Photoluminescence Of Quantum Dots Research Articles

Electrospun polyacrylonitrile nanofibers as graphene oxide quantum dot precursors with improved photoluminescent properties

Graphene oxide quantum dots were synthesized from carbonization, ultrasonic peeling, and oxidation of electrospun polyacrylonitrile (PAN) nanofibers. By energy scattering X-ray spectroscopy, a strong increase/decrease in the carbon/oxygen concentration was found during the stabilization stage and during carbonization, which resulted in the formation of carbon-enrich nanofibers. FTIR spectroscopy and Raman scattering results of electrospun PAN nanofibers demonstrated changes in structural and optical properties during the carbonization process. By X-ray diffraction was found that after the carbonization and oxidation processes of the PAN nanofibers, they showed a hexagonal graphene structure with two main crystallographic directions (002) and (101). The formation of graphene oxide quantum dots resulting from the ultrasonic exfoliation process was demonstrated by TEM with nanocrystal sizes of 10.98 nm, which were obtained after the ultrasonic exfoliation of carbonized/graphitized PAN nanofibers in highly oxidizing solvents. The absorbance in the UV spectral region showed a band at approximately 265 nm, which was assigned to the π→π* excitation of the π bonds of aromatic CC, and another band at 325 nm that was assigned to the n→π* transition of CO bonds, showing the presence of graphene oxide quantum dots (GOQDs). By Raman scattering is found that the synthesized GOQDs have a density of 22.6 ppm of crystalline defects, which indicates a higher order in their crystal lattices. The fluorescence and photoluminescence of the graphene oxide quantum dots showed radiative bands associated with possible crystalline defects in the graphene oxide quantum dot network, the radiative emissions of which correspond to the blue spectral region. The preparation protocol is simple and the yield of graphene oxide quantum dots is high.

39.3: Hybrid Full‐Color Micro‐LED Display with Quantum Dots Color Conversion by Using Inkjet‐Printing and Photo‐Lithography Methods

In this work, a full‐color micro‐LED display is demonstrated with blue micro‐LED as backlight, photoluminescence quantum dots as color conversion layers. Both the inkjet‐printing and photolithography methods are used to fabricate the color conversion layers, in which the backlight and color conversion layers are bonded together by a UV glue.

Pb-Doped Ag2 Se Quantum Dots with Enhanced Photoluminescence in the NIR-II Window.

Ag2 Se quantum dots (QDs) as an effective biological probe in the second near-infrared window (NIR-II, 1000-1700nm) have been widely applied in bioimaging with high tissue penetration depth and high spatiotemporal resolution. However, the ions deficiency and crystal defects caused by the high Ag+ mobility in Ag2 Se crystals are mainly responsible for the inefficient photoluminescence (PL) of Ag2 Se QDs. Herein, a tailored route is reported to achieve controllable doping of Ag2 Se QDs in which Ag is exchanged by Pb via cation exchange (CE), which is unattainable by direct synthetic methods. The Pb-doped Ag2 Se QDs (denoted as Pb:Ag2 Se QDs) present fire-new optical features with significantly enhanced PL intensity of 4.2 folds. Photoelectron spectroscopy confirms that Pb acts as an n-type dopant for Ag2 Se QDs and therefore the electronic impurities provide additional carriers to fill the traps. Moreover, the general validity of this method is demonstrated to convert different sized Ag2 Se into Pb:Ag2 Se QDs, so that a wide range of NIR-II PL with high intensity is obtained. The bright NIR-II emission of Pb:Ag2 Se QDs is further successfully performed in lymphatic system mapping.

Photoluminescence enhancement of CsPbBr3 quantum dots on Au island fiber film surface for optical communication and quantum information communication

Compared with the glass surface, the photoluminescence intensity of CsPbBr3 quantum dots excited by 1200 nm femtosecond laser on the surface of Au island fiber film (AIF) is significantly enhanced. On the other hand, the photoluminescence intensity decay of CsPbBr3 quantum dots on the AIF surface shows a fast decay of the average photoluminescence lifetime. The Photoluminescence enhancement effect of CsPbBr3 quantum dots was analysed by photoluminescence spectrum, transmission electron microscope, absorption spectrum and photoluminescence decay. The spectral changes of CsPbBr3 quantum dots on the AIF surface are related to surface plasmon resonance. The enhanced photoluminescence of CsPbBr3 quantum dots on the AIF surface can be used in optical communication and quantum information communication.

Spectroelectrochemistry of Colloidal CdSe Quantum Dots

Solution-phase spectroelectrochemistry was used to study electron injection into colloidal CdSe quantum dots (QDs) with sizes ranging from 3.4 to 11.1 nm in tetrahydrofuran (THF). The absorbance and photoluminescence of the QDs were monitored in response to both charging and discharging cycles, and the optical changes were reversible on a timescale of minutes. Bleaching of the QD 1S3/2h1Se exciton state was used to determine the conduction band energy levels. We found that the negative trion state was stable in THF for hours under an applied cathodic potential. Both the degree of bleaching and the recovery of the exciton state depended on the applied potential. Based on the current and charge measurements, we found that between 10 and 150 electrons were injected into the QDs, depending on the electrode potential and QD size. Most of the electron injection occurred below the band edge and led to quenching of the QD photoluminescence. The potential at which injection into QDs occurred depended on the nature of the QD ligands.

InAs/InGaAs quantum dots confined by InAlAs barriers for enhanced room temperature light emission: Photoelectric properties and deep levels

InAs/InGaAs heterostructures with quantum dots (QDs) have been studied for quite some time for light-emitting diodes operating from the near to the far infrared range. However, the room temperature QD emission is rather low, thus it is needed to look for improved structure designs allowing efficient enhancement of luminescence. In this work, we study the modification of photo- and thermo-electrical properties of InAs/In0.15Ga0.85As QD heterostructure, when introducing wide-bandgap In0.15Al0.85As confining barriers (CBs) at one or both sides of the QD layer. The structures demonstrate interband QD photoluminescence (PL) peaked at 1.2 μm measured from room temperature down to 10 K. The introduction of CBs allows to enhance the PL intensity by more than four orders of magnitude. The reason is a strong decrease of the thermal escape of both charge carriers confined in QDs and wetting layer, leading to a highly increased radiative recombination. The changes in optical transitions, involving quantum confinement states and defect-related levels, are studied by photocurrent (PC) measurements, also showing the expectable quenching of PC in the structures with CBs. The existing deep levels of defects are determined by thermally stimulated current spectroscopy. Having the same defect spectrum in all the studied structures, an increase in the defect density was detected near CBs at the QD layer. At low temperatures, defect traps in vicinity of the QDs layer caused the Coulomb screening of conductivity channel, that is studied by kinetics measurements in view of the CB introduction. The PC decrement under the constant illumination is theoretically explained by the screening. We confidently show that, despite of a slight increase in defects and PL blueshift in the QD structure with In0.15Al0.85As CBs, they can serve as improved active elements for energy-efficient QD lasers, single-photon emitters and optical amplifiers.

Combined effects of surface plasmon coupling and Förster resonance energy transfer on the light color conversion behaviors of colloidal quantum dots on an InGaN/GaN quantum-well nanodisk structure

By forming nanodisk (ND) structures on a blue-emitting InGaN/GaN quantum-well (QW) template, the QWs become close to the red-emitting quantum dots (QDs) and Ag nanoparticles (NPs) attached onto the sidewalls of the NDs such that Förster resonance energy transfer (FRET) and surface plasmon (SP) coupling can occur to enhance the efficiency of blue-to-red color conversion. With a larger ND height, more QWs are exposed to open air on the sidewall for more QD/Ag NP attachment through QD self-assembly and Ag NP drop casting such that the FRET and SP coupling effects, and hence the color conversion efficiency can be enhanced. A stronger FRET process leads to a longer QD photoluminescence (PL) decay time and a shorter QW PL decay time. It is shown that SP coupling can enhance the FRET efficiency.

Lab-on-Microsphere-FRET-Based Multiplex Sensor Platform.

Here we report on the development and investigation of a novel multiplex assay model based on polymer microspheres (PMS) encoded with ternary AIS/ZnS quantum dots (QDs). The system was prepared via layer-by-layer deposition technique. Our studies of Förster resonance energy transfer (FRET) between the QD-encoded microspheres and two different cyanine dyes have demonstrated that the QD photoluminescence (PL) quenching steadily increases with a decrease in the QD-dye distance. We have found that the sensitized dye PL intensity demonstrates a clear maximum at two double layers of polyelectrolytes between QDs and Dye molecules on the polymer microspheres. Time resolved PL measurements have shown that the PL lifetime decreases for the QDs and increases for the dyes due to FRET. The designed system makes it possible to record spectrally different bands of FRET-induced dye luminescence with different decay times and thereby allows for the multiplexing by wavelength and photoluminescence lifetimes of the dyes. We believe that PMS encoded with AIS/ZnS QDs have great potential for the development of new highly selective and sensitive sensor systems for multiplex analysis to detect cell lysates and body fluids’ representative biomarkers.

State filling effects on photoluminescence and photovoltaic characteristic of aluminium-doped CdTe colloidal quantum dots stabilized in aqueous medium

CdTe and aluminium (Al)-doped CdTe (Al:CdTe QDs) colloidal quantum dots (QDs) were synthesized through an aqueous route. CdTe and Al:CdTe QDs colloidal quantum dots of different size were obtained by collecting the samples at different refluxing time. The size of the synthesized QDs collected after 6 h of refluxing time was measured to 3.3 and 4.8 nm for Al:CdTe QDs and CdTe QDs, respectively. The size shrinkages of Al:CdTe QDs were due to chlorine ions from AlCl3 precursor, which controls the growth kinetics of QDs and stabilizes the QDs in the aqueous phase. The size shrinkages of Al:CdTe QDs result in an increase of bandgap from 2.13 to 2.3 eV and congruently blue-shifted absorbance and emission spectra were discerned. The state filling effect, gradual filling of energy state, observed clearly in photoluminescence spectra of Al:CdTe QDs for samples collected after 30 min of refluxing time. We also fabricated Gratzel-type QDs-sensitized solar cells by loading CdTe and Al:CdTe QDs on mesoporous TiO2 photoanode. Photovoltaic efficiency is marginally increased (13%) from 0.45 to 0.51% for Al-doped CdTe QDs as compared to CdTe QDs.

Light-Triggered Switching of Quantum Dot Photoluminescence through Excited-State Electron Transfer to Surface-Bound Photochromic Molecules.

This paper describes reversible "on-off" switching of the photoluminescence (PL) intensity of CdSe quantum dots (QDs), mediated by photochromic furylfulgide carboxylate (FFC) molecules chemisorbed to the surfaces of the QDs. Repeated cycles of UV and visible illumination switch the FFC between "closed" and "open" isomers. Reversible switching of the QDs' PL intensity by >80% is enabled by different rates and yields of PL-quenching photoinduced electron transfer (PET) from the QDs to the respective isomers. This difference is consistent with cyclic voltammetry measurements and density functional calculations of the isomers' frontier orbital energies. This work demonstrates fatigue-resistant modulation of the PL of a QD-molecule complex through remote control of PET. Such control potentially enables applications, such as all-optical memory, sensing, and imaging, that benefit from a fast, tunable, and reversible response to light stimuli.

Size-focusing results in highly photoluminescent sulfur quantum dots with a stable emission wavelength.

Sulfur quantum dots (SQDs) are a new kind of functional nanomaterial, but several challenges still exist in relation to their synthesis and application, such as low-yield and time-consuming synthetic methods, low photoluminescence quantum yields (PLQYs), and the non-selectivity of their detection mechanisms. Herein, we report the drastic enhancement of the fluorescence performance of water-soluble SQDs via the one-pot synthesis of size-focusing QDs using ultrasound microwave radiation. The synthetic period has been greatly shortened to 2 h via the present process. Notably, the proposed SQDs exhibit a highly stable emission wavelength with a record high PLQY of 58.6%. The mechanistic study indicates that size-focusing is a key factor relating to the proposed high-performance SQDs. As they also have robust stability, the proposed SQDs show a wide range of potential applications. Inspired by the characteristic properties of the SQDs and specific analytes, a simple SQD-based fluorescence sensing platform, via a redox-reaction-mediated mechanism, has been successfully developed for the rapid and selective detection of Ce(iv). In addition, this system has been effectively applied to some Ce(iv)-related biological assays, such as ascorbic acid (AA) analysis. This work is an important breakthrough in the SQD field, opening up avenues for solving the challenging problems relating to SQD-based probes, enriching the fundamental understanding of them, and greatly extending their applications, especially in biomedicine.

Design of cross-linked polyisobutylene matrix for efficient encapsulation of quantum dots.

Photoluminescent quantum dots (QDs) are a prominent example of nanomaterials used in practical applications, especially in light-emitting and light-converting devices. Most of the current applications of QDs require formation of thin films or their incorporation in solid matrices. The choice of an appropriate host material capable of preventing QDs from degradation and developing a process of uniform incorporation of QDs in the matrix have become essential scientific and technological challenges. In this work, we developed a method of uniform incorporation of Cu–Zn–In–S (CZIS) QDs into a highly protective cross-linked polyisobutylene (PIB) matrix with high chemical resistance and low gas permeability. Our approach involves the synthesis of a methacrylate-terminated three-arm star-shaped PIB oligomeric precursor capable of quick formation of a robust 3D polymer network upon exposure to UV-light, as well as the design of a special ligand introducing short PIB chains onto the surface of the QDs, thus providing compatibility with the matrix. The obtained cross-linked QDs-in-polymer composites underwent a complex photostability test in air and under vacuum as well as a chemical stability test. These tests found that CZIS QDs in a cross-linked PIB matrix demonstrated excellent photo- and chemical stability when compared to identical QDs in widely used polyacrylate-based matrices. These results make the composites developed excellent materials for the fabrication of robust, stable and durable transparent light conversion layers.

Excitation dependence and independence of photoluminescence in carbon dots and graphene quantum dots: insights into the mechanism of emission.

Excitation-dependent, multicolor emission from different varieties of 0D carbon systems has attracted immense research attention. It is generally accepted that some variants of 0D carbon exhibit excitation dependent emission, while other variants do not. A third variant exhibits both excitation dependent as well as excitation independent emission. In this work we investigate the structure, composition, steady-state emission-excitation and photoluminescence decay dynamics of three distinctly different variants of 0D carbon - amorphous carbon dots (aCDs), graphene quantum dots (GQDs) and nitrogen-doped GQDs (NGQDs). We find that despite significant differences in the structure and composition there is a striking similarity in the excitation energy dependence of the emission characteristics of these three different dots. All of them exhibit excitation energy independent emission below some threshold wavelength (λth), and above this threshold the emission becomes excitation dependent. We also demonstrate that a similar trend is apparent for nearly all variants of 0D carbon reported in the literature. The threshold wavelength correlates well with the excitation wavelength for the most intense emission and the photoluminescence excitation peaks, suggesting a common origin of light emission in these carbon dots. The findings provide important clues for developing a unified general picture for understanding the light emission mechanism in 0D carbon nanostructures.

Reversible temperature-dependent photoluminescence in semiconductor quantum dots for the development of a smartphone-based optical thermometer.

Photoluminescence (PL) intensity-based non-contact optical temperature sensors are in great demand due to their non-contact nature, rapid response, sensitivity, as well as thermal and chemical stability at different environmental conditions. However, herein, reversible temperature dependent PL emission quenching properties of chemically synthesized Mn2+-doped ZnS QDs (MZQDs) have been advantageously utilized for achieving the development of a smartphone-based optical thermometer. The temperature dependent variations of PL have been studied by taking MZQDs in various forms, such as in aqueous dispersion, powder form, and a polymer-encapsulated thin film. The origin of the PL quenching of MZQD in the polymer film has been cross-verified through temperature-dependent electrical conductivity measurement and the movement of charge carriers has also been confirmed by the first-principles DFT simulation. Through thermal cycling experiments on QD-encapsulated polymer film and by utilizing an indigenously-developed Android App based on color coordinates, a novel smartphone-based colorimetric imaging method for the measurement of temperature has been demonstrated in this work. The synthesized smart QDs might be suitable candidates for temperature sensing and the colorimetric thermometer probe may be utilized in various photonics applications as a smart optical sensor for daily life applications.

Enhanced photoluminescence of silicon quantum dots in the presence of both energy transfer enhancement and emission enhancement mechanisms assisted by the double plasmon modes of gold nanorods.

We propose a scheme utilizing the double plasmon modes of gold nanorods (GNRs) to efficiently increase the Förster resonant energy transfer (FRET) efficiency and enhance the photoluminescence (PL) of Si quantum dots (Si QDs) nearby. Detailed PL and decay dynamics studies are performed for the hybrid nanostructures composed of metallic nanoparticles (MNPs) coated with a Si QD-absorbed silica shell. Plasmon enhanced FRET between Si QDs has been observed and proposed as the third enhancement mechanism for the plasmon-enhanced photoluminescence in addition to excitation enhancement and emission enhancement mechanisms. A maximum FRET efficiency of 46.3% is obtained, which is enhanced by a factor of 8.7 compared to that of samples without MNPs. The dependence of the energy transfer efficiency and the enhancement of the acceptor emission on the surface plasmon resonance (SPR) wavelength, metal-QD distance and QD ratio is examined. The FRET enhancement mechanism dominates when the coupling of plasmon-donor is much stronger than that of plasmon-acceptor with a high acceptor/donor ratio.

Photoluminescence (PL) characterization of InAs/GaAs quantum dots (QDs): A theoretical study

It is well known that before using thin films in applications, it is necessary to carry out their characterization because it provides informations on the degree of their quality. In this article, photoluminescence (PL) characterization of InAs Quantum Dots (QDs) embedded in a GaAs matrix is reported. Detailed analysis of PL mechanisms was introduced and illustrated.Analysis of photoluminescence spectra shows that the homogeneity and the density of the Quantum dots (QDs) depend on the temperature. A shift of PL peaks to lower energies with increasing temperature was reported.We have showed that the absorption and emission in QD are governed by the confinement principles.Our simulation model is mainly based on a single QD and temperature dependent photoluminescence (PL). A good agreement with experimental results is obtained.

Determination of atenolol based on the reversion of the fluorescence resonance energy transfer between AgInS2 quantum dots and Au nanoparticles.

The present work focused on the development of a fluorescence resonance energy transfer (FRET)-based sensing platform for the monitoring of atenolol in pharmaceutical formulations. The implemented approach involved the assembly of d-penicillamine-capped AgInS2/ZnS quantum dots (QDs), as energy donors, and gold nanoparticles (AuNPs) as acceptors and the establishment of electrostatic interaction between both capping ligands at the nanoparticle surface, which induced the inhibition of the ternary QD photoluminescence (PL). The presence of a ZnS shell around the ternary QD core and the use of cysteamine (CA) as the AuNP capping ligand, instead of the typical citrate, allowed a more efficient FRET process to occur. The ability of Cd-free ternary QDs to be used as a sensing element in FRET-based assays was demonstrated, emphasizing the advantages relative to the common Cd-based QDs, when seeking the implementation of more environmentally friendly and less toxic analytical methodologies. The influence of several β-blocker drugs on the FRET donor-acceptor assemblies was thoroughly assessed. Atenolol and nadolol caused the aggregation of CA-AuNPs via hydrogen bonding interactions which reduced the spectral overlap between the donor and acceptor, impairing the FRET process and consequently the emission of the QDs was restored. Under the optimized conditions, the obtained results exhibited a linear relationship between the QD PL recovery signal and atenolol concentration of up to 11.22 mg L-1 with a detection limit of 1.05 mg L-1. This FRET sensing platform was successfully applied in the determination of atenolol in pharmaceutical formulations with recovery values ranging from 97.4 to 104.3%.

ЛЮМИНЕСЦЕНТНОЕ ОПРЕДЕЛЕНИЕ САХАРА В НАТУРАЛЬНОМ МЕДЕ

The photoluminescence of carbon quantum dots synthesized from natural honey and mixtures of honey and sugar has been studied. An increase in the sugar content leads to a decrease in the photoluminescence intensity without changing the shape of the luminescence spectrum of these quantum dots aqueous solutions, which is associated with a decrease in the yield of their synthesis in the sugar presence. The discovered effect can be used to detect sugar in honey. When examining five different market samples of flower honey using this method, two of them showed a significant decrease in the photoluminescence intensity. A laboratory test for compliance with GOST 19792-2017 Standard requirements established an excess of the sucrose content in these samples. Luminescent determination of sugar in honey does not require complicated equipment and can be used to develop a new analytical method for determining the sugar content in counterfeit natural honey.

Interplay of Multiexciton Relaxation and Carrier Trapping in Photoluminescent CdS Quantum Dots Prepared in Aqueous Medium

A comprehensive understanding of exciton dynamics of water-soluble quantum dots (QDs), especially those synthesized directly in aqueous media, is critical for devising their applications. Trapping ...

Relaxation Processes and Exciton-Phonon Interactions in Nanocomposites Based on CdSe/ZnS Semiconductor Quantum Dots and Porphyrin Molecules

Using spectral-kinetic data obtained for nanoassemblies based on CdSe/ZnS semiconductor quantum dots and tetrapyridylporphyrin molecules in methylcyclohexane-toluene mixture 6:1, it was justified that the temperature lowering is accompanied by conformational transformation of the surface ligand (trioctylphosphine oxide or amine) layer in individual quantum dots, which is accelerated in nanoassemblies. It has been shown for the CdSe/ZnS quantum dots that he states determining the absorption band of the first exciton transition, on the one hand, and the photoluminescence band, on the other hand, have different natures. In the frames of existing models for exciton-phonon coupling in semiconductor nanostructures, an analysis has been carried out for the temperature dependence (77–293 K) of quantum dot absorption and photoluminescence properties taking into account conformational effects. It has been established that the formation of the absorption band for the first exciton transition takes place with participation of CdSe core LO phonons, while photoluminescence properties reflect also additional interactions with ZnS shell LO phonons.