Compared to efficient green and near‐infrared light‐emitting diodes (LEDs), less progress has been made on deep‐blue perovskite LEDs. They suffer from inefficient domain various number of PbX6− ...layers (n) control, resulting in a series of unfavorable issues such as unstable color, multipeak profile, and poor fluorescence yield. Here, a strategy involving a delicate spacer modulation for quasi‐2D perovskite films via an introduction of aromatic polyamine molecules into the perovskite precursor is reported. With low‐dimensional component engineering, the n1 domain, which shows nonradiative recombination and retarded exciton transfer, is significantly suppressed. Also, the n3 domain, which represents the population of emission species, is remarkably increased. The optimized quasi‐2D perovskite film presents blue emission from the n3 domain (peak at 465 nm) with a photoluminescence quantum yield (PLQY) as high as 77%. It enables the corresponding perovskite LEDs to deliver stable deep‐blue emission (CIE (0.145, 0.05)) with an external quantum efficiency (EQE) of 2.6%. The findings in this work provide further understanding on the structural and emission properties of quasi‐2D perovskites, which pave a new route to design deep‐blue‐emissive perovskite materials.
A quasi‐two‐dimensional perovskite film with stable domain distribution is prepared based on a new spacer. The film containing pure bromide perovskite exhibits enhanced deep‐blue fluorescence with quantum yield of 77% by low‐dimensional component engineering. As a result, the corresponding light‐emitting diodes deliver stable deep‐blue emission with a peak external quantum efficiency of 2.6%.
Multi‐layer π‐stacked emitters based on spatially confined donor/acceptor/donor (D/A/D) patterns have been developed to achieve high‐efficiency thermally activated delayed fluorescence (TADF). In ...this case, dual donor moieties and a single acceptor moiety are introduced to form two three‐dimensional (3D) emitters, DM‐BD1 and DM‐BD2, which rely on spatial charge transfer (CT). Owing to the enforced face‐to‐face D/A/D pattern, effective CT interactions are realized, which lead to high photoluminescence quantum yields (PLQYs) of 94.2 % and 92.8 % for the two molecules, respectively. The resulting emitters exhibit small singlet–triplet energy splitting (ΔEST) and fast reverse intersystem crossing (RISC) processes. Maximum external quantum efficiencies (EQEs) of 28.0 % and 26.6 % were realized for devices based on DM‐BD1 and DM‐BD2, respectively, which are higher than those of their D/A‐type analogues.
Multi‐Layer π‐stacked molecules are designed to realize efficient thermally activated delayed fluorescence. Spatially confined molecules with stereochemical structures are constructed in donor/acceptor/donor architectures with different conformations. Their organic light‐emitting diode (OLED) devices exhibit high external quantum efficiencies (EQEs) of 28.0 %/26.6 %, respectively.
High-dimensional data analysis is a challenge for researchers and engineers in the fields of machine learning and data mining. Feature selection provides an effective way to solve this problem by ...removing irrelevant and redundant data, which can reduce computation time, improve learning accuracy, and facilitate a better understanding for the learning model or data. In this study, we discuss several frequently-used evaluation measures for feature selection, and then survey supervised, unsupervised, and semi-supervised feature selection methods, which are widely applied in machine learning problems, such as classification and clustering. Lastly, future challenges about feature selection are discussed.
Near‐infrared (NIR) organic solid‐state lasers play an essential role in applications ranging from laser communication to infrared night vision, but progress in this area is restricted by the lack of ...effective excited‐state gain processes. Herein, we originally proposed and demonstrated the cascaded occurrence of excited‐state intramolecular proton transfer for constructing the completely new energy‐level systems. Cascading by the first ultrafast proton transfer of <430 fs and the subsequent irreversible second proton transfer of ca. 1.6 ps, the stepwise proton transfer process favors the true six‐level photophysical cycle, which supports efficient population inversion and thus NIR single‐mode lasing at 854 nm. This work realizes longest wavelength beyond 850 nm of organic single‐crystal lasing to date and originally exploits the cascaded excited‐state molecular proton transfer energy‐level systems for organic solid‐state lasers.
Six‐level energy systems are constructed through the cascaded occurrence of excited‐state intramolecular proton transfer consisting of a first ultrafast proton transfer of <430 fs and a following dominant and irreversible proton transfer of ca. 1.6 ps, which support the NIR single‐mode lasing at 854 nm for exploiting energy‐level systems of OSSLs, especially at the NIR region from 780 to 2500 nm.
•The novel ultrathin hydrated V2O5·4VO2·2.72H2O nanobelts was obtained through a hydrothermal method.•The existence of crystal water can effectively improve performance.•V2O5·4VO2·2.72H2O delivers ...excellent cycling stability and the specific discharge capacity.•The high reversibility of Zn2+ insertion/extraction in V2O5·4VO2·2.72H2O was demonstrated by in-situ XRD.
Although rechargeable aqueous zinc-ion batteries (AZIBs) are emerging candidates for high energy density, safety and cost effectiveness large-scale energy storage, they still lack suitable cathodes with high rate capabilities. In the present work, ultrathin V2O5·4VO2·2.72H2O nanobelts were synthesized via a facile hydrothermal method as cathode materials for ZIBs. Benefiting from expanded interlayer spacing that results from crystal water, the V2O5·4VO2·2.72H2O cathode exhibits an improved capacity of 567 mAh·g−1 at 0.1 A·g−1 and superior rate capability of 10.0 A·g−1 with a decent capacity of 215 mAh·g−1. When at 10.0 A g−1, a capacity retention of 94.0% with respect to the initial specific capacity was retained after 1000 cycles, and 85.2% was obtained even after 2000 cycles. Furthermore, in-situ X-ray diffraction and various structural measurements proved the high reversibility of Zn2+ insertion and extraction in V2O5·4VO2·2.72H2O cathode. Further investigations show that ultrathin V2O5·4VO2·2.72H2O nanobelts have become a promising cathode material for the high-potential rechargeable AZIBs, and may clarify effective interlayer engineering strategies triggered by crystal water.
The plant immune system is fundamental for plant survival in natural ecosystems and for productivity in crop fields. Substantial evidence supports the prevailing notion that plants possess a ...two-tiered innate immune system, called pattern-triggered immunity (PTI) and effector-triggered immunity (ETI). PTI is triggered by microbial patterns via cell surface-localized pattern-recognition receptors (PRRs), whereas ETI is activated by pathogen effector proteins via predominantly intracellularly localized receptors called nucleotide-binding, leucine-rich repeat receptors (NLRs)
. PTI and ETI are initiated by distinct activation mechanisms and involve different early signalling cascades
. Here we show that Arabidopsis PRR and PRR co-receptor mutants-fls2 efr cerk1 and bak1 bkk1 cerk1 triple mutants-are markedly impaired in ETI responses when challenged with incompatible Pseudomonas syrinage bacteria. We further show that the production of reactive oxygen species by the NADPH oxidase RBOHD is a critical early signalling event connecting PRR- and NLR-mediated immunity, and that the receptor-like cytoplasmic kinase BIK1 is necessary for full activation of RBOHD, gene expression and bacterial resistance during ETI. Moreover, NLR signalling rapidly augments the transcript and/or protein levels of key PTI components. Our study supports a revised model in which potentiation of PTI is an indispensable component of ETI during bacterial infection. This revised model conceptually unites two major immune signalling cascades in plants and mechanistically explains some of the long-observed similarities in downstream defence outputs between PTI and ETI.
Rational manipulation of frontier orbital distribution and singlet‐triplet splitting is crucial to exploit the luminescent properties of organic molecules. To realize ultra‐blue luminescence, both ...blue‐shifted wavelength peak (λpeak) and narrow full‐width at half‐maximum (FWHM) are required. Herein, a new thermally activated delayed fluorescence (TADF) skeleton by inserting the diphenyl methylene intramolecular‐lock to adjust the torsion angles and restrict the intramolecular relaxation is developed. Two rigid emitters, incorporating phenoxazine (PXZN‐B) and acridine (DMACN‐B) as donors and mesitylboron as an acceptor, exhibit narrow FWHMs (<50 nm) with deep‐blue (0.133, 0.147) and violet‐blue emission (0.151, 0.045), respectively. In particular, the Commission Internationale de l'Eclairage (CIE) coordinates of a DMACN‐B‐based device closely approach the Rec.2020 standard (0.131, 0.046). Moreover, both of the organic light‐emitting diodes (OLEDs) based on PXZN‐B and DMACN‐B show TADF character, with high external quantum efficiencies (EQEs) exceeding 10%. Furthermore, owing to the large orbital overlap, these TADF emitters own a fast S1–S0 transition rate exceeding 108 s–1, thereby exhibiting marked amplified spontaneous emission (ASE) with low thresholds. Therefore, the intramolecular‐lock strategy provides not only innovation for realizing high‐efficiency deep‐blue TADF emission with high color purity but also an avenue for a TADF‐based ASE and lasing application.
An “intramolecular‐lock” is proposed as part of the thermally activated delayed fluorescence (TADF) molecular design for manipulating torsion angles and wave function distributions. The quasi‐planar TADF emitters lead to ultrapure violet‐blue TADF electroluminescence with CIE‐(0.151, 0.045), approaching the Rec. 2020 standard. Furthermore, a TADF‐based amplified spontaneous emission with low thresholds is triggered, which paves the way for future TADF‐based lasing application.
The aboveground parts of terrestrial plants, collectively called the phyllosphere, have a key role in the global balance of atmospheric carbon dioxide and oxygen. The phyllosphere represents one of ...the most abundant habitats for microbiota colonization. Whether and how plants control phyllosphere microbiota to ensure plant health is not well understood. Here we show that the Arabidopsis quadruple mutant (min7 fls2 efr cerk1; hereafter, mfec)
, simultaneously defective in pattern-triggered immunity and the MIN7 vesicle-trafficking pathway, or a constitutively activated cell death1 (cad1) mutant, carrying a S205F mutation in a membrane-attack-complex/perforin (MACPF)-domain protein, harbour altered endophytic phyllosphere microbiota and display leaf-tissue damage associated with dysbiosis. The Shannon diversity index and the relative abundance of Firmicutes were markedly reduced, whereas Proteobacteria were enriched in the mfec and cad1
mutants, bearing cross-kingdom resemblance to some aspects of the dysbiosis that occurs in human inflammatory bowel disease. Bacterial community transplantation experiments demonstrated a causal role of a properly assembled leaf bacterial community in phyllosphere health. Pattern-triggered immune signalling, MIN7 and CAD1 are found in major land plant lineages and are probably key components of a genetic network through which terrestrial plants control the level and nurture the diversity of endophytic phyllosphere microbiota for survival and health in a microorganism-rich environment.
This work describes a strategy to produce circularly polarized thermally activated delayed fluorescence (CP-TADF). A set of two structurally similar organic emitters SFST and SFOT are constructed, ...whose spiro architectures containing asymmetric donors result in chirality. Upon grafting within the spiro frameworks, the donor and acceptor are fixed proximally in a face-to-face manner. This orientation allows intramolecular through-space charge transfer (TSCT) to occur in both emitters, leading to TADF properties. The donor units in SFST and SFOT have a sulfur and oxygen atom, respectively; such a subtle difference has great impacts on their photophysical, chiroptical, and electroluminescence (EL) properties. SFOT exhibits greatly enhanced EL performance in doped organic light-emitting diodes, with external quantum efficiency (EQE) up to 23.1%, owing to the concurrent manipulation of highly photoluminescent quantum efficiency (PLQY, ∼90%) and high exciton utilization. As a comparison, the relatively larger sulfur atom in SFST introduces heavy atom effects and leads to distortion of the molecular backbone that lengthens the donor–acceptor distance. SFST thus has lower PLQY and faster nonradiative decay rate. The collective consequence is that the EQE value of SFST, i.e., 12.5%, is much lower than that of SFOT. The chirality of these two spiro emitters results in circularly polarized luminescence. Because SFST has a more distorted molecular architecture than SFOT, the luminescence dissymmetry factor (|g lum|) of circularly polarized luminescence of one enantiomer of the former, namely, either (S)-SFST or (R)-SFST, is almost twice that of (S)-SFOT/(R)-SFOT. Moreover, the CP organic light-emitting diodes (CP-OLEDs) show obvious circularly polarized electroluminescence (CPEL) signals with g EL of 1.30 × 10–3 and 1.0 × 10–3 for (S)-SFST and (S)-SFOT, respectively.
Organic materials with multi‐stimulus response (MSR) properties have demonstrated many potential and practical applications. Herein, a π‐stacked thermally activated delayed fluorescence (TADF) ...material with multi‐stimulus response (MSR) properties, named SDMAC, was designed and synthesized using distorted 9,9‐dimethyl‐10‐phenyl‐9,10‐dihydroacridine as a donor. SDMAC possesses a rigid π‐stacked configuration with intramolecular through‐space interactions and exhibits aggregation‐induced emission enhancement (AIEE), solvatochromic, piezochromic, and circularly polarized luminescence (CPL) under different external stimuli. The rigid molecular structure and efficient TADF properties of SDMAC can be used in displays and lighting. Using SDMAC as an emitter, the maximum external quantum efficiency (EQE) of the fabricated organic light‐emitting diodes (OLEDs) is as high as 28.4 %, which make them the most efficient CP‐TADF OLEDs based on the through‐space charge transfer strategy. The CP organic light‐emitting diodes (CP‐OLEDs) exhibit circularly polarized electroluminescence (CPEL) signals.
An efficient thermally activated delayed fluorescence (TADF) emitter has been developed that possesses a rigid π‐stacked configuration with intramolecular through‐space interactions. This emitter exhibits solvatochromism, piezochromism, aggregation‐induced emission enhancement (AIEE), and circularly polarized luminescence (CPL) under different external stimuli.
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