Ag2ZnSnS4-ZnS core-shell colloidal quantum dots: a near-infrared luminescent material based on environmentally friendly elements.
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ABSTRACT:
SUBMITTER: Saha A
PROVIDER: S-EPMC8101413 | biostudies-literature |
REPOSITORIES: biostudies-literature
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Project description:An aqueous-phase synthesis of 3-mercaptopropionic acid (3-MPA)-capped core/shell/shell ZnSeS/Cu:ZnS/ZnS QDs was developed. The influence of the Cu-dopant location on the photoluminescence (PL) emission intensity was investigated, and the results show that the introduction of the Cu dopant in the first ZnS shell leads to QDs exhibiting the highest PL quantum yield (25%). The influence of the Cu-loading in the dots on the PL emission was also studied, and a shift from blue-green to green was observed with the increase of the Cu doping from 1.25 to 7.5%. ZnSeS/Cu:ZnS/ZnS QDs exhibit an average diameter of 2.1 ± 0.3 nm and are stable for weeks in aqueous solution. Moreover, the dots were found to be photostable under the continuous illumination of an Hg-Xe lamp and in the presence of oxygen, indicating their high potential for applications such as sensing or bio-imaging.
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Project description:In this study, the CuInS2/ZnS core/shell quantum dots (QDs) were prepared via simple and environmentally friendly solvothermal synthesis and were used as phosphors for white light-emitting diodes (WLEDs). The surface defect of the CuInS2 core QDs were passivated by the ZnS shell by forming CuInS2/ZnS core/shell QDs. By adjusting the Cu/In ratio and the nucleation temperature, the photoluminescence (PL) peak of the CuInS2 QDs was tunable in a range of 651-775 nm. After coating the ZnS layer and modifying oleic acid ligands, the PL quantum yield increased to 85.06%. The CuInS2/ZnS QD powder thermal stability results showed that the PL intensity of the QDs remained 91% at 100°C for 10 min. High color rendering index values (CRI, 90) and correlated color temperature of 4360 K for the efficient WLEDs were fabricated using CuInS2/ZnS QDs and (Ba,Sr)2SiO4:Eu2+ as color converters in combination with a blue GaN light-emitting diode chip.
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Project description:We carried out first-principles calculations to simulate Ag2ZnSnS4 and Ag2CdSnS4 and calculated enthalpies of different plausible structural models (kesterite-type, stannite-type, wurtzkesterite-type, wurtzstannite-type, and GeSb-type) to identify low- and high-pressure phases. For Ag2ZnSnS4, we predict the following transition: kesterite-type→[8.2GPa]→ GeSb-type. At the transition pressure, the electronic structure changes from semiconducting to metallic. For Ag2CdSnS4, we cannot decide which of the experimentally observed structures (kesterite-type or wurtzkesterite-type) is the ground-state structure because their energy difference is too small. At 4.7 GPa, however, we predict a transition to the GeSb-type structure with metallic character for both structures. Regarding the sensitivity of the material to disorder, a major drawback for solar cell applications, Ag2CdSnS4 behaves similar to Cu2ZnSnS4, both showing a high tendency to cationic disorder. In contrast, the disordered structures in Ag2ZnSnS4 are much higher in energy, and therefore, the material is less affected by disorder.
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Project description:Pirquitasite, ideally Ag(2)ZnSnS(4) (disilver zinc tin tetra-sulfide), exhibits tetra-gonal symmetry and is a member of the stannite group that has the general formula A(2)BCX(4), with A = Ag, Cu; B = Zn, Cd, Fe, Cu, Hg; C = Sn, Ge, Sb, As; and X = S, Se. In this study, single-crystal X-ray diffraction data are used to determine the structure of pirquitasite from a twinned crystal from the type locality, the Pirquitas deposit, Jujuy Province, Argentina, with anisotropic displacement parameters for all atoms, and a measured composition of (Ag(1.87)Cu(0.13))(Zn(0.61)Fe(0.36)Cd(0.03))SnS(4). One Ag atom is located on Wyckoff site Wyckoff 2a (symmetry -4..), the other Ag atom is statistically disordered with minor amounts of Cu and is located on 2c (-4..), the (Zn, Fe, Cd) site on 2d (-4..), Sn on 2b (-4..), and S on general site 8g. This is the first determination of the crystal structure of pirquitasite, and our data indicate that the space group of pirquitasite is I-4, rather than I-42m as previously suggested. The structure was refined under consideration of twinning by inversion [twin ratio of the components 0.91?(6):0.09?(6)].
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Project description:Sewage sludge, produced daily and inherent to urban development, presents problems of disposal that are still challenging today. Its disposal still offers palliative solutions, where the final destination is generally in landfills or, restrictively, to use in agriculture. The synthesis of carbon quantum dots (CQDs) from sewage sludge is a better alternative to use the stock of organic material present in the sludge. The present work aims to produce Carbon quantum dots (CQDs) using principles of green chemistry and to use an alternative raw material intrinsic stock of carbon present in sewage sludge, making its final disposal more sustainable. The material obtained has a core structure mainly composed of sp2 carbon and nitrogen. The surface functional groups containing sulfur, nitrogen, and oxygen of CQDs were investigated using FTIR and TG/DSC coupled FTIR techniques. The CQDs showed a luminescence decay time equivalent to fluorescent compounds and with satisfying quantum yield since no passive/oxidizing agent or material purification process was used. The photoluminescence spectroscopy analysis showed that the CDQs excitation λmax was at 360 nm and caused a λmax emission at 437 nm (CQDsa) and 430 nm (CQDsb). The CQDs obtained showed sizes of 9.69 ± 2.64 nm (CQDsa) and 10.92 ± 2.69 nm (CQDsb). In vitro experiments demonstrated the uptake of CQDs by the endothelial cell line EAhy 926 and their nontoxicity. However, the production of CQDs can be used for the sustainable disposal of sewage sludge.
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Project description:Exploring the temperature-dependent photoluminescence (PL) properties of quantum dots (QDs) is not only important for understanding the carrier recombination processes in QD-based devices but also critical for expanding their special applications at different temperatures. However, there is still no clear understanding of the optical properties of CdS/ZnS core/shell QDs as a function of temperature. Herein, the temperature-dependent PL spectra of CdS/ZnS core/shell QDs were studied in the temperature range of 77-297 K. It was found that the band-edge emission (BEE) intensity decreases continuously with increasing temperature, while the surface-state emission (SSE) intensity first increases and then decreases. For BEE intensity, in the low temperature range, a small activation energy (29.5 meV) in the nonradiative recombination process led to the decrease of PL intensity of CdS/ZnS core/shell QDs; and at high temperature the PL intensity attenuation was caused by the thermal escape process. On the other hand, the temperature-dependent variation trend of the SSE intensity was determined by the competition of the trapping process of the surface trap states and the effect of thermally activated non-radiative defects. As the temperature increased, the PL spectra showed a certain degree of redshift in the peak energies of both band-edge and surface states and the PL spectrum full width at half-maximum (FWHM) increases, which was mainly due to the coupling of exciton and acoustic phonon. Furthermore, the CIE chromaticity coordinates turned from (0.190, 0.102) to (0.302, 0.194), which changed dramatically with temperature. The results indicated that the CdS/ZnS core/shell QDs are expected to be applied in temperature sensors.
| S-EPMC9698013 | biostudies-literature
Project description:BackgroundQuantum dots (QDs) have been used as fluorophores in various imaging fields owing to their strong fluorescent intensity, high quantum yield (QY), and narrow emission bandwidth. However, the application of QDs to bio-imaging is limited because the QY of QDs decreases substantially during the surface modification step for bio-application.ResultsIn this study, we fabricated alloy-typed core/shell CdSeZnS/ZnS quantum dots (alloy QDs) that showed higher quantum yield and stability during the surface modification for hydrophilization compared with conventional CdSe/CdS/ZnS multilayer quantum dots (MQDs). The structure of the alloy QDs was confirmed using time-of-flight medium-energy ion scattering spectroscopy. The alloy QDs exhibited strong fluorescence and a high QY of 98.0%. After hydrophilic surface modification, the alloy QDs exhibited a QY of 84.7%, which is 1.5 times higher than that of MQDs. The QY was 77.8% after the alloy QDs were conjugated with folic acid (FA). Alloy QDs and MQDs, after conjugation with FA, were successfully used for targeting human KB cells. The alloy QDs exhibited a stronger fluorescence signal than MQD; these signals were retained in the popliteal lymph node area for 24 h.ConclusionThe alloy QDs maintained a higher QY in hydrophilization for biological applications than MQDs. And also, alloy QDs showed the potential as nanoprobes for highly sensitive bioimaging analysis.
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