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1.
ACS Appl Bio Mater ; 2024 Jul 04.
Artigo em Inglês | MEDLINE | ID: mdl-38963757

RESUMO

The increasing prevalence of multidrug-resistant (MDR) pathogens has promoted the development of innovative approaches, such as drug repurposing, synergy, and efficient delivery, in complement to traditional antibiotics. In this study, we present an approach based on biocompatible nanocarriers containing antimicrobial cations and known antibiotics. The matrices were prepared by coordinating GaIII or InIII to formulations of chitosan/tripolyphosphate or catechol-functionalized chitosan with or without encapsulated antibiotics, yielding particles of 100-200 nm in hydrodynamic diameter. MDR clinical isolates of Pseudomonas aeruginosa were found to be effectively inhibited by the nanocarriers under nutrient-limiting conditions. Fractional inhibitory concentration (FIC) indices revealed that cation- and antibiotic-encapsulated nanomatrices were effective against both Gram-negative and Gram-positive pathogens. Metallophores, such as deferoxamine (DFO), were probed to facilitate the sequestration and transport of the antimicrobial cations GaIII or InIII. Although the antimicrobial activities were less significant with DFO, the eradication of biofilm-associated bacteria showed promising trends against P. aeruginosa and Staphylococcus epidermidis. Interestingly, indium-containing compounds showed enhanced activity on biofilm formation and eradication, neutralizing P. aeruginosa under Fe-limiting conditions. In particular, InIII-cross-linked catechol-modified chitosan matrices were able to inhibit pathogenic growth together with DFO. The nanocarriers showed low cytotoxicity toward A549 cells and improvable CC50 values with NIH/3T3 cells.

2.
Adv Sci (Weinh) ; : e2404272, 2024 Jul 02.
Artigo em Inglês | MEDLINE | ID: mdl-38953411

RESUMO

The phenomenon of flexoelectricity, wherein mechanical deformation induces alterations in the electron configuration of metal oxides, has emerged as a promising avenue for regulating electron transport. Leveraging this mechanism, stress sensing can be optimized through precise modulation of electron transport. In this study, the electron transport in 2D ultra-smooth In2O3 crystals is modulated via flexoelectricity. By subjecting cubic In2O3 (c-In2O3) crystals to significant strain gradients using an atomic force microscope (AFM) tip, the crystal symmetry is broken, resulting in the separation of positive and negative charge centers. Upon applying nano-scale stress up to 100 nN, the output voltage and power values reach their maximum, e.g. 2.2 mV and 0.2 pW, respectively. The flexoelectric coefficient and flexocoupling coefficient of c-In2O3 are determined as ≈0.49 nC m-1 and 0.4 V, respectively. More importantly, the sensitivity of the nano-stress sensor upon c-In2O3 flexoelectric effect reaches 20 nN, which is four to six orders smaller than that fabricated with other low dimensional materials based on the piezoresistive, capacitive, and piezoelectric effect. Such a deformation-induced polarization modulates the band structure of c-In2O3, significantly reducing the Schottky barrier height (SBH), thereby regulating its electron transport. This finding highlights the potential of flexoelectricity in enabling high-performance nano-stress sensing through precise control of electron transport.

3.
Artigo em Inglês | MEDLINE | ID: mdl-38968699

RESUMO

In this work, the production of novel multishell silver indium selenide quantum dots (QDs) shelled with zinc selenide and zinc sulfide through a multistep synthesis precisely designed to develop high-quality red-emitting QDs is explored. The formation of the multishell nanoheterostructure significantly improves the photoluminescence quantum yield of the nanocrystals from 3% observed for the silver indium selenide core to 27 and 46% after the deposition of the zinc selenide and zinc sulfide layers, respectively. Moreover, the incorporation of the multishelled QDs in a poly(methyl methacrylate) (PMMA) matrix via in situ radical polymerization is investigated, and the role of thiol ligand passivation is proven to be fundamental for the stabilization of the QDs during the polymerization step, preventing their decomposition and the relative luminescence quenching. In particular, the role of interface chemistry is investigated by considering both surface passivation by inorganic zinc chalcogenide layers, which allows us to improve the optical properties, and organic thiol ligand passivation, which is fundamental to ensuring the chemical stability of the nanocrystals during in situ radical polymerization. In this way, it is possible to produce silver-indium selenide QD-PMMA composites that exhibit bright red luminescence and high transparency, making them promising for potential applications in photonics. Finally, it is demonstrated that the new silver indium selenide QD-PMMA composites can serve as an efficient color conversion layer for the production of red light-emitting diodes.

4.
J Environ Manage ; 365: 121521, 2024 Jul 02.
Artigo em Inglês | MEDLINE | ID: mdl-38959774

RESUMO

As part of electronic waste (e-waste), the fastest growing solid waste stream in the world, discarded liquid crystal displays (LCDs) contain substantial amounts of both valuable and potentially harmful metal, offering valuable opportunities for resource extraction but posing environmental threats. The present comprehensive study is an investigation into the bioleaching of indium from discarded LCD panels, with a particular focus on high pulp density shredded (Sh-LCDs) and powdered (P-LCDs) materials. This study involved an acidophilic consortium, with two pathways, namely the mixed sulfur-iron pathways and sulfur pathways, being explored to understand the bioleaching mechanisms. Indium bioleaching efficiencies through the mixed sulfur-iron pathway were approximately 60% and 100% for Sh-LCDs and P-LCDs, respectively. Three mechanisms were involved in the extraction of indium from LCD samples: acidolysis, complexolysis, and redoxolysis. The microbial community adapted to a pulp density of 32.5 g/L was streak-plated and it was revealed that sulfur-oxizing bacteria dominated, resulting in the minimum indium extraction of 10% and 55% for both Sh-LCDs and P-LCDs samples, respectively. It was generally accepted that ferric ions as oxidants were effective for indium bioleaching from both the Sh-LCDs and P-LCDs. This implies that the cooperation or interaction within the microbial community used in the bioleaching process had a beneficial impact, enhancing the overall effectiveness of extracting indium from LCD panels. The adapted consortium utilizes a combination of microbial transformation, efflux systems, and chelation through extracellular substances to detoxify heavy metals. The adapted microbial community demonstrated better indium leaching efficiency (50%) compared to the non-adapted microbial community which achieved a maximum of 29% and 5% respectively from Sh-LCDs and P-LCDs at a pulp density of 32.5 g/L. The advantages of an adapted microbial community for indium leaching efficiency, attributing this advantage to factors such as high metabolic activity and improved tolerance to heavy metals. Additionally, the protective role of the biofilm formed by the adapted microbial community is particularly noteworthy, as it contributes to the community's resilience in the presence of inhibitory substances. This information is valuable for understanding and optimizing bioleaching processes for indium recovery, and by extension to possibly other metals.

5.
Artigo em Inglês | MEDLINE | ID: mdl-38961586

RESUMO

The development of broadband photosensors has become crucial in various fields. Indium-gallium-zinc oxide (IGZO, In:Ga:Zn = 1:1:1) phototransistors with PbS quantum dots (QDs) have shown promising features for such sensors, such as reasonable mobility, low leakage current, good photosensitivity, and low-cost fabrication. However, the instability of PbS QD/IGZO phototransistors under an air atmosphere and prolonged storage remain serious concerns. In this article, two concepts to improve the reliability of PbS QD/IGZO phototransistors were implemented. P-type doping in the PbS QD layer through oxidation allows increasing the built-in potential between IGZO and PbS QDs, leading to enhancement in photoinduced electron-hole pair creation. Second, agglomeration and fusion of a PbS QDs layer were controlled via thermal annealing, which facilitated the transport of photocreated carriers. The p-type doping and interconnection of a PbS QD layer can be achieved by deposition and subsequent thermal annealing of gallium oxide (Ga2O3) on PbS QD/IGZO stacks. The resulting Ga2O3/PbS QD/IGZO phototransistors exhibited high-performance switching characteristics under dark conditions. Notably, they showed a remarkable photoresponsivity of 196.69 ± 4.05 A/W and a detectivity of (5.47 ± 1.4) × 1012 Jones even at a long-wavelength illumination of 1550 nm. While the unpassivated PbS/IGZO phototransistor suffered serious degradation in optical performance after 2 weeks of storage, the Ga2O3/PbS QD/IGZO phototransistor demonstrated enhanced stability, maintaining high performance for over 5 weeks. These findings suggest that Ga2O3/PbS QD/IGZO phototransistors offer a feasible approach for the fabrication of large-scale active matrix broadband photosensor arrays, potentially revolutionizing optical sensing in various cutting-edge applications.

6.
Artigo em Inglês | MEDLINE | ID: mdl-38972068

RESUMO

Tin oxide is a promising channel material, offering the advantages of being low-cost and environmentally friendly and having a wide band gap. However, despite the high electron mobility of SnO2 in bulk, the corresponding thin-film transistors (TFTs) generally exhibit moderate performance, hindering their widespread application. Herein, we proposed a codoping strategy to improve both the electrical property and the stability of SnO2 TFTs. A comparative analysis between doped and undoped SnO2 was conducted. It is observed that taking advantage of the difference in ionic radii between two dopants (indium and gallium) and the tin ions in the host lattice can effectively reduce impurity-induced strain. Additionally, we investigated the effect of codoping content on SnO2 TFTs. The optimal codoped SnO2 (TIGO) TFTs demonstrate high performance, featuring a field-effect mobility of 15.9 cm2/V·s, a threshold voltage of 0.2 V, a subthreshold swing of 0.5 V/decade, and an on-to-off current ratio of 2.2 × 107. Furthermore, the devices show high stability under both positive and negative bias stress conditions with a small threshold voltage shift of 1.8 and -1.2 V, respectively. Utilizing the TIGO TFTs, we successfully constructed a resistor-loaded unipolar inverter with a high gain of 10.76. This study highlights the potential of codoped SnO2 TFTs for advanced applications in electronic devices.

7.
Materials (Basel) ; 17(11)2024 Jun 06.
Artigo em Inglês | MEDLINE | ID: mdl-38894047

RESUMO

This study examined the impact of temperature optimization on indium tin oxide (ITO) films in monolithic HJT/perovskite tandem solar cells. ITO films were deposited using magnetron sputtering at temperatures ranging from room temperature (25 °C) to 250 °C. The sputtering target was ITO, with a mass ratio of In2O3 to SnO2 of 90% to 10%. The effects of temperature on the ITO film were analyzed using X-ray diffraction (XRD), spectroscopic ellipsometry, and sheet resistance measurements. Results showed that all ITO films exhibited a polycrystalline morphology, with diffraction peaks corresponding to planes (211), (222), (400), (440), and (622), indicating a cubic bixbyite crystal structure. The light transmittance exceeded 80%, and the sheet resistance was 75.1 Ω/sq for ITO deposited at 200 °C. The optical bandgap of deposited ITO films ranged between 3.90 eV and 3.93 eV. Structural and morphological characterization of the perovskite solar cell was performed using XRD and FE-SEM. Tandem solar cell performance was evaluated by analyzing current density-voltage characteristics under simulated sunlight. By optimizing the ITO deposition temperature, the tandem cell achieved a power conversion efficiency (PCE) of 16.74%, resulting in enhanced tandem cell efficiency.

8.
Small ; : e2402432, 2024 Jun 08.
Artigo em Inglês | MEDLINE | ID: mdl-38850181

RESUMO

This paper presents a scalable and straightforward technique for the immediate patterning of liquid metal/polymer composites via multiphase 3D printing. Capitalizing on the polymer's capacity to confine liquid metal (LM) into diverse patterns. The interplay between distinctive fluidic properties of liquid metal and its self-passivating oxide layer within an oxidative environment ensures a resilient interface with the polymer matrix. This study introduces an inventive approach for achieving versatile patterns in eutectic gallium indium (EGaIn), a gallium alloy. The efficacy of pattern formation hinges on nozzle's design and internal geometry, which govern multiphase interaction. The interplay between EGaIn and polymer within the nozzle channels, regulated by variables such as traverse speed and material flow pressure, leads to periodic patterns. These patterns, when encapsulated within a dielectric polymer polyvinyl alcohol (PVA), exhibit an augmented inherent capacitance in capacitor assemblies. This discovery not only unveils the potential for cost-effective and highly sensitive capacitive pressure sensors but also underscores prospective applications of these novel patterns in precise motion detection, including heart rate monitoring, and comprehensive analysis of gait profiles. The amalgamation of advanced materials and intricate patterning techniques presents a transformative prospect in the domains of wearable sensing and comprehensive human motion analysis.

9.
Adv Sci (Weinh) ; : e2401990, 2024 Jun 13.
Artigo em Inglês | MEDLINE | ID: mdl-38868931

RESUMO

Photocatalytic CO2 reduction is considered as a promising strategy for CO2 utilization and producing renewable energy, however, it remains challenge in the improvement of photocatalytic performance for wide-band-gap photocatalyst with controllable product selectivity. Herein, the sulfur-doped In(OH)3 (In(OH)xSy-z) nanocubes are developed for selective photocatalytic reduction of CO2 to CH4 under simulated light irradiation. The CH4 yield of the optimal In(OH)xSy-1.0 can be enhanced up to 39 times and the CH4 selectivity can be regulated as high as 80.75% compared to that of pristine In(OH)3. The substitution of sulfur atoms for hydroxyl groups in In(OH)3 enhances the visible light absorption capability, and further improves the hydrophilicity behavior, which promotes the H2O dissociation into protons (H*) and accelerates the dynamic proton-feeding CO2 hydrogenation. In situ DRIFTs and DFT calculation confirm that the non-metal sulfur sites significantly weaken the over-potential of the H2O oxidation and prevent the formation of ·OH radicals, enabling the stabilization of *CHO intermediates and thus facilitating CH4 production. This work highlights the promotion effect of the non-metal doping engineering on wide-band-gap photocatalysts for tailoring the product selectivity in photocatalytic CO2 reduction.

10.
Ups J Med Sci ; 1292024.
Artigo em Inglês | MEDLINE | ID: mdl-38863725

RESUMO

Background: The development of bispecific antibodies that can traverse the blood-brain barrier has paved the way for brain-directed immunotherapy and when radiolabelled, immunoPET imaging. The objective of this study was to investigate how indium-111 (111In) radiolabelling with compatible chelators affects the brain delivery and peripheral biodistribution of the bispecific antibody RmAb158-scFv8D3, which binds to amyloid-beta (Aß) and the transferrin receptor (TfR), in Aß pathology-expressing tg-ArcSwe mice and aged-matched wild-type control mice. Methods: Bispecific RmAb158-scFv8D3 (biAb) was radiolabelled with 111In using CHX-A"-DTPA, DOTA, or DOTA-tetrazine (DOTA-Tz). Affinity toward TfR and Aß, as well as stability, was investigated in vitro. Mice were then intravenously administered with the three different radiolabelled biAb variants, and blood samples were collected for monitoring pharmacokinetics. Brain concentration was quantified after 2 and 72 h, and organ-specific retention was measured at 72 h by gamma counting. A subset of mice also underwent whole-body Single-photon emission computed tomography (SPECT) scanning at 72 h after injection. Following post-mortem isolation, the brains of tg-ArcSwe and WT mice were sectioned, and the spatial distribution of biAb was further investigated with autoradiography. Results: All three [111In]biAb variants displayed similar blood pharmacokinetics and brain uptake at 2 h after administration. Radiolabelling did not compromise affinity, and all variants showed good stability, especially the DOTA-Tz variant. Whole-body SPECT scanning indicated high liver, spleen, and bone accumulation of all [111In]biAb variants. Subsequent ex vivo measurement of organ retention confirmed SPECT data, with retention in the spleen, liver, and bone - with very high bone marrow retention. Ex vivo gamma measurement of brain tissue, isolated at 72 h post-injection, and ex vivo autoradiography showed that WT mice, despite the absence of Aß, exhibited comparable brain concentrations of [111In]biAb as those found in the tg-ArcSwe brain. Conclusions: The successful 111In-labelling of biAb with retained binding to TfR and Aß, and retained ability to enter the brain, demonstrated that 111In can be used to generate radioligands for brain imaging. A high degree of [111In]biAb in bone marrow and intracellular accumulation in brain tissue indicated some off-target interactions or potential interaction with intrabrain TfR resulting in a relatively high non-specific background signal.


Assuntos
Peptídeos beta-Amiloides , Encéfalo , Radioisótopos de Índio , Tomografia Computadorizada de Emissão de Fóton Único , Animais , Tomografia Computadorizada de Emissão de Fóton Único/métodos , Camundongos , Encéfalo/diagnóstico por imagem , Encéfalo/metabolismo , Distribuição Tecidual , Peptídeos beta-Amiloides/metabolismo , Camundongos Transgênicos , Anticorpos Biespecíficos/farmacocinética , Barreira Hematoencefálica/metabolismo , Barreira Hematoencefálica/diagnóstico por imagem , Receptores da Transferrina/metabolismo , Receptores da Transferrina/imunologia , Compostos Radiofarmacêuticos/farmacocinética , Doença de Alzheimer/diagnóstico por imagem , Doença de Alzheimer/metabolismo
11.
Nanotechnology ; 35(37)2024 Jun 26.
Artigo em Inglês | MEDLINE | ID: mdl-38876085

RESUMO

This study introduces a novel heteroleptic indium complex, which incorporates an amidinate ligand, serving as a high-temperature atomic layer deposition (ALD) precursor. The most stable structure was determined using density functional theory and synthesized, demonstrating thermal stability up to 375 °C. We fabricated indium oxide thin-film transistors (In2O3TFTs) prepared with DBADMI precursor using ALD in wide range of window processing temperature of 200 °C, 300 °C, and 350 °C with an ozone (O3) as the source. The growth per cycle of ALD ranged from 0.06 to 0.1 nm cycle-1at different deposition temperatures. X-ray diffraction and transmission electron microscopy were employed to analyze the crystalline structure as it relates to the deposition temperature. At a relatively low deposition temperature of 200 °C, an amorphous morphology was observed, while at 300 °C and 350 °C, crystalline structures were evident. Additionally, x-ray photoelectron spectroscopy analysis was conducted to identify the In-O and OH-related products in the film. The OH-related product was found to be as low as 1% with an increase the deposition temperature. Furthermore, we evaluated In2O3TFTs and observed an increase in field-effect mobility, with minimal change in the threshold voltage (Vth), at 200 °C, 300 °C, and 350 °C. Consequently, the DBADMI precursor, given its stability at highdeposition temperatures, is ideal for producing high-quality films and stable crystalline phases, with wide processing temperature range makeing it suitable for various applications.

12.
Environ Res ; 259: 119435, 2024 Jun 22.
Artigo em Inglês | MEDLINE | ID: mdl-38914255

RESUMO

Herein, the study introduces a novel bifunctional In2S3/MgTiO3/TiO2@N-CNT (IMTNC) nanocomposite, which is poised to revolutionize the detection and removal of clothianidin (CLD) from aquatic environments by synergistic adsorption and photodegradation. Confirmation of the material's synthesis was done using structural, optical, morphological, and chemical characterizations. An outstanding sensitivity of 2.168 µA/nM.cm2 with a linear range of 4-100 nM and a LOD of 0.04 nM, along with an exceptional elimination efficiency of 98.06 ± 0.84% for about 10 ppm CLD within 18 min was demonstrated by the IMTNC nanocomposite. Extensive studies were carried out to appraise the material's effectiveness in the presence of various interfering species, such as cations, anions, organic compounds, and different water matrices, and a comprehensive assessment of its stability throughout several cycles was made. Response Surface Methodology (RSM) study was used to determine the ideal removal conditions for improved performance. In addition, the catalytic performance in removing various other pollutants was also analyzed. Adding In2S3 and developing N-doped Carbon Nanotubes (N-CNT) increased conductivity and higher electrochemical sensing skills, improving charge transfer and increasing photocatalytic activity. This research underscores the potential of the IMTNC nanocomposite as a promising candidate for advanced environmental sensing and remediation applications.

13.
Adv Mater ; : e2404010, 2024 Jun 27.
Artigo em Inglês | MEDLINE | ID: mdl-38935245

RESUMO

The imperfect charge behavior at the interfaces of perovskite/electron-transport layer (ETL)/transparent conducting oxide (TCO) limits the further performance improvement of perovskite/silicon tandem solar cells. Herein, an indium tin oxide interlayer is deposited between ETL and TCO to address this issue. Specifically, the interlayer is prepared using an all-physical and H2O-free method, electron-beam evaporation, which can avoid any potential damage to the underlying perovskite and ETL layers. Moreover, the interlayer's composition can be readily tuned by changing the evaporator component, enabling authors to regulate the contact resistance and energy-level alignment of the ETL/TCO interface. Consequently, the resultant perovskite/silicon tandem solar cells exhibit an impressive power conversion efficiency (PCE) of 30.8% (certified 30.3%). Moreover, the device retains 98% of its initial PCE after continuous operation under ambient conditions for 1078 h, representing one of the most stable and efficient perovskite/silicon tandem solar cells.

14.
ACS Appl Mater Interfaces ; 16(26): 33461-33474, 2024 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-38888106

RESUMO

The synthesis, physicochemical, and functional properties of composite solids resulting from the surface spread of oxidized indium species onto nanoplatelets of anatase were investigated. Both the size and the interaction between the indium- and titanium-containing components control the functional properties. In the reduction of CO2 to CO, the best samples have an indium content between ca. 2 and 5 mol % and showed an excess rate over the photo and thermo-alone processes above 33% and an energy efficiency of 1.3%. Subnanometric (monomeric and dimeric) indium species present relatively weak thermal catalytic response but strong thermo-photo promotion of the activity. A gradual change in functional properties was observed with the growth of the indium content of the solids, leading to a progressive increase of thermal activity but lower thermo-photo promotion. The study provides a well-defined structure-activity relationship rationalizing the dual thermo-photo properties of the catalysts and establishes a guide for the development of highly active and stable composite solids for the elimination and valorization of CO2.

15.
Fundam Res ; 4(3): 635-641, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38933190

RESUMO

Constructing structure-function relationships is critical for the rational design and development of efficient catalysts for CO2 electroreduction reaction (CO2RR). In2O3 is well-known for its specific ability to produce formic acid. However, how the crystal phase and surface affect the CO2RR activity is still unclear, making it difficult to further improve the intrinsic activity and screen for the most active structure. In this work, cubic and hexagonal In2O3 with different stable surfaces ((111) and (110) for cubic, (120) and (104) for hexagonal) are investigated for CO2RR. Theoretical results demonstrate that the adsorption of reactants on cubic In2O3 is stronger than that on hexagonal In2O3, with the cubic (111) surface being the most active for CO2RR. In experiments, synthesized cubic In2O3 nanosheets with predominantly exposed (111) surfaces exhibited a high HCOO- Faradaic efficiency (87.5%) and HCOO- current density (-16.7 mA cm-2) at -0.9 V vs RHE. In addition, an aqueous Zn-CO2 battery based on a cubic In2O3 cathode was assembled. Our work correlates the phases and surfaces with the CO2RR activity, and provides a fundamental understanding of the structure-function relationship of In2O3, thereby contributing to further improvements in its CO2RR activity. Moreover, the results provide a principle for the directional preparation of materials with optimal phases and surfaces for efficient electrocatalysis.

16.
Nanomaterials (Basel) ; 14(12)2024 Jun 19.
Artigo em Inglês | MEDLINE | ID: mdl-38921931

RESUMO

This work highlights the novel approach of incorporating potassium iodide (KI) doping during the synthesis of In0.53P0.47 core quantum dots (QDs) to significantly reduce the concentration of vacancies (i.e., In vacancies; VIn-) within the bulk of the core QD and inhibit the formation of InPOx at the core QD-Zn0.6Se0.4 shell interfaces. The photoluminescence quantum yield (PLQY) of ~97% and full width at half maximum (FWHM) of ~40 nm were achieved for In0.53P0.47/Zn0.6Se0.4/Zn0.6Se0.1S0.3/Zn0.5S0.5 core/multi-shell QDs emitting red light, which is essential for a quantum-dot organic light-emitting diode (QD-OLED) without red, green, and blue crosstalk. KI doping eliminated VIn- in the core QD bulk by forming K+-VIn- substitutes and effectively inhibited the formation of InPO4(H2O)2 at the core QD-Zn0.6Se0.4 shell interface through the passivation of phosphorus (P)-dangling bonds by P-I bonds. The elimination of vacancies in the core QD bulk was evidenced by the decreased relative intensity of non-radiative unpaired electrons, measured by electron spin resonance (ESR). Additionally, the inhibition of InPO4(H2O)2 formation at the core QD and shell interface was confirmed by the absence of the {210} X-ray diffraction (XRD) peak intensity for the core/multi-shell QDs. By finely tuning the doping concentration, the optimal level was achieved, ensuring maximum K-VIn- substitution, minimal K+ and I- interstitials, and maximum P-dangling bond passivation. This resulted in the smallest core QD diameter distribution and maximized optical properties. Consequently, the maximum PLQY (~97%) and minimum FWHM (~40 nm) were observed at 3% KI doping. Furthermore, the color gamut of a QD-OLED display using R-, G-, and B-QD functional color filters (i.e., ~131.1%@NTSC and ~98.2@Rec.2020) provided a nearly perfect color representation, where red-light-emitting KI-doped QDs were applied.

17.
Nano Lett ; 2024 Jun 06.
Artigo em Inglês | MEDLINE | ID: mdl-38843032

RESUMO

The widespread application of III-V colloidal quantum dots (QDs) as nontoxic, highly tunable emitters is stymied by their high density of trap states. Here, we utilize density functional theory (DFT) to investigate trap state formation in a diverse set of realistically passivated core-only InP and GaP QDs. Through orbital localization techniques, we deconvolute the dense manifold of trap states to allow for detailed assignment of surface defects. We find that the three-coordinate species dominate trapping in III-V QDs and identify features in the geometry and charge environment of trap centers capable of deepening, or sometimes passivating, traps. Furthermore, we observe stark differences in surface reconstruction between InP and GaP, where the more labile InP reconstructs to passivate three-coordinate indium at the cost of distortion elsewhere. These results offer explanations for experimentally observed trapping behavior and suggest new avenues for controlling trap states in III-V QDs.

18.
Adv Sci (Weinh) ; : e2402158, 2024 Jun 25.
Artigo em Inglês | MEDLINE | ID: mdl-38923280

RESUMO

Sol-gel processed zinc oxide (ZnO) is one of the most widely used electron transport layers (ETLs) in inverted organic solar cells (OSCs). The high annealing temperature (≈200 °C) required for sintering to ensure a high electron mobility however results in severe damage to flexible substrates. Thus, flexible organic solar cells based on sol-gel processed ZnO exhibit significantly lower efficiency than rigid devices. In this paper, an indium-doping approach is developed to improve the optoelectronic properties of ZnO layers and reduce the required annealing temperature. Inverted OSCs based on In-doped ZnO (IZO) exhibit a higher efficiency than those based on ZnO for a range of different active layer systems. For the PM6:L8-BO system, the efficiency increases from 17.0% for the pristine ZnO-based device to 17.8% for the IZO-based device. The IZO-based device with an active layer of PM6:L8-BO:BTP-eC9 exhibits an even higher efficiency of up to 18.1%. In addition, a 1.2-micrometer-thick inverted ultrathin flexible organic solar cell is fabricated based on the IZO ETL that achieves an efficiency of 17.0% with a power-per-weight ratio of 40.4 W g-1, which is one of the highest efficiency for ultrathin (less than 10 micrometers) flexible organic solar cells.

19.
ACS Nano ; 18(23): 15130-15138, 2024 Jun 11.
Artigo em Inglês | MEDLINE | ID: mdl-38804707

RESUMO

Narrow gaps between plasmon-supporting materials can confine infrared electromagnetic energy at the nanoscale, thus enabling applications in areas such as optical sensing. However, in nanoparticle dimers, the nature of the transition between touching (zero gap) and nearly nontouching (nonzero gap ≲15 nm) regimes is still a subject of debate. Here, we observe both singular and nonsingular transitions in infrared plasmons confined to dimers of fluorine-doped indium oxide nanocubes when moving from touching to nontouching configurations depending on the dimensionality of the contact region. Through spatially resolved electron energy-loss spectroscopy, we find a continuous spectral evolution of the lowest-order plasmon mode across the transition for finite touching areas, in excellent agreement with the simulations. This behavior challenges the widely accepted idea that a singular transition always emerges in the near-touching regime of plasmonic particle dimers. The apparent contradiction is resolved by theoretically examining different types of gap morphologies, revealing that the presence of a finite touching area renders the transition nonsingular, while one-dimensional and point-like contacts produce a singular behavior in which the lowest-order dipolar mode in the touching configuration, characterized by a net induced charge in each of the particles, becomes unphysical as soon as they are separated. Our results provide valuable insights into the nature of dimer plasmons in highly doped semiconductors.

20.
ACS Nano ; 18(23): 15139-15153, 2024 Jun 11.
Artigo em Inglês | MEDLINE | ID: mdl-38804721

RESUMO

We develop here a comprehensive experimental approach to independently determine charge carrier parameters, namely, carrier density and mass, in plasmonic indium tin oxide nanocrystals. Typically, in plasmonic nanocrystals, only the ratio between these two parameters is accessible through optical absorption experiments. The multitechnique methodology proposed here combines single particle and ensemble optical and magneto-optical spectroscopies, also using 119Sn solid-state nuclear magnetic resonance spectroscopy to probe the surface depletion layer. Our methodology overcomes the limitations of standard fitting approaches based on absorption spectroscopy and ultimately gives access to carrier effective mass directly on the NCs, discarding the use of literature value based on bulk or thin film materials. We found that mass values depart appreciably from those measured on thin films; consequently, we found carrier density values that are different from reported literature values for similar systems. The effective mass was found to deviate from the parabolic approximation at a high carrier density. Finally, the dopant activation and defect diagram for ITO NCs for tin doping between 2.5 and 15% are determined. This approach can be generalized to other plasmonic heavily doped semiconductor nanostructures and represents, to the best of our knowledge, the only method to date to characterize the full Drude parameter space of 0-D nanosystems.

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