Morphology Of Quantum Dots Research Articles

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.

Unveiling the 3D Morphology of Epitaxial GaAs/AlGaAs Quantum Dots.

Strain-free GaAs/AlGaAs semiconductor quantum dots (QDs) grown by droplet etching and nanohole infilling (DENI) are highly promising candidates for the on-demand generation of indistinguishable and entangled photon sources. The spectroscopic fingerprint and quantum optical properties of QDs are significantly influenced by their morphology. The effects of nanohole geometry and infilled material on the exciton binding energies and fine structure splitting are well-understood. However, a comprehensive understanding of GaAs/AlGaAs QD morphology remains elusive. To address this, we employ high-resolution scanning transmission electron microscopy (STEM) and reverse engineering through selective chemical etching and atomic force microscopy (AFM). Cross-sectional STEM of uncapped QDs reveals an inverted conical nanohole with Al-rich sidewalls and defect-free interfaces. Subsequent selective chemical etching and AFM measurements further reveal asymmetries in element distribution. This study enhances the understanding of DENI QD morphology and provides a fundamental three-dimensional structural model for simulating and optimizing their optoelectronic properties.

Zincblende InAsxP1-x/InP Quantum Dot Nanowires for Telecom Wavelength Emission.

InAsxP1-x quantum dots (QDs) in InP nanowires (NWs) have been realized as a platform for emission at telecom wavelengths. These QDs are typically grown in NWs with the wurtzite crystal phase, but in this case, ultrathin diameters are required to achieve defect-free heterostructures, making the structures less robust. In this work, we demonstrate the growth of pure zincblende InAsxP1-x QDs in InP NWs, which enabled an increase in NW diameters to about 45 nm, achieved by employing Au-assisted vapor liquid solid growth in a chemical beam epitaxy system. We studied the growth of InP/InAsxP1-x heterostructures with different compositions to control the straight growth along the ⟨100⟩ direction and to tune the emission wavelength. Interestingly, we found that the growth mechanism for pure InAs QDs is different compared to that for InAsxP1-x alloy QDs. This allowed us to optimize different growth protocols to achieve straight growth of the final QD NWs. We successfully obtained the growth of InAsxP1-x QDs with a composition in the range of x = 0.24-1.00. By means of microphotoluminescence measurements, we demonstrate the tunability of the emission in dependence of the InAsxP1-x QD composition and morphology, remarkably observing an emission at the telecom O-band for a 10 nm thick QD with 80% of As content.

Detection of ferric ions by nitrogen and sulfur co-doped potato-derived carbon quantum dots as a fluorescent probe

This paper reports the detection of ferric ions (Fe3+) based on nitrogen and sulfur co-doped carbon quantum dots. These nitrogen and sulfur co-doped carbon quantum dots were synthesized via a hydrothermal route using northern Shaanxi potatoes as carbon sources and ammonium sulfate as nitrogen and sulfur sources. The quantum yields of the carbon quantum dots were found to be 16.96% and 4.23% with and without doping, respectively. The structural details, morphology, and optical properties of carbon quantum dots were analyzed using Fourier transform infrared spectroscopy (FT-IR), x-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), ultraviolet-visible absorption spectroscopy (UV–vis), and fluorescence spectroscopy. The as-prepared co-doped carbon quantum dots were utilized as a fluorescent probe for detecting Fe3+ ions, where the fluorescence intensity of carbon quantum dots was remarkably quenched in the presence of Fe3+ ions. A good linear relationship for Fe3+ ion detection was obtained from 0 to 500 μmol/L with a detection limit as low as 0.26 μmol/L. Furthermore, the proposed method also provided satisfactory results in the tap water.

Unique properties of titanium dioxide quantum dots assisted regulation of growth and biochemical parameters of Hibiscus sabdariffa plants

Owing to the uniqueness of quantum dots (QDs) as a potential nanomaterial for agricultural application, hence in the present study, titanium dioxide quantum dots (TiO2 QDs) were successfully synthesized via sol-gel technique and the physico-chemical properties of the prepared TiO2 QDs were analyzed. Based on the results, the TiO2 QDs showed the presence of anatase phase of TiO2. TEM examination revealed spherical QDs morphology with an average size of 7.69 ± 1.22 nm. The large zeta potential value (-20.9 ± 2.3 mV) indicate greater stability of the prepared TiO2 QDs in aqueous solutions. Moreover, in this work, the application of TiO2 QDs on Hibiscus sabdariffa plants was conducted, where H. sabdariffa plants were foliar sprayed twice a week in the early morning with different concentrations of TiO2 QDs (0, 2, 5, 10, 15 and 30 ppm) to evaluate their influence on these plants in terms of morphological indexes and biochemical parameters. The results exhibited an increasing impact of the different used concentrations of TiO2 QDs on morphological indexes, such as fresh weight, dry weight, shoot length, root length, and leaf number, and physio-biochemical parameters like chlorophyll a, chlorophyll b, carotenoid contents, total pigments and total phenolic contents. Remarkably, the most prominent result was recorded at 15 ppm TiO2 QDs where plant height, total protein and enzymatic antioxidants like catalase and peroxidase were noted to increase by 47.6, 20.5, 29.5 and 38.3%, respectively compared to control. Therefore, foliar spraying with TiO2 QDs positively serves as an effective strategy for inducing optimistic effects in H. sabdariffa plants.

Proton-Prompted Ligand Exchange to Achieve High-Efficiency CsPbI3 Quantum Dot Light-Emitting Diodes

HighlightsA new proton-promoted in situ ligand exchange strategy based on CsPbI3 quantum dots.The ligand exchange strategy maintains the quantum confinement effect of quantum dots and significantly improves the stability and photophysical properties of CsPbI3 quantum dots.The performance of light-emitting diodes based on CsPbI3 quantum dots is significantly improved, the external quantum efficiency is increased from 18.63% to 24.45%, and the half-operational lifetime is increased by 70 times.

ZnSeTe quantum dots modified with zinc chloride toward bright trap-state emission.

ZnSeTe quantum dots (QDs) attract growing interest owing to their low threats to health and the environment. They are widely applied as emitters in displays and lighting devices. Previous findings have indicated that inorganic halides are excellent candidates for surface ligands on QDs. By incorporating inorganic halides during the synthesis process, the photoluminescence (PL) intensity and quantum yield (QY) of QDs can be significantly enhanced. However, the alteration of surface states in QDs induced by zinc halide modification and the mechanism of formation of trap-state radiative recombination processes have been less discussed. Herein, we proposed a synthesis strategy for ZnSeTe/ZnSe/ZnSeS/ZnS core/shell/shell/shell QDs modified with ZnCl2, and by comparing the morphology and elemental composition of QDs with different amounts of ZnCl2 added, we revealed the regulatory mechanism of nanocrystal growth in the presence of ZnCl2. QDs with modification of ZnCl2 exhibited broad yellow fluorescence, distinct from the intrinsic blue emission. Through spectroscopic and surface ligand analyses, we attributed this yellow emission to the intermediate state energy levels caused by the defects on the surface. Finally, we used the QDs with broad linewidth emission to fabricate a simple white-light-emitting diode (WLED). This work provided new insights into the role of inorganic ligands and the use of a single emitting material in solid-state lighting devices.

Growth of Medium-Sized InP Quantum Dots with High Photoluminescence Efficiency and Enhanced Stability

This study introduces medium-sized core/shell InP quantum dots (QDs) with high photoluminescence (PL) efficiency and remarkable material stability. The incorporation of a ZnSe interlayer between the core and the thicker outer ZnS shell enhances both the optical performance and material stability. When further increasing the S/Se ratio to synthesize larger QDs with a thicker ZnS layer, optical performance significantly declines despite the improvement in stability. To achieve QDs with superior optical performance and stability, we controlled the S/Se ratio variation during shell growth and examined its impact on the structure, morphology, and size of InP QDs. Our approach resulted in medium-sized InP/ZnSe/ZnS QDs with tunable wavelengths (606-630 nm), PL quantum yields (PLQY) > 90%, full width at half maximum (FWHM) values < 40 nm, and enhanced material stability.Keywords: indium phosphide (InP), quantum dots (QDs), high efficiency and stability, S/Se ratio of shell, medium-size quantum dots, stainless steel reactor Figure 1

Acid selenites as new selenium precursor for CdSe quantum dot synthesis

Chemical precursors for nanomaterials synthesis have become essential to tune particle size, composition, morphology, and unique properties. New inexpensive precursors investigation that precisely controls these characteristics is highly relevant. We studied new Se precursors, the acid selenites (R–O–SeOOH), to synthesize CdSe quantum dots (QDs). They were produced at room temperature by the ▪ reaction with alcohols having different alkyl chains and were characterized by 1H NMR confirming their structures. This unprecedented precursor generates high-quality CdSe nanocrystals with narrow size distribution in the zinc-blend structure showing controlled optical properties. Advanced characterization detailed the CdSe structure showing stacking fault defects and its dependence on the used R–O–SeOOH. The QDs formation was examined using a time-dependent growth kinetics model. Differences in the nanoparticle surface structure influenced the optical properties, and they were correlated to the Se-precursor nature. Small alkyl chain acid selenites generally lead to more controlled QDs morphology, while the bigger alkyl chain leads to slightly upper quantum yields. Acid selenites can potentially replace Se-precursors at competitive costs in the metallic chalcogenide nanoparticles. ▪ is chemically stable, and alcohols are cheap and less toxic than the reactants used today, making acid selenites a more sustainable Se precursor.

Transmission Electron Microscopy Peeled Surface Defect of Perovskite Quantum Dots to Improve Crystal Structure.

Transmission electron microscopy (TEM) is an excellent characterization method to analyze the size, morphology, crystalline state, and microstructure of perovskite quantum dots (PeQDs). Nevertheless, the electron beam of TEM as an illumination source provides high energy, which causes morphological variation (fusion and melting) and recession of the crystalline structure in low radiolysis tolerance specimens. Hence, a novel and facile strategy is proposed: electron beam peel [PbBr6]4- octahedron defects from the surface of QDs to optimize the crystal structure. TEM and high-angle annular dark-field scanning TEM (HAADF) tests indicate that the [PbBr6]4- octahedron would be peeled from the surface of QDs when QDs samples were irradiated under high-power irradiation, and then a clear image would be obtained. To avoid interference from a protective film of "carbon deposits" on the surface of the sample when using high resolution TEM, amorphous carbon film (15-20 nm) was deposited on the surface of QDs film and then characterized by TEM and HAADF. The detection consequences showed that the defection of PbBr2 on the surface of QDs will gradually disappear with the extension of radiation time, which further verifies the conjecture.

Identifying the effect of tributyl phosphate on the growth of PbTe quantum dots: Linking experimental and theoretical approaches

The effects of tributyl phosphate (TBP), as a process control agent (PCA), on morphology, size and dispersion of PbTe quantum dots (QDs), at 5 h of milling time, are investigated. By using X-ray diffraction, the occurrence of PbTe is detected, while the PbTe formation and morphology, during milling, are studied via transmission electron microscopy (TEM). According to TEM results, the occurrence of nearly spherical and faceted PbTe QDs are ruled by highly structural-defect and oriented attachment mechanisms, respectively. What is more, mechanical kneading is effectively inhibited when 3 wt% TBP is added during milling. Dispersion-corrected density functional theory (DFT) calculations are carried out to understand the factors that affect growth and morphology of PbTe QDs. DFT results demonstrated that both the intrinsic characteristics of PbTe and the adsorption of certain reaction species are responsible for the shape control of PbTe QDs, which is useful to propose adsorption modes of TBF on PbTe surface and to rationalize the facets exposed by PbTe after the surface treatment. In agreement with experimental results, Wulff constructions proposed are cube-like quantum dots with sharp edges, but rounded edges are possible as well.

GaAs quantum dots under quasiuniaxial stress: Experiment and theory

The optical properties of excitons confined in initially unstrained GaAs/AlGaAs quantum dots are studied as a function of a variable quasiuniaxial stress. To allow the validation of state-of-the-art computational tools for describing the optical properties of nanostructures, we determine the quantum dot morphology and the in-plane components of externally induced strain tensor at the quantum dot positions. Based on these experimental parameters, we calculate the strain-dependent excitonic emission energy, degree of linear polarization, and fine-structure splitting using a combination of eight-band $\mathbf{k}\ifmmode\cdot\else\textperiodcentered\fi{}\mathbf{p}$ formalism with multiparticle corrections using the configuration interaction method. The experimental observations are quantitatively well reproduced by our calculations and deviations are discussed.

Study of Photophysical Properties of Thiol-capped CdS Quantum Dots Doped with Gold Nanoparticles.

In this study, CdS quantum dots (QDs) capped with benzyl mercaptan (thiol) were prepared by microwave irradiation technique. The shape, size, morphology, and spectral properties of thiol-capped CdS QDs were characterized with transmission electron microscopy (TEM), scanning electron microscopy (SEM), UV-vis absorption, and photoluminescence (PL) spectrometry. The photophysical properties of synthesized thiol-capped CdS QDs in the presence of different amounts of gold nanoparticles (AuNPs) have been investigated, exhibiting strong PL quenching. The amount of fluorescence quenching was found to be dependent on the concentration of metal nanoparticles. A Stern-Volmer kinetics model was used to analyze the observed quenching mechanism as a function of the quencher (AuNPs) concentration. The Stern-Volmer plot along with the absorption spectra of thiol-capped CdS QDs in the absence and presence of AuNPs suggest the dynamic (collision) nature of quenching and rule out the possibility of static quenching. The energy transfers from QDs to Au NPs, and hence the quenching of QDs emissions provides new insight into designing novel optical-based materials and the development of FRET-based bionanosensors and phototherapeutic applications.

Surface Vertical Multi-Emission Laser with Distributed Bragg Reflector Feedback from CsPbI3 Quantum Dots.

Quantum dots (QDs) laser has become an important way to solve micro-application problems in many fields. However, single wavelength distributed Bragg reflector (DBR) has many limitations in practical applications, such as signal transmission. How to realize multiwavelength DBR lasing output simply is a challenge. To achieve a stable multi-wavelength quantum dots laser in the near-infrared region, the perovskite CsPbI3 QDs laser with DBR structure is developed in this paper. A tetragonal crystal structure with complete bonding information and no defect is explained by X-ray diffractions (XRD) and Raman spectrum. The cross-section morphology of the DBR laser and the surface morphology of QDs is measured by scanning electron microscope (SEM) and transmission electron microscope (TEM), respectively. An elliptical light propagation field and a double wavelength laser radiation are obtained from the finite-difference time-domain (FDTD) simulation. The output of the three wavelength lasers at 770 nm, 823 nm, and 873 nm is measured. The emission time of a DBR laser is about 2 h, and the average fluorescence quantum yield is 60%. The cavity length selection and energy level model are put in place to clearly see the working mechanism. All the results suggest that an effective and stable CsPbI3 quantum dots DBR laser is realized.

InAs quantum emitters at telecommunication wavelengths grown by droplet epitaxy

InAs quantum dots at telecommunication wavelengths are desired as single-photon sources, but a growth technique that enables wide control over quantum dot size, density, and morphology is needed. Droplet epitaxy is well suited for this purpose, but InAs nanostructures tend to form as rings on (001) InGaAs, InAlAs, and InP surfaces. In this work, we investigate how surface diffusion can be manipulated to grow quantum dots by molecular beam epitaxy without using high-index substrates or metamorphic buffers. First, surface diffusion characteristics of In on In0.52Al0.48As are compared to In and Ga on In0.53Ga0.47As. Then, a two-step arsenic exposure protocol is applied to modify the droplet crystallization step, resulting in a series of different nanostructure morphologies that have narrow-linewidth emission between 1200 and 1520 nm at 4 K. Ultimately, we show that controlling surface diffusion of the group-III species during growth is critical for achieving quantum dots appropriate for single-photon sources at telecommunication wavelengths.

An investigation on the structural and optical properties of mercaptosuccinic acid capped cadmium telluride quantum dots

In this work, a sonication induced modified wet chemical approach is adopted to synthesize highly luminescent and water soluble cadmium telluride (CdTe) quantum dots (QDs). The morphology, size, crystal structural, and optical properties of CdTe QDs are investigated for different refluxing time (1–4 h). The refluxing time-dependent optical constants viz. band gap energy and Urbach energy of the QDs are estimated from UV–Visible absorption spectra. The optical band gap energy decreased from ~ 2.12 to 1.92 eV and the Urbach energy increased from ~ 361 to 487 meV, with the increase in refluxing time. CdTe QDs are found to be uniform in size. The average size of the QDs estimated from the High Resolution Transmission Electron Microscope image analysis is about 5.8 and 8.2 nm for refluxing times 1 and 4 h, respectively. The growth mechanism of the QDs as a function of refluxing time has also been discussed. The fluorescence spectra of the QDs, revealed emission peaks having wavelength from ~ 534 to 585 nm, under the excitation wavelength of 320 nm. The fluorescence emission peaks showed a bathochromic shift with increasing refluxing time. CdTe QDs also exhibit excitation-dependent fluorescence behaviour. Two crystalline phases of the CdTe QDs, namely hexagonal and cubic are confirmed from the High Resolution Transmission Electron Microscope images and Selected Area Electron Diffraction patterns analysis. The phase transformation from hexagonal to cubic is successfully achieved by tuning the refluxing time from 1 to 4 h.

Supercritical millifluidic reactor for the synthesis of efficient GaN nanophotocatalysts

Here, we demonstrate the continuous synthesis of gallium nitride (GaN) nanophotocatalysts exhibiting high quantum confinement using a preheated supercritical millireactor. The GaN quantum dots (QDs) are obtained from the direct thermolysis of a single source amido complex precursor (tris(dimethyl)amido gallium(III) dimer), in anhydrous supercritical cyclohexane. The quality of the synthesized QDs is highly dependent on the chemical pathways for the single source precursor thermolysis. Through the use of numerical modeling, we designed a millifluidic reactor allowing a sufficiently high heating rate for a direct precursor thermolysis towards efficient GaN nanoparticles. The as-designed preheated supercritical flow reactor yields highly reproducible GaN QDs (optical properties, crystallite phase and morphology) at high throughput, enabling gram scale production. Eventually, the photocatalytic properties of the GaN QDs were evaluated in a direct photochemical reaction through the degradation of a dye molecule (Methyl Orange). The obtained results demonstrate the higher photocatalytic activity of such photocatalysts compared to the commercially and reference available Degussa P25.

Effective growth strategy of colloidal quantum dots with low defects and high brightness

Quantum dots (QDs) with an alloy shell (CdSe@ZnS/ZnS) are one of the most promising emitters for optoelectronic devices for their superior properties such as narrow full width at half maximum (FWHM), high color purity and tunable wavelength. However, the presence of lattice stresses during the internal growth of quantum dots can cause severe exciton bursts. Optimizing the ramp-up process during the core growth of quantum dots and rising the temperature when cladding with ZnS shells is an effective strategy for obtaining high-quality quantum dots. Besides, the stability of quantum dots is further modified by using 1-Octanethiol (OT) as ligands. Detailed analyses of the morphology, colloidal stability, and luminescence performance of QDs were represented. Finally, green CdSe@ZnS/ZnS QLEDs with prolonged carrier lifetimes and less defect state densities achieved peak luminescence at 361850 cd/m2 with a current efficiency (CE) of 33 cd/A. This work provides a better understanding of the relationship between defect state density and the performance of quantum dots for designing and fabricating high-performance light-emitting diodes.

Ligand and local surface strain-assisted doping for cadmium chalcogenide II-VI quantum dots

Different specific preparation methods of Ag-doped cadmium chalcogenide nanocrystals (NCs) in the post-synthetic stage were proposed by many groups. These methods usually emphasize the Ag precursors but ignore other factors that can influence the Ag-doping process. We used Ag film to dope the CdSe and CdS quantum dots to achieve the Ag-dopant photoluminescence (PL). That Ag-doping process can be modified effectively via tuning the surface stoichiometry, ligands, and morphology of cadmium chalcogenide quantum dots. Ag source is not the key factor influencing the doping process. We attributed those phenomena to that the local surface strain caused by those factors can lower the barrier of the Ag–Cd cation exchange. We also found that Ag+ can passivate the chalcogenide-rich QDs to enhance the band edge emission. This conclusion can explain the diversity of Ag-doping in various cadmium chalcogenide nanocrystals. The pure Ag-dopant PL was obtained by artificially constructing a strain-rich surface on CdSe QDs.

On the Molecular Origin of the Red Emission in the Newly Synthesized Carbon‐Based Quantum Dots

AbstractCarbon‐based quantum dots (QDs) represent a new family of luminescent nanomaterials with intriguing emission properties. They are synthesized predominately with the emission in the blue and green region of the visible spectrum, with limited success in producing red emission. Furthermore, the current literature on the subject lacks consensus with respect to the morphology of QDs. Contrary to their semiconductor counterparts, the data on the structure of fluorescing centers is scarce. Herein, we describe a facile one‐pot synthesis of red emissive QDs using citric acid and formamide as precursors without addition of any other source of nitrogen. The photophysical properties of the synthesized species were investigated by steady state and transient absorption and fluorescence spectroscopy. Some structural peculiarities were revealed using fluorescence correlation spectroscopy. Our findings show that the newly synthesized carbon‐based QDs, at least their emissive centers, are not part of nanoparticles but rather resemble small organic fluorophores. Furthermore, we have not eliminated the possibility that multiple fluorophores with different emission properties may be embedded within a single molecular entity.