework of the finite-depth square-well effective mass approximation accounting for band nonparabolicity effects. Such a quantum mechanical approach correctly predicts the expected transition to the intermediate confinement regime in sufficiently large quantum dots, which are traditionally described by the well-known bandgap equation in the infinite potential barrier limit with a spatially correlated electron-hole wavefunction and nonparabolic carrier effective masses. The proposed calculation scheme originates from general theoretical considerations so that it can be readily adapted to semiconductor quantum dots of many other systems, from all inorganic metal halides to hybrid perovskite materials, regardless of the adopted chemical synthesis route.

Synthesis of uniform sized ZnS quantum dots using hydrodynamic cavitation and their characterization

As representative non-toxic cadmium-free quantum dots (QDs), ZnS QDs with high quantum efficiency, super stability and excellent biocompatibility had attracted wide attention in the fields of photocatalysis, solar cells and biomedicine. In this study, hydrodynamic cavitation (HC) technology was applied to the preparation of ZnS QDs. By adjusting HC device parameters, water soluble ZnS QDs with small particle size, narrow particle size distribution range, high absorbance, high luminous efficiency and high quantum yield were prepared. The morphology, size distribution, element composition and optical properties of ZnS QDs were studied by various characterization methods. ZnS QDs with average particle size of 1.48 nm, fluorescence quantum yield of 34.07% and Stokes shift of 112 nm were obtained. In addition, the mechanism of preparation of ZnS QDs by using HC method was also studied. It is hoped that this HC technology can provide a new idea for large-scale preparation of ZnS QDs with excellent properties.

Direct Visualization of Confinement and Many‐Body Correlation Effects in 2D Spectroscopy of Quantum Dots

AbstractThe size tunable color of colloidal semiconductor quantum dots (QDs) is probably the most elegant illustration of the quantum confinement effect. As explained by the simple “particle‐in‐a‐box” model, the transition energies between the levels increase when the “box” becomes smaller. To investigate quantum confinement effects, typically a well‐defined narrow size distribution of the nanoparticles is needed. In this contribution, how coherent electronic two‐dimensional spectroscopy (2DES) can directly visualize the quantum size effect in a sample with broad size distribution of QDs is demonstrated. The method is based on two features of the 2DES – the ability to resolve inhomogeneous broadening and the capability to reveal correlations between the states. In QD samples, inhomogeneous spectral broadening is mainly caused by the size distribution and leads to elongated diagonal peaks of the spectra. Since the cross peaks correlate the energies of two states, they allow drawing conclusions about the size dependence of the corresponding states. It is also found that the biexciton binding energy changes between 3 and 8 meV with the QD size. Remarkably, the size dependence is non‐monotonic with a clear minimum.

Role of annealing on the structural, optoelectronic and antibacterial properties of Sm-doped TiO2 quantum dots

In this study, the sol-gel method was adopted to create the Sm-doped TiO2 quantum dots (QDs), which were then annealed at different temperatures of 300, 400, and 500 °C. The XRD data show that all samples' crystal structures correspond to the tetragonal anatase phase, with the annealed sample at 500 °C exhibiting improved crystallinity. According to the TEM investigations, the particles are almost homogeneous, ultra-fine, and exhibit the quantum size effect. The presence of elements such as Ti, Sm, and O in the sample was confirmed by EDS, while the average particle size distribution of the Sm-doped TiO2 QDs, which were annealed at 500 °C, was 1.82 ± 0.06 nm, as confirmed by TEM. UV–visible spectra reveal that the bandgap increases from 3.12 to 3.27 eV because of the increasing temperature. Studies carried out on photoluminescence demonstrate that as the annealing temperature is raised, the PL emission intensity also increases over the entire UV–visible region. These findings suggest that TiO2 QDs characteristics can be modified for optoelectronic applications by adjusting the annealing temperature. In addition to these intriguing results, Sm-doped TiO2 QDs that underwent 500 °C annealing demonstrate a larger zone of inhibition (11 mm for 300 μg/mL) against E. coli in comparison to other annealed samples, while S. aureus does not exhibit a discernible enhancement.

Graphene nanosheet-supported ultrafine RuO2 quantum dots as electrochemical energy materials

Ruthenium oxide (RuO2) shows great promise as an electrode material for supercapacitors, which are energy storage devices that have large power densities. However, RuO2 materials suffer low surface area, poor electrical conductivity and a tendency to aggregate after reactions, limiting their rate capability and cycle stability and can lead to inadequate redox reactions with electrolytes. To address these problems, this work synthesized homogeneous ultrafine-RuO2 quantum dots (QDs) materials with a size of around 2 nm on the surface of graphene nanosheets (GNS) via a facile hydrothermal method. The small size and uniform distribution of RuO2 QDs in the composite electrode material allowed for a high concentration of active adsorption sites for ions in the electrolyte while also facilitating efficient electrochemical redox reactions. The resulting RuO2/GNS composite exhibited a large specific area of 177.34 m2g‐1 and demonstrated an excellent capacitance performance of 1138.5 Fg‐1 at a current density of 0.5 Ag‐1. Additionally, a retention rate of 91.4 % when applying current densities from 0.5 to 10 Ag‐1 and cycling stability with 94.5 % retention after 20000 cycles, demonstrates the occurrence of a rapid and reversible faradaic redox reaction on the electrode surface. The symmetrical supercapacitor configuration with two identical RuO2/GNS electrodes was fabricated and demonstrated a high capacity (309.16 Fg‐1 at a current density of 0.5 Ag‐1) and an outstanding retention rate of 91.2 % at a current density of 10 A g−1). A device operated within a 1.8 V potential window showed high energy density from 126 Whkg‐1 to 139.2 Whkg‐1 and a power density from 440.1 Wkg‐1 to 8494.4 Wkg‐1 at current densities ranging from 0.5 Ag‐1 to 10 Ag‐1, respectively. This ultrafine-RuO2 quantum dots composite is a potentially promising advanced functional electrode material for electrochemical applications beyond supercapacitors and may be suitable for a broader range of energy storage and conversion applications.

Modelling and experimental characterization of double layer InP/AlGaInP quantum dot laser

Spectrum of an InP/AlGaInP self- assembled double-layer quantum dot (QD) laser fabricated by metal–organic vapor-phase epitaxy is theoretically and experimentally investigated. A bimodal QD size distribution (small and large QD groups) was detected which is formed during the fabrication. A model is proposed based on rate equations accounting for the superposition of two inhomogeneous QD groups. The total output power and the power spectral density (PSD) of the fabricated QD laser are experimentally characterized at room temperature. The output spectrum is segmented into the sum of two Gaussians curves (super Gaussian) belonging to the small and large QD groups. The peak PSD and the spectral width of each group are extracted and their dependency on the injected current density is analysed. The peak of the large QDs is found to be dominant at small current while the peak of the small QDs dominated at high current alongside a reduction in its spectral width leading to lasing based on them. This behaviour is attributed to the saturation of the large QDs energy levels due to its relatively long radiative lifetime. The experimental analysis is in a good agreement with the theoretical results.

Controlled mixing during colloidal quantum dot synthesis: A proxy-concept based on equivalent parameters

Mixing is a key process parameter during liquid phase particle synthesis that requires special attention, in particular for scalable process and reactor development. This issue is especially pressing for advanced materials where on the one hand multifunctional properties require products of utmost quality, while on the other hand only few strategies for process design are yet developed. One material class in this context is quantum dot (QD) nanocrystals. By making use of automation and high throughout (HT) experimentation, we could recently demonstrate qualitatively the role of mixing on focusing and defocusing during QD synthesis by hot injection. In this work, we demonstrate the application of HT methodologies to investigate the effect of mixing as an important process parameter during process optimization and scale up. We performed reaction optimization by screening a multi-parameter design space using design of experiments (DoE) and machine learning (ML). We developed a so-called cold model as proxy that is based on equivalent mixing times (EMTs) derived from a competing parallel reaction system. Experimentally, we realized a fully automated approach using a HT platform for particle synthesis. The final dataset (128 experiments for model development including repeats and 29 experiments for prediction testing) was combined with DoE and complimented with machine learning. By doing so, with DoE, we could reduce the number of experiments required to develop a predictive, statistical knowledge base for EMTs at ambient conditions. Finally, we demonstrated the applicability of EMTs for two defined stirrer geometries to fine tune the widths of the particle size distribution and photoluminescence of QDs at increasing reaction volumes from 20 mL to 80 mL. This opens the door towards scalable processes for QDs at increased reaction volumes while maintaining product quality.

Electroluminescence from GaN‐Based Quantum Dots

AbstractBulk gallium nitride (GaN) has shown great success in light‐emitting diodes (LEDs), but the use of its counterpart GaN quantum dots (QDs) to obtain electroluminescence has not yet been reported. In this work, the first GaN‐based QLED is demonstrated using Zn‐doped GaN (GaN: Zn) QDs, which is achieved through the combination of trap passivation, energy level adjustment, and morphology engineering. Pure GaN QDs and GaN: Zn QDs are synthesized, and it is found that Zn doping shifts the GaN QD emission from 321 to 377 nm and tunes the highest occupied molecular orbital energy level from 8.6 eV (of original GaN QDs) to 6.9 eV. Multiple washing posttreatment is further developed to improve QD film morphology and size distribution. The optimized GaN: Zn QDs are employed to fabricate solution‐processed LEDs, and the first GaN‐based QLEDs are reported with a maximum quantum efficiency of 0.004%.

Multi-step photon upconversion in quantum-dot-based solar cells with a double-heterointerface structure

Photon upconversion (PU) is a process where an electron is excited from the valence band to the conduction band of a wide-gap semiconductor by the sequential absorption of two or more photons via real states. For example, two-step PU can generate additional photocurrent in the so-called intermediate-band solar cells. In this work, we consider two- and three-step processes; we study multi-step PU in a quantum dot (QD)-based single-junction solar cell with a double-heterointerface structure. The solar cell consists of three different absorber layers: Al0.7Ga0.3As, Al0.3Ga0.7As, and GaAs, which form two heterointerfaces. Just beneath each heterointerface, an InAs/GaAs QD layer was inserted. After band-to-band excitation, electrons accumulate at each heterointerface, and then, below-bandgap photons excite a certain fraction of these electrons above the barrier energy. The photoluminescence spectra of the InAs QDs reveal slightly different QD size distributions at the two heterointerfaces. We show that the external quantum efficiency is improved by additional irradiation with below-bandgap infrared photons, which suggests a multi-step PU process that involves the two heterointerfaces. The dependence of the photocurrent on the infrared excitation power density only shows a superlinear behavior when the GaAs layer is excited but the Al0.3Ga0.7As layer is not. These data demonstrate a multi-step PU process that consists of one intraband transition at each of the two heterointerfaces and one interband transition in GaAs.

Hybrid Nanomat: Copolymer Template CdSe Quantum Dots In Situ Stabilized and Immobilized within Nanofiber Matrix

Fabrication and characterization of hybrid nanomats containing quantum dots can play a prominent role in the development of advanced biosensors and bio-based semiconductors. Owing to their size-dependent properties and controlled nanostructures, quantum dots (QDs) exhibit distinct optical and electronic characteristics. However, QDs include heavy metals and often require stabilizing agents which are toxic for biological applications. Here, to mitigate the use of toxic ligands, cadmium selenide quantum dots (CdSe QDs) were synthesized in situ with polyvinylpyrrolidone (PVP) at room temperature. The addition of PVP polymer provided size regulation, stability, and control over size distribution of CdSe QDs. The characterization of the optical properties of the CdSe QDs was performed using fluorescence and ultraviolet-visible (UV-Vis) spectroscopy. CdSe QDs exhibited a typical absorbance peak at 280 nm and a photoluminescence emission peak at 580 nm. Transmission electron microscopy (TEM) micrographs demonstrated that CdSe QDs having an average size of 6 ± 4 nm were obtained via wet chemistry method. CdSe QDs were immobilized in a blend of PVP and poly(L-lactide-co-ε-caprolactone) (PL-b-CL) copolymer that was electrospun to produce nanofibers. Scanning electron microscopy (SEM), thermal analyses and attenuated total reflectance Fourier-transform infrared spectroscopy (ATR-FTIR) were used to characterize properties of fabricated nanofibers. Both pristine and hybrid nanofibers possessed cylindrical geometry and rough surface features, facilitating increased surface area. Infrared absorption spectra showed a slight shift in absorbance peaks due to interaction of PVP-coated CdSe QDs and nanofiber matrix. The presence of CdSe QDs influenced the fiber diameter and their thermal stability. Further, in vitro biological analyses of hybrid nanofibers showed promising antibacterial effect and decline in cancer cell viability. This study offers a simple approach to obtain hybrid nanomats immobilized with size-controlled PVP-coated CdSe QDs, which have potential applications as biosensors and antibacterial and anticancer cell agents.

Photoluminescence Properties of InAs Quantum Dots Overgrown by a Low-Temperature GaAs Layer under Different Arsenic Pressures

We studied the influence of the arsenic pressure during low-temperature GaAs overgrowth of InAs quantum dots on their optical properties. In the photoluminescence spectrum of quantum dots overgrown at a high arsenic pressure, we observed a single broad line corresponding to unimodal size distribution of quantum dots. Meanwhile, two distinct peaks (~1080 and ~1150 nm) at larger wavelengths are found in the spectra of samples with quantum dots overgrown at a low arsenic pressure. We attributed this phenomenon to the high-pressure suppression of atom diffusion between InAs islands at the overgrowth stage, which makes it possible to preserve the initial unimodal size distribution of quantum dots. The same overgrowth of quantum dots at the low arsenic pressure induces intensive mass transfer, which leads to the formation of arrays of quantum dots with larger sizes. Integrated photoluminescence intensity at 300 K is found to be lower for quantum dots overgrown at the higher arsenic pressure. However, a difference in the photoluminescence intensity for the high- and low-pressure overgrowths is not so significant for a temperature of 77 K. This indicates that excess arsenic incorporates into the capping layer at high arsenic pressures and creates numerous nonradiative recombination centers, diminishing the photoluminescence intensity.

Roles of TOPO Coordinating Solvent on Prepared Nano-Flower/Star and Nano-Rods Nickel Sulphides for Solar Cells Applications.

The present study describes a cheap, safe, and stable chemical process for the formation of nickel sulphide (NiS) with the use of mixed and single molecular precursors. The production pathway is uncomplicated, energy-efficient, quick, and toxic-free, with large-scale commercialization potential. The obtained results show the effect of tri-N-octylphosphine oxide (TOPO) as a coordinating solvent on the reaction chemistry, size distributions, morphology, and optical properties of both precursors. Ni[N,N-benz-N-p-anisldtc] as NiSa, Ni[N,N-benzldtc] as NiSb, and Ni[N-p-anisldtc] as NiSc thermally decompose in a single step at 333–334 °C. The X-ray diffraction peaks for NiSa, NiSb, and NiSc matched well with the cubic NiS nanoparticles and corresponded to planes of (111), (220), and (311). The extrapolated linear part from the Tauc plots reveals band gap values of 3.12 eV, 2.95 eV, and 2.5 eV, which confirms the three samples as potential materials for solar cell applications. The transmission electron microscopy (TEM) technique affirmed the quantum dot size distribution at 19.69–28.19 nm for NISa, 9.08–16.63 nm for NISb, and 9.37–10.49 nm for NISc, respectively. NiSa and NiSc show a clearly distinguishable flower/star like morphology, while NiSb displays a compact nano-rod shape. To the best of the authors’ knowledge, very few studies have been reported on the flower/star like and nano-rod shapes, but none with the dithiocarbamate molecular precursor for NiS nanoparticles.

Colloidal stability and aggregation kinetics of nanocrystal CdSe/ZnS quantum dots in aqueous systems: Effects of ionic strength, electrolyte type, and natural organic matter

Understanding the stability and aggregation of nanoparticles in aqueous milieu is critical for assessing their behavior in the natural and engineered environmental systems and establishing their threat to human and ecosystems health. In this study, the colloidal stability and aggregation kinetics of nanocrystal quantum dots (QDs) —CdSe/ZnS QDs—were thoroughly explored under a wide range of aqueous environmental conditions. The z-average hydrodynamic diameters (z-avg. HDs) and zeta potential (ξ potential) of CdSe/ZnS QDs were measured in monovalent electrolyte (NaCl) and divalent electrolyte (CaCl2) solutions in both the absence and presence of natural organic matter (NOM)—Suwannee River natural organic matter, SRNOM to assess the dynamic growth of these nanoaggregate-QD-complexes, and the evaluation of their colloidal stability. Results show that CaCl2 was more effective to destabilize the QDs compared to NaCl at similar concentrations. An increase in NaCl concentration from 0.01 to 3.5 M increased the z-avg. HD of QD aggregates from 61.4 nm to 107.2 nm. The aggregation rates of QDs increased from 0.007 to 0.042 nm·s−1 with an increase in ionic strength from 0.5 to 3.5 M NaCl solutions, respectively. In the presence of Na+ cations, the aggregation of QDs was limited as steric forces generated by the original surface coating of QDs prevailed. In the presence of CaCl2, the aggregation of QDs was observed at a low concentration of CaCl2 (0.0001 M) with a z-avg. HD of 74.2 nm that significantly increased when the CaCl2 was higher than 0.002 M. Larger sizes of QD aggregates were observed at each level of CaCl2 concentration in suspensions of 0.002–0.1 M, as the z-avg. HDs of QDs increased from 125.1 to 560.4 nm, respectively. In the case of CaCl2, an increase in aggregation rates occurred from 0.035 to 0.865 nm·s−1 with an increase in ionic strength from 0.0001 M to 0.004 M, respectively. With Ca2+ cations, the aggregation of QDs was enhanced due to the bridging effects from the formation of complexes between Ca2+ cations in solution and the carboxyl group located on the surface coating of QDs. In the presence of SRNOM, the aggregation of QDs was enhanced in both monovalent and divalent electrolyte solutions. The degree of aggregation formation between QDs through cation-NOM bridges was superior for Ca2+ cations compared to Na+ cations. The presence of SRNOM resulted in a small increase in the size of the QD aggregates for each of NaCl concentrations tested (i.e., 0.01 to 3.5 M, except 0.1 M), and induced a monodispersed and narrower size distribution of QDs suspended in the monovalent electrolyte NaCl concentrations. In the presence of SRNOM, the aggregation rates of QDs increased from 0.01 to 0.024 nm 1 with the increase of NaCl concentrations from 0.01 to 2 M, respectively. The presence of SRNOM in QDs suspended in divalent electrolyte CaCl2 solutions enhanced the aggregation of QDs, resulting in the increase of z-avg. HDs of QDs by approximately 19.3%, 42.1%, 13.8%, 1.5%, and 24.8%, at CaCl2 concentrations of 0.002, 0.003, 0.005, 0.01, and 0.1 M, respectively. In the case of CaCl2, an increase in aggregation rates occurred from 0.035 to 0.865 nm·s−1 with an increase in ionic strength from 0.0001 to 0.004 M, respectively. Our findings demonstrated the colloidal stability of QDs and cations-NOM-QD nanoparticle complexes under a broad spectrum of conditions encountered in the natural and engineered environment, indicating and the potential risks from these nanoparticles in terms of human and ecosystem health.

Narrowing of the Particle Size Distribution of InP Quantum Dots for Green Light Emission by Synthesis in Micro‐Flow Reactor

AbstractQuantum dots (QDs), with their superior efficiency, color purity, and color controllability, are expected to be applied in next generation displays and other devices. The development of methods to synthesize QDs still provide equivalent or better performance without restricted substances such as cadmium (Cd) and lead (Pb) is a meaningful challenge. In this study, InP QDs were synthesized using the micro‐flow reactor (MFR) with an extremely high rate of temperature change to shorten the nucleation time and avoid Ostwald ripening during QD synthesis. As a result, the particle size distribution was narrowed and the emission full‐width at half maximum (FWHM) was reduced to less than 40 nm. While other related studies have tried complex methods, in our efforts, it was achieved by using the simple MFR. These results can accelerate the application of InP QDs as a promising option for commercially viable QDs.

Manipulating time-dependent size distribution of sulfur quantum dots and their fluorescence sensing for ascorbic acid.

Unlike the previous commonly used strong alkaline solvent sodium hydroxide, we employ an eco-friendly solvent, ethanol, as a solvent for the preparation of ultra-small-sized sulfur quantum dots (SQDs). Ethanol can disperse bulk sulfur and allow sufficient transfer of large-sized sulfur to smaller-sized SQDs through a one-pot synthesis approach. The SQDs obtained from ethanol as the solvent displays superior photoluminescence properties to those in water and sodium hydroxide. By delicately controlling the reaction conditions, including the amount of bulk sulfur, the reaction time, and the proportion of sulfur to oxidizing reagent, highly blue emissive SQDs with a photoluminescence quantum yield (PLQY) of 7.04% with ultra-high stability for several months can be successfully prepared. Furthermore, we found out that the SQDs display a dynamic photoluminescence properties and varied particle sizes as the reaction time increases, which is possibly realized via the etching-aggregation process. Morevoer, the fluorescence of SQDs-72 can be effectively quenched by CoOOH nanosheets and recovered upon addition of ascorbic acid (AA) by consuming CoOOH nanosheets through the redox reaction, leading to fluorescence recovery. Therefore, a fluorescence "off-on" nanosensor for the detection of AA with a limit of detection (LOD) of 0.85 μM was constructed.

Polyimide composite films reinforced by graphene quantum dots

Polyimide composite films have been widely used in some advanced field of microelectronic devices, precision instruments and national defense applications. Graphene quantum dots have great application potential in polymer doping modification because of their good mechanical strength, high specific surface area and excellent tunability of physical and chemical properties. In this paper, Graphene quantum dots are prepared by pyrolysis at different temperatures. The results show that different reaction temperatures have a great influence on the size and size distribution of graphene quantum dots. When the pyrolysis temperature is 200 °C, the size of graphene quantum dots is uniform at 3–5 nm. Graphene quantum dots-polyimide nanocomposite films prepared by in-situ polymerization show excellent mechanical properties. When the doping amount of graphene quantum dots is 0.5 wt%, the tensile strength and elastic modulus of the composite films can reach 130.24 MPa and 2.93 GPa respectively, which are 41.3% and 108% higher than that of pure polyimide films, respectively. Moreover, the thermal stability of polyimide composite films increases with the increase of the doping amount of graphene quantum dots. This shows that graphene quantum dots have good dispersion in polyimide matrix and can effectively improve the interface of composites. These results provide a successful preparation method to help guide to fabricate graphene quantum dots-polyimide composite films with high performance for the advanced applications.

Activation energy distribution in thermal quenching of exciton and defect-related photoluminescence of InP/ZnS quantum dots

Thermal quenching is one of the essential factors in reducing the efficiency of radiative processes in luminophores of various nature. The emission activity of low-dimensional structures is influenced also by multiplicity of parameters that are related to synthesis processes, treatment regimes, etc. In the present work, we have investigated the temperature dependence of photoluminescence caused by exciton and defect-related transitions in ensembles of biocompatible InP/ZnS core/shell nanocrystals with an average size of 2.1 and 2.3 nm. The spread in the positions of energy levels is shown to be due to size distribution of quantum dots in the ensembles under study. For a quantitative analysis of the experimental data, we have proposed a band model accounting for the Gaussian distribution of the thermally activated barriers in the photoluminescence quenching processes. The model offers the thermal escape of an electrons from the core into the shell as the main mechanism for non-radiative decay of excitons. In turn, the quenching of defect-related emission is predominantly brought about through the emptying of the hole capture centers based on dangling phosphorus bonds. We have revealed the correlation between size distributions of quantum dots and scatter of the activation energy of exciton luminescence quenching. The developed approach will give further the possibility to optimize technological regimes and methods for band engineering of indium phosphide-based type-I quantum dots.

Evaluation of In(Ga)As capping in a multilayer coupled InAs quantum dot system: Growth strategy involving the same overgrowth percentage

Strain-coupled multilayer Quantum Dot (QD) structures draw a great attention these days because of their superior optical and device performance. However, these coupled multilayer QD structures have limitations such as non-uniform QD size distribution, defects, and dislocations due to the propagation of strain in QD layers. Furthermore, the carrier relaxation lifetime must be improved in these coupled QD structures for sought-after device performance. This study serves for three main purposes. Firstly, we have utilized a growth strategy to maintain the overgrowth percentage such that the Stranski-Krastanov (SK) QD dimensions in every layer is same for all the multilayer structures. Secondly, these multilayer SK QDs are made to electronically couple with the Sub-monolayer (SML) QDs in such a way that the carrier relaxation lifetime can be increased, that could ameliorate the photoconductive gain and the responsivity. Lastly, the amount of cumulative strain generated inside QDs can be reduced by the incorporation of In0.15Ga0.85As strain reducing layer (capping layer) in a multilayer structure. Five different multilayer structures with single (x1), bi (x2), penta (x5), hepta (x7), and ten-layers (x10) of SK QDs electronically coupled to six stacks of SML QDs are used in this study. Photoluminescence (PL) studies reveal that the SK QD dimensions is maintained to be the same in all multilayer structures due to the proposed growth strategy, which is also observed through transmission electron microscopy (TEM) images. Photoluminescence excitation (PLE) analysis shows the match of excited states of SK QDs to the ground state of the SML QDs, aiding the carrier tunnel phenomena. The ω/2Ө measurements from high resolution X-ray diffraction (HRXRD) is carried out to calculate the overall strain in the grown heterostructures. The optical properties and the strain components obtained from the nextnano simulation tool are in good agreement with the experimental results. Thus, coupled multilayer QD structures with a growth strategy in the current study would be more suitable for the realization of quantum dot infrared photodetectors and intermediate band solar cell applications accommodated with high device efficiency.

Exploring the physics of cesium lead halide perovskite quantum dots via Bayesian inference of the photoluminescence spectra in automated experiment

Abstract The unique optoelectronic properties of metal halide perovskite quantum dots (QDs) make them promising candidates for applications in light-emitting diodes (LEDs), scintillators, and other photonic devices. The automated micropipetting synthesis platform equipped with an optical reader enables the opportunity for high throughput synthesis and photoluminescent (PL) characterization of metal halide perovskite QDs for the first time. Here, we explore the compositional dependence of the PL behavior and stability of the combinatorial library of cesium lead halide (CsPbX3) perovskites QDs via the automated platform. To study the stability of synthesized QDs in the binary and ternary configurations, we study the time-dependent PL properties using previously developed machine learning analysis. To systematically explore the PL behavior in the ternary CsPbX3 QDs system, we introduce the Bayesian inference framework that allows the probabilistic fit of multiple models to the PL data and establishes both optimal model and model parameter robustly. Furthermore, these behaviors can be used as a control parameter for the navigation of the multidimensional compositional spaces in automated synthesis. This analysis shows the nonuniformity of the PL peak behavior in the ternary CsPbX3 QDs system. Further, the analysis confirms narrow size distribution and good quality of CsPbBr3 QDs alloyed with low concentrations of iodide and chloride. We note that Bayesian Inference fit parameters can be further used as a control signal for navigation of the chemical spaces in automated synthesis.

Selectively depositing Bi2O3 quantum dots on TiO2 nanotubes for efficient visible-light-driven photocatalysis

By utilizing the strong interaction between Bi3+ and TiO2, we successfully decorate TiO2 nanotubes with Bi2O3 quantum dots (QDs) by three different strategies. The similar size distribution but distinct photosensitization performance of these Bi2O3 QDs lead us to investigate decisive factors other than particle size. It is suggested that the photochemical method can selectively deposit Bi2O3 QDs on electron-rich sites of TiO2, which provides a facile channel for the electron-hole separation and transfer. As a result, abundant h+ and ·OH are generated to effectively degrade RhB.