Fluorinated ketones are widely prevalent in numerous biologically interesting molecules, and the development of novel transformations to access these structures is an important task in organic ...synthesis. Herein, we report the multicomponent radical acylfluoroalkylation of a variety of olefins in the presence of various commercially available aromatic aldehydes and fluoroalkyl reagents through N‐heterocyclic carbene organocatalysis. With this protocol, over 120 examples of functionalized ketones with diverse fluorine substituents have been synthesized in up to 99 % yield with complete regioselectivity. The generality of this catalytic strategy was further highlighted by its successful application in the late‐stage functionalization of pharmaceutical skeletons. Excellent diastereoselectivity could be achieved in the reactions forging multiple stereocenters. In addition, preliminary results have been achieved on the catalytic asymmetric variant of the olefin difunctionalization process.
Organocatalytic acylfluoroalkylation: A multicomponent radical acylfluoroalkylation of olefins through NHC organocatalysis was developed, and over 120 examples of fluoroketones were facilely accessed from simple materials. Moreover, a dearomative difunctionalization of indoles could be readily achieved in a highly diastereoselective manner. The generality and practicality were highlighted by the late‐stage modification of drug skeletons.
Organic photodetectors (OPDs) have attracted continuous attention due to their outstanding advantages, such as tunability of detecting wavelength, low‐cost manufacturing, compatibility with ...lightweight and flexible devices, as well as ease of processing. Enormous efforts on performance improvement and application of OPDs have been devoted in the past decades. In this Review, recent advances in device architectures and operation mechanisms of phototransistor, photoconductor, and photodiode based OPDs are reviewed with a focus on the strategies aiming at performance improvement. The application of OPDs in spectrally selective detection, wearable devices, and integrated optoelectronics are also discussed. Furthermore, some future prospects on the research challenges and new opportunities of OPDs are covered.
Recent progress in organic photodetectors is reviewed, including different device structures, features, and operation mechanisms. Benefiting from the improved performance, the applications of organic photodetectors for selective detection, wearability, and integrated devices are highlighted.
Perovskite light‐emitting diodes (PeLEDs) show great application potential in high‐quality flat‐panel displays and solid‐state lighting due to their steadily improved efficiency, tunable colors, ...narrow emission peak, and easy solution‐processing capability. However, because of high optical confinement and nonradiative charge recombination during electron–photon conversion, the highest reported efficiency of PeLEDs remains far behind that of their conventional counterparts, such as inorganic LEDs, organic LEDs, and quantum‐dot LEDs. Here a facile route is demonstrated by adopting bioinspired moth‐eye nanostructures at the front electrode/perovskite interface to enhance the outcoupling efficiency of waveguided light in PeLEDs. As a result, the maximum external quantum efficiency and current efficiency of the modified cesium lead bromide (CsPbBr3) green‐emitting PeLEDs are improved to 20.3% and 61.9 cd A−1, while retaining spectral and angular independence. Further reducing light loss in the substrate mode using a half‐ball lens, efficiencies of 28.2% and 88.7 cd A−1 are achieved, which represent the highest values reported to date for PeLEDs. These results represent a substantial step toward achieving practical applications of PeLEDs.
Highly efficient perovskite light‐emitting diodes are achieved by implementing a simple and cost‐effective method for efficient outcoupling of waveguided light. A record external quantum efficiency of 28.2% is realized for the device based on cesium lead bromide (CsPbBr3), while retaining the same spectral response for broad viewing angles.
The direct functionalization of inert C(sp3)−H bonds under environmentally benign catalytic conditions remains a challenging task in synthetic chemistry. Here, we report an organocatalytic remote ...C(sp3)−H acylation of amides and cascade cyclization through a radical‐mediated 1,5‐hydrogen atom transfer mechanism using N‐heterocyclic carbene as the catalyst. Notably, a diversity of nitrogen‐containing substrates, including simple linear aliphatic carbamates and ortho‐alkyl benzamides, can be successfully applied to this organocatalytic system. With the established protocol, over 120 examples of functionalized δ‐amino ketones and isoquinolinones with diverse substituents were easily synthesized in up to 99 % yield under mild conditions. The robustness and generality of the organocatalytic strategy were further highlighted by the successful acylation of unactivated C(sp3)−H bonds and late‐stage modification of pharmaceutical molecules. Then, the asymmetric control of the radical reaction was attempted and proven feasible by using a newly designed chiral thiazolium catalyst, and moderate enantioselectivity was obtained at the current stage. Preliminary mechanistic investigations including several control reactions, KIE experiments, and computational studies shed light on the organocatalytic radical reaction mechanism.
An N‐heterocyclic carbene catalyzed remote C(sp3)−H acylation of amides was developed, and also combined with a cascade cyclization. Over 120 functionalized δ‐amino ketones and isoquinolinones with diverse substituents were synthesized in up to 99 % yield under mild conditions. Preliminary mechanistic investigations shed light on the organocatalytic radical reaction mechanism.
Mesogenic soft materials, having single or multiple mesogen moieties per molecule, commonly exhibit typical self‐organization characteristics, which promotes the formation of elegant helical ...superstructures or supramolecular assemblies in chiral environments. Such helical superstructures play key roles in the propagation of circularly polarized light and display optical properties with prominent handedness, that is, chiro‐optical properties. The leveraging of light to program the chiro‐optical properties of such mesogenic helical soft materials by homogeneously dispersing photosensitive chiral material into an achiral soft system or covalently connecting photochromic moieties to the molecules has attracted considerable attention in terms of materials, properties, and potential applications and has been a thriving topic in both fundamental science and application engineering. State‐of‐the‐art technologies are described in terms of the material design, synthesis, properties, and modulation of photoprogrammable chiro‐optical mesogenic soft helical architectures. Additionally, the scientific issues and technical problems that hinder further development of these materials for use in various fields are outlined and discussed. Such photoprogrammable mesogenic soft helical materials are competitive candidates for use in stimulus‐controllable chiro‐optical devices with high optical efficiency, stable optical properties, and easy miniaturization, facilitating the future integration and systemization of chiro‐optical chips in photonics, photochemistry, biomedical engineering, chemical engineering, and beyond.
Photoprogrammable mesogenic helical soft materials with both photosensitive and mesogenic moieties in molecules possess typical chiro‐optical properties, showing handedness dependency on the transmission, reflection, and absorption of an incident circularly polarized light (photonic bandgap and circular dichroism). This can be modulated readily by light irradiation, thus paving the way toward future chiro‐optical devices and systems.
Efficient and stable blue emission of perovskite light‐emitting diodes (PeLEDs) is a requisite toward their potential applications in full‐color displays and solid‐state lighting. Rational ...manipulation over the entire electroluminescence process is promising to break the efficiency limit of blue PeLEDs. Herein, a facile device architecture is proposed to achieve efficient blue PeLEDs for simultaneously reducing the energetic loss during electron‐photon conversion and boosting the light outcoupling. Effective interfacial engineering is employed to manipulate the perovskite crystallization nucleation, enabling highly compact perovskite nanocrystal assemblies and suppressing the trap‐induced carrier losses by means of interfacial hydrogen bonding interactions. This strategy contributes to a high external quantum efficiency (EQE) of 12.8% for blue PeLEDs emitting at 486 nm as well as improved operational stability. Moreover, blue PeLEDs reach a peak EQE of 16.8% with the incorporation of internal outcoupling structures for waveguided light, which can be further raised to 27.5% by integrating a lens‐based structure for substrate‐mode light. These results verify the validity of this strategy in producing efficient and stable blue PeLEDs for practical applications.
Synergistic manipulation of the whole electroluminescence process in blue perovskite light‐emitting diodes has been proposed with an interfacial nucleation seeding scheme. Efficient and stable blue devices achieve a maximum external quantum efficiency of 27.5% and improved electroluminescent stability during operation.
A single‐junction polymer solar cell with an efficiency of 10.1% is demonstrated by using deterministic aperiodic nanostructures for broadband light harvesting with optimum charge extraction. The ...performance enhancement is ascribed to the self‐enhanced absorption due to collective effects, including pattern‐induced anti‐reflection and light scattering, as well as surface plasmonic resonance, together with a minimized recombination probability.
Background and Aim
Lugol chromoendoscopy is the standard technique to detect an esophageal squamous cell carcinoma (ESCC). However, a high concentration of Lugol's solution can induce mucosal injury ...and adverse events. We aimed to investigate the optimal concentration of Lugol's solution to reduce mucosal injury and adverse events without degrading image quality.
Methods
This was a two‐phase double‐blind randomized controlled trial. In phase I, 200 eligible patients underwent esophagogastroduodenoscopy and then were randomly (1:1:1:1:1) sprayed with 1.2%, 1.0%, 0.8%, 0.6%, or 0.4% Lugol's solution. Image quality, gastric mucosal injury, adverse events, and operation satisfaction were compared to investigate the minimal effective concentration. In phase II, 42 cases of endoscopic mucosectomy for early ESCC were included. The patients were randomly assigned (1:1) to the minimal effective (0.6%) or conventional (1.2%) concentration of Lugol's solution for further comparison of the effectiveness.
Results
In phase I, the gastric mucosal injury was significantly reduced in 0.6% group (P < 0.05). Furthermore, there was no statistical significance in image quality between 0.6% and higher concentrations of Lugol's solution (P > 0.05, respectively). It also showed that the operation satisfaction decreased in 1.2% group compared with the lower concentration groups (P < 0.05). In phase II, the complete resection rate was 100% in both groups, while 0.6% Lugol's solution showed higher operation satisfaction (W = 554.500, P = 0.005).
Conclusions
The study indicates that 0.6% might be the optimal concentration of Lugol's solution for early detection and delineation of ESCC, considering minimal mucosal injury and satisfied image. The registry of clinical trials: ClinicalTrials.gov (NCT03180944).
A tandem organic light‐emitting diode (OLED) is an organic optoelectronic device that has two or more electroluminescence (EL) units connected electrically in series with unique intermediate ...connectors within the device. Researchers have studied this new OLED architecture with growing interest and have found that the current efficiency of a tandem OLED containing N EL units (N > 1) should be N times that of a conventional OLED containing only a single EL unit. Therefore, this new architecture is potentially useful for constructing high‐efficiency, high‐luminance, and long‐lifetime OLED displays and organic solid‐state lighting sources. In a tandem OLED, the intermediate connector plays a crucial role in determining the effectiveness of the stacked EL units. The interfaces in the connector control the inner charge generation and charge injection into the adjacent EL units. Meanwhile, the transparency and the thickness of the connector affect the light output of the device. Therefore, the intermediate connector should be made to meet both the electrical and optical requirements for achieving optimal performance. Here, recent advances in the research of the tandem OLEDs is discussed, with the main focus on material selection and interface studies in the intermediate connectors, as well as the optical design of the tandem OLEDs.
Recent advances of tandem organic light‐emitting diodes (OLEDs) including the material selection, interface engineering, and optical design of numerous intermediate connectors are reviewed. Their interfaces are crucial in determining the driving voltage, efficiencies, and lifetime. The optical transparency, microcavity, light out‐coupling, and voltage drop across the intermediate connectors have to be carefully considered for high‐performance tandem OLEDs.
Perovskite light‐emitting diodes (PeLEDs) are emerging candidates for the applications of solution‐processed full‐color displays. However, the device performance of deep‐blue PeLED still lags far ...behind that of their red and green counterparts, which is largely limited by low external quantum efficiency (EQE) and poor operational stability. Here, a facile and reliable crystallization strategy for perovskite grains is proposed, with improved deep‐blue emission through rational interfacial engineering. By modifying the substrate with potassium cation (K+) as the supplier of heterogeneous nucleation seeds, the interfacial K+‐guided grain growth is realized for well‐packed perovskite assemblies with high surface coverage and the controlled crystal orientation, leading to the enhanced radiative recombination and hole‐transport capabilities. Synergistical boost in device performance is achieved for deep‐blue PeLEDs emitting at 469 nm with a peak EQE of 4.14%, a maximum luminance of 451 cd m–2, and spectrally stable color coordinates of (0.125, 0.076) that matches well with the National Television System Committee (NTSC) standard blue.
A rational interface engineering strategy is presented for the potassium‐guided grain growth of deep‐blue perovskites with controlled crystal orientation. Efficient and stable perovskite LEDs emitting at 469 nm exhibit an external quantum efficiency of 4.14% and a Commission Internationale de l'Eclairage coordinate of (0.125, 0.076), matching well the National Television System Committee (NTSC) standard blue.
PDF
