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1.
Small ; : e2403325, 2024 Sep 23.
Artículo en Inglés | MEDLINE | ID: mdl-39314054

RESUMEN

The solution-derived non-stoichiometric nickel oxide (NiOx) is a promising hole-injecting material for stable quantum dot light-emitting diodes (QLEDs). However, the carrier imbalance due to the misalignment of energy levels between the NiOx and polymeric hole-transporting layers (HTLs) curtails the device efficiency. In this study, the modification of the NiOx surface is investigated using either 3-cyanobenzoic acid (3-CN-BA) or 4-cyanobenzoic acid (4-CN-BA) in the QLED fabrication. Morphological and electrical analyses revealed that both 4-CN-BA and 3-CN-BA can enhance the work function of NiOx, reduce the oxygen vacancies on the NiOx surface, and facilitate a uniform morphology for subsequent HTL layers. Moreover, it is found that the binding configurations of dipole molecules as a function of the substitution position of the tail group significantly impact the work function of underlying layers. When integrated in QLEDs, the modification layers resulted in a significant improvement in the electroluminescent efficiency due to the enhancement of energy level alignment and charge balance within the devices. Specifically, QLEDs incorporating 4-CN-BA achieved a champion external quantum efficiency (EQE) of 20.34%, which is a 1.8X improvement in comparison with that of the devices utilizing unmodified NiOx (7.28%). Moreover, QLEDs with 4-CN-BA and 3-CN-BA modifications exhibited prolonged operational lifetimes, indicating potential for practical applications.

2.
IEEE Trans Image Process ; 33: 4998-5013, 2024.
Artículo en Inglés | MEDLINE | ID: mdl-39236121

RESUMEN

Blind video quality assessment (VQA) has become an increasingly demanding problem in automatically assessing the quality of ever-growing in-the-wild videos. Although efforts have been made to measure temporal distortions, the core to distinguish between VQA and image quality assessment (IQA), the lack of modeling of how the human visual system (HVS) relates to the temporal quality of videos hinders the precise mapping of predicted temporal scores to the human perception. Inspired by the recent discovery of the temporal straightness law of natural videos in the HVS, this paper intends to model the complex temporal distortions of in-the-wild videos in a simple and uniform representation by describing the geometric properties of videos in the visual perceptual domain. A novel videolet, with perceptual representation embedding of a few consecutive frames, is designed as the basic quality measurement unit to quantify temporal distortions by measuring the angular and linear displacements from the straightness law. By combining the predicted score on each videolet, a perceptually temporal quality evaluator (PTQE) is formed to measure the temporal quality of the entire video. Experimental results demonstrate that the perceptual representation in the HVS is an efficient way of predicting subjective temporal quality. Moreover, when combined with spatial quality metrics, PTQE achieves top performance over popular in-the-wild video datasets. More importantly, PTQE requires no additional information beyond the video being assessed, making it applicable to any dataset without parameter tuning. Additionally, the generalizability of PTQE is evaluated on video frame interpolation tasks, demonstrating its potential to benefit temporal-related enhancement tasks.


Asunto(s)
Procesamiento de Imagen Asistido por Computador , Grabación en Video , Humanos , Grabación en Video/métodos , Procesamiento de Imagen Asistido por Computador/métodos , Percepción Visual/fisiología , Algoritmos
3.
Angew Chem Int Ed Engl ; : e202412712, 2024 Aug 21.
Artículo en Inglés | MEDLINE | ID: mdl-39168820

RESUMEN

Organic heterostructures (OHs) with multi-segments exhibit special optoelectronic properties compared with monomeric structures. Nevertheless, the synthesis of multi-block heterostructures remains challenging due to compatibility issues between segment parts, which restricts their application in optical waveguides and integrated optics. Herein, we demonstrate programmable in-situ co-assembly engineering, combining multi-step spontaneous self-assembly processes to promote the synthesis of multi-block heterostructures with a rational arrangement of three or more segments. The rational design of segments enables exciton manipulation and ensures optical waveguides and proper output among the multi-segment OHs. This work enables the controllable growth of segments within multi-block OHs, providing a pathway to construct complex OHs for the rational development of future optical applications.

4.
Angew Chem Int Ed Engl ; 63(40): e202407833, 2024 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-38984901

RESUMEN

Near-infrared light-emitting diodes (NIR LEDs) based on perovskite quantum dots (QDs) have produced external quantum efficiency (EQE) of ~15 %. However, these high-performance NIR-QLEDs suffer from immediate carrier quenching because of the accumulation of migratable ions at the surface of the QDs. These uncoordinated ions and carriers-if not bound to the nanocrystal surface-serve as centers for exciton quenching and device degradation. In this work, we overcome this issue and fabricate high-performance NIR QLEDs by devising a ligand anchoring strategy, which entails dissolving the strong-binding ligand (Guanidine Hydroiodide, GAI) in the mediate-polar solvent. By employing the dye-sensitized device structure (phosphorescent indicator), we demonstrate the elimination of the interface defects. The treated QDs films exhibit an exciton binding energy of 117 meV: this represents a 1.5-fold increase compared to that of the control (74 meV). We report, as a result, the NIR QLEDs with an EQE of 21 % which is a record among NIR perovskite QLEDs. These QLEDs also exhibit a 7-fold higher operational stability than that of the best previously reported NIR QLEDs. Furthermore, we demonstrate that the QDs are compatible with large-area QLEDs: we showcase 900 mm2 QLEDs with EQE approaching 20 %.

5.
Angew Chem Int Ed Engl ; : e202408712, 2024 Jul 04.
Artículo en Inglés | MEDLINE | ID: mdl-38962896

RESUMEN

Noncovalent spatial interaction has become an intriguing and important tool for constructing optoelectronic molecules. In this study, we linearly attached three conjugated units in a multi π-stacked manner by using just one trident bridge based on indeno[2,1-b]fluorene. To achieve this structure, we improved the synthetic approach through double C-H activation, significantly simplifying the preparation process. Due to the proximity of the C10, C11, and C12 sites in indeno[2,1-b]fluorene, we derived two novel donor|acceptor|donor (D|A|D) type molecules, 2DMB and 2DMFB, which exhibited closely packed intramolecular stacking, enabling efficient through-space charge transfer. This molecular construction is particularly suitable for developing high-performance thermally activated delayed fluorescence materials. With donor(s) and acceptor(s) constrained and separated within this spatially rigid structure, elevated radiative transition rates, and high photoluminescence quantum yields were achieved. Organic light-emitting diodes incorporating 2DMB and 2DMFB demonstrated superior efficiency, achieving maximum external quantum efficiencies of 28.6 % and 16.2 %, respectively.

6.
J Neurointerv Surg ; 2024 Jun 14.
Artículo en Inglés | MEDLINE | ID: mdl-38876784

RESUMEN

BACKGROUND: Saccular aneurysms of the proximal A1 segment (SAPA1) are rare, but their treatment is challenging and scarcely described in the literature. We report the immediate and long term outcomes of their endovascular management. METHODS: We retrospectively analyzed all consecutive SAPA1 cases treated endovascularly at our center between 2003 and 2023. Per procedural complications and radioclinical outcomes were prospectively recorded. RESULTS: Among 2468 patients followed up for aneurysms, 12 (0.49%) had an SAPA1 (average age 53.8±9.6 years, 9 women). The SAPA1 averaged 3.3 mm, all posteriorly oriented. Ten were ruptured (83.3%). Initial treatments included conventional coiling or balloon assisted coiling (CC/BAC) for nine aneurysms, and proximal A1 segment focal occlusion (PA1FO) for three. Initial occlusion was deemed satisfactory in all instances: total occlusion in eight cases (67%) and subtotal occlusion in four cases (33%). Four aneurysmal perforations occurred (33%), all during CC/BAC on ruptured aneurysms. Over a 10.2 year average follow-up, six recanalizations (50%) were noted, all after initial CC/BAC: three were early (≤14 days), with one causing fatal rebleeding. No recanalizations after PA1FO was observed (five in total, two as a complement after CC/BAC). Favorable clinical outcomes (modified Rankin Scale score of 0-2) were seen in 91% of cases (11/12) at the last follow-up. CONCLUSIONS: Selective coiling of the aneurysmal sac is technically difficult due to their small size and the complex microcatheterization pathway. This method presents a significant risk of aneurysmal perforation, especially in ruptured cases, and a high rate of recanalization. PA1FO, when collateralization permits, appears to be a reliable therapeutic alternative offering favorable long term outcomes.

7.
Molecules ; 29(12)2024 Jun 13.
Artículo en Inglés | MEDLINE | ID: mdl-38930893

RESUMEN

The growing demand for wearable and attachable displays has sparked significant interest in flexible quantum-dot light-emitting diodes (QLEDs). However, the challenges of fabricating and operating QLEDs on flexible substrates persist due to the lack of stable and low-temperature processable charge-injection/-transporting layers with aligned energy levels. In this study, we utilized NiOx nanoparticles that are compatible with flexible substrates as a hole-injection layer (HIL). To enhance the work function of the NiOx HIL, we introduced a self-assembled dipole modifier called 4-(trifluoromethyl)benzoic acid (4-CF3-BA) onto the surface of the NiOx nanoparticles. The incorporation of the dipole molecules through adsorption treatment has significantly changed the wettability and electronic characteristics of NiOx nanoparticles, resulting in the formation of NiO(OH) at the interface and a shift in vacuum level. The alteration of surface electronic states of the NiOx nanoparticles not only improves the carrier balance by reducing the hole injection barrier but also prevents exciton quenching by passivating defects in the film. Consequently, the NiOx-based red QLEDs with interfacial modification demonstrate a maximum current efficiency of 16.1 cd/A and a peak external quantum efficiency of 10.3%. This represents a nearly twofold efficiency enhancement compared to control devices. The mild fabrication requirements and low annealing temperatures suggest potential applications of dipole molecule-modified NiOx nanoparticles in flexible optoelectronic devices.

8.
Lancet Neurol ; 23(7): 700-711, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38876748

RESUMEN

BACKGROUND: Positive susceptibility vessel sign (SVS) in patients with acute ischaemic stroke has been associated with friable red blood cell-rich clots and more effective recanalisation using stent retrievers versus contact aspiration. We compared the safety and efficacy of stent retrievers plus contact aspiration (combined technique) versus contact aspiration alone as the first-line thrombectomy technique in patients with acute ischaemic anterior circulation stroke and SVS-positive occlusions. METHODS: Adaptive Endovascular Strategy to the Clot MRI in Large Intracranial Vessel Occlusion (VECTOR) was a prospective, randomised, open-label study with blinded evaluation. Patients with SVS-positive anterior circulation occlusions on pretreatment MRI and arterial puncture within 24 h of symptom onset were enrolled from 22 centres in France. A centralised web-based method was used by interventional neuroradiologists for dynamic randomisation by minimisation. Patients were randomly assigned 1:1 to the combined technique or contact aspiration alone. The primary outcome was expanded Thrombolysis in Cerebral Infarction (eTICI) grade 2c or 3 reperfusion after three or fewer passes on post-treatment angiogram, adjudicated by a blinded independent central imaging core laboratory. The intention-to-treat population was used to assess the primary and secondary outcomes. This trial is registered with ClinicalTrials.gov (NCT04139486) and is complete. FINDINGS: Between Nov 26, 2019, and Feb 14, 2022, 526 patients were enrolled, of whom 521 constituted the intention-to-treat population (combined technique, n=263; contact aspiration alone, n=258). The median age of participants was 74·9 years (IQR 64·4-83·3); 284 (55%) were female and 237 (45%) male. The primary outcome did not differ significantly between groups (152 [58%] of 263 patients for the combined technique vs 135 [52%] of 258 for contact aspiration; odds ratio [OR] 1·27; 95% CI 0·88-1·83; p=0·19). Procedure-related adverse events occurred in 32 (12%) of 263 patients in the combined technique group and 27 (11%) of 257 in the contact aspiration group (OR 1·14; 0·65-2·00; p=0·65). The most common adverse event was intracerebral haemorrhage (146 [56%] of 259 patients for the combined technique vs 123 [49%] of 251 for contact aspiration; OR 1·32; 0·91-1·90; p=0·13). All-cause mortality at 3 months occurred in 57 (23%) of 251 patients in the combined technique group and 48 (19%) of 247 in the contact aspiration group (OR 1·19; 0·76-1·86; p=0·45), none of which was treatment-related. INTERPRETATION: The results of the VECTOR trial do not show superiority of the combined stent retriever plus contact aspiration technique over contact aspiration alone in patients with SVS-positive occlusion with respect to achieving eTICI 2c-3 within three passes. These findings support the use of either the combined technique or contact aspiration alone as the initial thrombectomy strategy in patients with acute anterior circulation stroke with SVS on pretreatment MRI. FUNDING: Cerenovus.


Asunto(s)
Accidente Cerebrovascular Isquémico , Stents , Trombectomía , Humanos , Femenino , Masculino , Anciano , Francia , Método Simple Ciego , Accidente Cerebrovascular Isquémico/cirugía , Accidente Cerebrovascular Isquémico/terapia , Accidente Cerebrovascular Isquémico/diagnóstico por imagen , Trombectomía/métodos , Trombectomía/instrumentación , Persona de Mediana Edad , Anciano de 80 o más Años , Procedimientos Endovasculares/métodos , Procedimientos Endovasculares/instrumentación , Estudios Prospectivos , Resultado del Tratamiento , Succión/métodos
9.
Adv Mater ; 36(30): e2403076, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38733295

RESUMEN

The spotlight has shifted to near-infrared (NIR) luminescent materials emitting beyond 1000 nm, with growing interest due to their unique characteristics. The ability of NIR-II emission (1000-1700 nm) to penetrate deeply and transmit independently positions these NIR luminescent materials for applications in optical-communication devices, bioimaging, and photodetectors. The combination of rare earth metals/transition metals with a variety of matrix materials provides a new platform for creating new chemical and physical properties for materials science and device applications. In this review, the recent advancements in NIR emission activated by rare earth and transition metal ions are summarized and their role in applications spanning bioimaging, sensing, and optoelectronics is illustrated. It started with various synthesis techniques and explored how rare earths/transition metals can be skillfully incorporated into various matrixes, thereby endowing them with unique characteristics. The discussion to strategies of enhancing excitation absorption and emission efficiency, spotlighting innovations like dye sensitization and surface plasmon resonance effects is then extended. Subsequently, a significant focus is placed on functionalization strategies and their applications. Finally, a comprehensive analysis of the challenges and proposed strategies for rare earth/transition metal ion-doped near-infrared luminescent materials, summarizing the insights of each section is provided.

10.
Nature ; 629(8012): 586-591, 2024 May.
Artículo en Inglés | MEDLINE | ID: mdl-38720080

RESUMEN

Light-emitting diodes (LEDs) based on perovskite quantum dots (QDs) have produced external quantum efficiencies (EQEs) of more than 25% with narrowband emission1,2, but these LEDs have limited operating lifetimes. We posit that poor long-range ordering in perovskite QD films-variations in dot size, surface ligand density and dot-to-dot stacking-inhibits carrier injection, resulting in inferior operating stability because of the large bias required to produce emission in these LEDs. Here we report a chemical treatment to improve the long-range order of perovskite QD films: the diffraction intensity from the repeating QD units increases three-fold compared with that of controls. We achieve this using a synergistic dual-ligand approach: an iodide-rich agent (aniline hydroiodide) for anion exchange and a chemically reactive agent (bromotrimethylsilane) that produces a strong acid that in situ dissolves smaller QDs to regulate size and more effectively removes less conductive ligands to enable compact, uniform and defect-free films. These films exhibit high conductivity (4 × 10-4 S m-1), which is 2.5-fold higher than that of the control, and represents the highest conductivity recorded so far among perovskite QDs. The high conductivity ensures efficient charge transportation, enabling red perovskite QD-LEDs that generate a luminance of 1,000 cd m-2 at a record-low voltage of 2.8 V. The EQE at this luminance is more than 20%. Furthermore, the stability of the operating device is 100 times better than previous red perovskite LEDs at EQEs of more than 20%.

11.
Small ; : e2401701, 2024 May 05.
Artículo en Inglés | MEDLINE | ID: mdl-38705844

RESUMEN

Enhancing the intrinsic stability of perovskite and through encapsulation to isolate water, oxygen, and UV-induced decomposition are currently common and most effective strategies in perovskite solar cells. Here, the atomic layer deposition process is employed to deposit a nanoscale (≈100 nm), uniform, and dense Al2O3 film on the front side of perovskite devices, effectively isolating them from the erosion caused by water and oxygen in the humid air. Simultaneously, nanoscale (≈100 nm) TiO2 films are also deposited on the glass surface to efficiently filter out the ultraviolet (UV) light in the light source, which induces degradation in perovskite. Ultimately, throughthe collaborative effects of both aspects, the stability of the devices is significantly improved under conditions of humid air and illumination. As a result, after storing the devices in ambient air for 1000 h, the efficiency only declines to 95%, and even after 662 h of UV exposure, the efficiency remains at 88%, far surpassing the performance of comparison devices. These results strongly indicate that the adopted Al2O3 and TiO2 thin films play a significant role in enhancing the stability of perovskite solar cells, demonstrating substantial potential for widespread industrial applications.

12.
Int J Comput Assist Radiol Surg ; 19(9): 1667-1675, 2024 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-38632166

RESUMEN

PURPOSE: Intracranial aneurysm detection from 3D Time-Of-Flight Magnetic Resonance Angiography images is a problem of increasing clinical importance. Recently, a streak of methods have shown promising performance by using segmentation neural networks. However, these methods may be less relevant in a clinical settings where diagnostic decisions rely on detecting objects rather than their segmentation. METHODS: We introduce a 3D single-stage object detection method tailored for small object detection such as aneurysms. Our anchor-free method incorporates fast data annotation, adapted data sampling and generation to address class imbalance problem, and spherical representations for improved detection. RESULTS: A comprehensive evaluation was conducted, comparing our method with the state-of-the-art SCPM-Net, nnDetection and nnUNet baselines, using two datasets comprising 402 subjects. The evaluation used adapted object detection metrics. Our method exhibited comparable or superior performance, with an average precision of 78.96%, sensitivity of 86.78%, and 0.53 false positives per case. CONCLUSION: Our method significantly reduces the detection complexity compared to existing methods and highlights the advantages of object detection over segmentation-based approaches for aneurysm detection. It also holds potential for application to other small object detection problems.


Asunto(s)
Imagenología Tridimensional , Aneurisma Intracraneal , Angiografía por Resonancia Magnética , Aneurisma Intracraneal/diagnóstico por imagen , Aneurisma Intracraneal/diagnóstico , Humanos , Angiografía por Resonancia Magnética/métodos , Imagenología Tridimensional/métodos , Sensibilidad y Especificidad , Algoritmos , Interpretación de Imagen Asistida por Computador/métodos
13.
J Am Chem Soc ; 146(17): 11845-11854, 2024 May 01.
Artículo en Inglés | MEDLINE | ID: mdl-38648548

RESUMEN

Organic molecules have been regarded as ideal candidates for near-infrared (NIR) optoelectronic active materials due to their customizability and ease of large-scale production. However, constrained by the intricate molecular design and severe energy gap law, the realization of optoelectronic devices in the second near-infrared (NIR (II)) region with required narrow band gaps presents more challenges. Herein, we have originally proposed a cocrystal strategy that utilizes intermolecular charge-transfer interaction to drive the redshift of absorption and emission spectra of a series BFXTQ (X = 0, 1, 2, 4) cocrystals, resulting in the spectra located at NIR (II) window and reducing the optical bandgap to ∼0.98 eV. Significantly, these BFXTQ-based optoelectronic devices can exhibit dual-mode optoelectronic characteristics. An investigation of a series of BFXTQ-based photodetectors exhibits detectivity (D*) surpassing 1013 Jones at 375 to 1064 nm with a maximum of 1.76 × 1014 Jones at 1064 nm. Moreover, the radiative transition of CT excitons within the cocrystals triggers NIR emission over 1000 nm with a photoluminescence quantum yield (PLQY) of ∼4.6% as well as optical waveguide behavior with a low optical-loss coefficient of 0.0097 dB/µm at 950 nm. These results promote the advancement of an emerging cocrystal approach in micro/nanoscale NIR multifunctional optoelectronics.

14.
IEEE Trans Image Process ; 33: 2404-2418, 2024.
Artículo en Inglés | MEDLINE | ID: mdl-38517711

RESUMEN

Image Quality Assessment (IQA) is a fundamental task in computer vision that has witnessed remarkable progress with deep neural networks. Inspired by the characteristics of the human visual system, existing methods typically use a combination of global and local representations (i.e., multi-scale features) to achieve superior performance. However, most of them adopt simple linear fusion of multi-scale features, and neglect their possibly complex relationship and interaction. In contrast, humans typically first form a global impression to locate important regions and then focus on local details in those regions. We therefore propose a top-down approach that uses high-level semantics to guide the IQA network to focus on semantically important local distortion regions, named as TOPIQ. Our approach to IQA involves the design of a heuristic coarse-to-fine network (CFANet) that leverages multi-scale features and progressively propagates multi-level semantic information to low-level representations in a top-down manner. A key component of our approach is the proposed cross-scale attention mechanism, which calculates attention maps for lower level features guided by higher level features. This mechanism emphasizes active semantic regions for low-level distortions, thereby improving performance. TOPIQ can be used for both Full-Reference (FR) and No-Reference (NR) IQA. We use ResNet50 as its backbone and demonstrate that TOPIQ achieves better or competitive performance on most public FR and NR benchmarks compared with state-of-the-art methods based on vision transformers, while being much more efficient (with only  âˆ¼ 13% FLOPS of the current best FR method). Codes are released at https://github.com/chaofengc/IQA-PyTorch.

15.
Adv Mater ; 36(24): e2400421, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38430204

RESUMEN

Thanks to the extensive efforts toward optimizing perovskite crystallization properties, high-quality perovskite films with near-unity photoluminescence quantum yield are successfully achieved. However, the light outcoupling efficiency of perovskite light-emitting diodes (PeLEDs) is impeded by insufficient light extraction, which poses a challenge to the further advancement of PeLEDs. Here, an anisotropic multifunctional electron transporting material, 9,10-bis(4-(2-phenyl-1H-benzo[d]imidazole-1-yl)phenyl) anthracene (BPBiPA), with a low extraordinary refractive index (ne) and high electron mobility is developed for fabricating high-efficiency PeLEDs. The anisotropic molecular orientations of BPBiPA can result in a low ne of 1.59 along the z-axis direction. Optical simulations show that the low ne of BPBiPA can effectively mitigate the surface plasmon polariton loss and enhance the photon extraction efficiency in waveguide mode, thereby improving the light outcoupling efficiency of PeLEDs. In addition, the high electron mobility of BPBiPA can facilitate balanced carrier injection in PeLEDs. As a result, high-efficiency green PeLEDs with a record external quantum efficiency of 32.1% and a current efficiency of 111.7 cd A-1 are obtained, which provides new inspirations for the design of electron transporting materials for high-performance PeLEDs.

16.
Interv Neuroradiol ; : 15910199241236323, 2024 Feb 29.
Artículo en Inglés | MEDLINE | ID: mdl-38425221

RESUMEN

Stenting of the dural venous sinuses has emerged as a therapeutic option for intracranial hypertension and pulsatile tinnitus. However, venous endovascular navigation faces challenges due to lower-quality roadmaps compared to arterial navigation. This study explores the application of three-dimensional (3D) rotational venography in assessing the cerebral venous vasculature and its potential for venous navigation. The methods involve venous 3D digital subtracted angiography (DSA) in patients with dural venous stenosis, with image acquisition using a biplane angiographic system. The results highlight the enhanced spatial resolution of 3D venous imaging, providing anatomical information crucial for precise characterization of stenosis and understanding cortical venous drainage. 3D venous roadmapping is shown to improve endovascular venous navigation, offering synchronized and rotatable 3D roadmaps, providing a comprehensive approach to optimize endovascular venous interventions.

17.
Nat Commun ; 15(1): 1130, 2024 Feb 07.
Artículo en Inglés | MEDLINE | ID: mdl-38326331

RESUMEN

Organic heterostructures (OHTs) with the desired geometry organization on micro/nanoscale have undergone rapid progress in nanoscience and nanotechnology. However, it is a significant challenge to elucidate the epitaxial-growth process for various OHTs composed of organic units with a lattice mismatching ratio of > 3%, which is unimaginable for inorganic heterostructures. Herein, we have demonstrated a vivid visualization of the morphology evolution of epitaxial-growth based on a doped interfacial-layer, which facilitates the comprehensive understanding of the hierarchical self-assembly of core-shell OHT with precise spatial configuration. Significantly, the barcoded OHT with periodic shells obviously illustrate the shell epitaxial-growth from tips to center parts along the seeded rods for forming the core-shell OHT. Furthermore, the diameter, length, and number of periodic shells were modulated by finely tuning the stoichiometric ratio, crystalline time, and temperature, respectively. This epitaxial-growth process could be generalized to organic systems with facile chemical/structural compatibility for forming the desired OHTs.

18.
Nano Lett ; 24(9): 2765-2772, 2024 Mar 06.
Artículo en Inglés | MEDLINE | ID: mdl-38393855

RESUMEN

Alloying lanthanide ions (Yb3+) into perovskite quantum dots (Yb3+:CsPb(Cl1-xBrx)3) is an effective method to achieve efficient near-infrared (NIR) luminescence (>950 nm). Increasing the Yb3+ alloying ratio in the perovskite matrix enhances the luminescence intensity of Yb3+ emission at 990 nm. However, high Yb3+ alloying (>15%) results in vacancy-induced inferior material stability. In this work, we developed a polarity-mediated antisolvent manipulation strategy to resolve the incompatibility between a high Yb3+ alloying ratio and inferior stability of Yb3+:CsPb(Cl1-xBrx)3. Precise control of solution polarity enables increased uniformity of the perovskite matrix with fewer trap densities. Employing this strategy, we obtain Yb3+:CsPb(Cl1-xBrx)3 with the highest Yb3+ alloying ratio of 30.2% and a 2-fold higher electroluminescence intensity at 990 nm. We lever the engineered Yb3+:CsPb(Cl1-xBrx)3 to fabricate NIR-LEDs, achieving a peak external quantum efficiency (EQE) of 8.5% at 990 nm: this represents the highest among perovskite NIR-LEDs with an emission wavelength above 950 nm.

19.
ACS Nano ; 18(8): 6513-6522, 2024 Feb 27.
Artículo en Inglés | MEDLINE | ID: mdl-38345358

RESUMEN

The performance of blue perovskite light-emitting diodes (PeLEDs) lags behind the green and red counterparts owing to high trap density and undesirable red shift of the electroluminescence spectrum under operation conditions. Organic molecular additives were employed as passivators in previous reports. However, most commonly have limited functions, making it challenging to effectively address both efficiency and stability issues simultaneously. Herein, we reported an innovatively dynamic in situ hydrolysis strategy to modulate quasi-2D sky-blue perovskites by the multifunctional passivator phenyl dichlorophosphate that not only passivated the defects but also underwent in situ hydrolysis reaction to stabilize the emission. Moreover, hydrolysis products were beneficial for low-dimensional phase manipulation. Eventually, we obtained high-performance sky-blue PeLEDs with a maximum external quantum efficiency (EQE) of 16.32% and an exceptional luminance of 5740 cd m-2. More importantly, the emission peak of devices located at 485 nm remained stable under different biases. Our work signified the significant advancement toward realizing future applications of PeLEDs.

20.
ACS Appl Mater Interfaces ; 16(3): 3809-3818, 2024 Jan 24.
Artículo en Inglés | MEDLINE | ID: mdl-38211320

RESUMEN

Narrowband blue emitters are indispensable in achieving ultrahigh-definition OLED displays that satisfy the stringent BT 2020 standard. Hereby, a series of bis-tridentate Ir(III) complexes bearing electron-deficient imidazo[4,5-b]pyridin-2-ylidene carbene coordination fragments and 2,6-diaryloxy pyridine ancillary groups were designed and synthesized. They exhibited deep blue emission with quantum yields of up to 89% and a radiative lifetime of 0.71 µs in the DPEPO host matrix, indicating both the high efficiency and excellent energy transfer process from the host to dopant. The OLED based on Irtb1 showed an emission at 468 nm with a maximum external quantum efficiency (EQE) of 22.7%. Moreover, the hyper-OLED with Irtb1 as a sensitizer for transferring energy to terminal emitter v-DABNA exhibited a narrowband blue emission at 472 nm and full width at half-maximum (FWHM) of 24 nm, a maximum EQE of 23.5%, and EQEs of 19.7, 16.1, and 12.9% at a practical brightness of 100, 1000, and 5000 cd/m2, respectively.

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