In this work, two novel thermally activated delayed fluorescence (TADF) emitters, 2tDMG and 3tDMG, are synthesized for high‐efficiency organic light‐emitting diodes (OLEDs), The two emitters have a ...tilted face‐to‐face alignment of donor (D)/acceptor (A) units presenting intramolecular noncovalent interactions. The two TADF materials are deposited either by an evaporation‐process or by a solution‐process, both of them leading to high OLED performance. 2tDMG used as the emitter in evaporation‐processed OLEDs achieves a high external quantum efficiency (EQE) of 30.8% with a very flat efficiency roll‐off of 7% at 1000 cd m−2. The solution‐processed OLEDs also display an interesting EQE of 16.2%. 3tDMG shows improved solubility and solution processability as compared to 2tDMG, and thus a high EQE of 20.2% in solution‐processed OLEDs is recorded. The corresponding evaporation‐processed OLEDs also reach a reasonably high EQE of 26.3%. Encouragingly, this work provides a novel strategy to address the imperious demands for OLEDs with high EQE and low roll‐off.
A thermally activated delayed fluorescence emitter, 2tDMG, is designed and synthesized based on the donor (D)/acceptor (A) spatially intramolecular noncovalent interaction. The D/A units are connected via a rigid linker, thereby confining them into a close‐packed coplanar configuration for small singlet–triplet splitting energy. 2tDMG achieves a high external quantum efficiency of 30.8% with a low efficiency roll‐off in evaporation‐processed organic light‐emitting diodes (OLEDs).
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Derivatives based on anthryleno1,2‐bpyrazine‐2,3‐dicarbonitrile (DCPA) are used as luminescent materials, to realize near‐infrared (NIR) electroluminescence. By functionalizing DCPA with aromatic ...amine donors, two emitters named DCPA‐TPA and DCPA‐BBPA are designed and synthesized. Both molecules have large dipole moments owing to the strong intramolecular charge transfer interactions between the amine donors and the DCPA acceptor. Thus, compared with doped films, the emission of neat films of DCPA‐TPA and DCPA‐BBPA can fully fall into the NIR region (>700 nm) with increasing surrounding polarity by increasing doping ratio. Moreover, the non‐doped devices based on DCPA‐TPA and DCPA‐BBPA provide NIR emission with peaks at 838 and 916 nm, respectively. A maximum radiance of 20707 mW Sr−1 m−2 was realized for the further optimized device based on DCPA‐TPA. This work provides a simple and efficient strategy of molecular design for developing NIR emitting materials.
Highly luminescent anthracene is incorporated in designing near‐infrared (NIR) molecules. Flanked with donor and acceptor units, the emitters, named DCPA‐TPA and DCPA‐BBPA with strong dipole moment, were constructed to realize NIR electroluminescence. Their non‐doped devices can achieve high radiance and efficiency with nearly all the emission in the NIR region (>700 nm).
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
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.
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IJS, KILJ, NUK, PNG, UL, UM
Cleavage of transfer (t)RNA and ribosomal (r)RNA are critical and conserved steps of translational control for cells to overcome varied environmental stresses. However, enzymes that are responsible ...for this event have not been fully identified in high eukaryotes. Here, we report a mammalian tRNA/rRNA-targeting endoribonuclease: SLFN13, a member of the Schlafen family. Structural study reveals a unique pseudo-dimeric U-pillow-shaped architecture of the SLFN13 N'-domain that may clamp base-paired RNAs. SLFN13 is able to digest tRNAs and rRNAs in vitro, and the endonucleolytic cleavage dissevers 11 nucleotides from the 3'-terminus of tRNA at the acceptor stem. The cytoplasmically localised SLFN13 inhibits protein synthesis in 293T cells. Moreover, SLFN13 restricts HIV replication in a nucleolytic activity-dependent manner. According to these observations, we term SLFN13 RNase S13. Our study provides insights into the modulation of translational machinery in high eukaryotes, and sheds light on the functional mechanisms of the Schlafen family.
Hydrogen evolution reaction (HER) is more sluggish in alkaline than in acidic media because of the additional energy required for water dissociation. Numerous catalysts, including NiO, that offer ...active sites for water dissociation have been extensively investigated. Yet, the overall HER performance of NiO is still limited by lacking favorable H adsorption sites. Here we show a strategy to activate NiO through carbon doping, which creates under-coordinated Ni sites favorable for H adsorption. DFT calculations reveal that carbon dopant decreases the energy barrier of Heyrovsky step from 1.17 eV to 0.81 eV, suggesting the carbon also serves as a hot-spot for the dissociation of water molecules in water-alkali HER. As a result, the carbon doped NiO catalyst achieves an ultralow overpotential of 27 mV at 10 mA cm
, and a low Tafel slope of 36 mV dec
, representing the best performance among the state-of-the-art NiO catalysts.
This meta-analysis examined roles of several metabolites in differentiating recurrent tumor from necrosis in patients with brain tumors using MR perfusion and spectroscopy.
Medline, Cochrane, EMBASE, ...and Google Scholar were searched for studies using perfusion MRI and/or MR spectroscopy published up to March 4, 2015 which differentiated between recurrent tumor vs. necrosis in patients with primary brain tumors or brain metastasis. Only two-armed, prospective or retrospective studies were included. A meta-analysis was performed on the difference in relative cerebral blood volume (rCBV), ratios of choline/creatine (Cho/Cr) and/or choline/N-acetyl aspartate (Cho/NAA) between participants undergoing MRI evaluation. A χ2-based test of homogeneity was performed using Cochran's Q statistic and I2.
Of 397 patients in 13 studies who were analyzed, the majority had tumor recurrence. As there was evidence of heterogeneity among 10 of the studies which used rCBV for evaluation (Q statistic = 31.634, I2 = 97.11%, P < 0.0001) a random-effects analysis was applied. The pooled difference in means (2.18, 95%CI = 0.85 to 3.50) indicated that the average rCBV in a contrast-enhancing lesion was significantly higher in tumor recurrence compared with radiation injury (P = 0.001). Based on a fixed-effect model of analysis encompassing the six studies which used Cho/Cr ratios for evaluation (Q statistic = 8.388, I2 = 40.39%, P = 0.137), the pooled difference in means (0.77, 95%CI = 0.57 to 0.98) of the average Cho/Cr ratio was significantly higher in tumor recurrence than in tumor necrosis (P = 0.001). There was significant difference in ratios of Cho to NAA between recurrent tumor and necrosis (1.02, 95%CI = 0.03 to 2.00, P = 0.044).
MR spectroscopy and MR perfusion using Cho/NAA and Cho/Cr ratios and rCBV may increase the accuracy of differentiating necrosis from recurrent tumor in patients with primary brain tumors or metastases.
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DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
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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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Hydrogen embrittlement of high-strength steel is an obstacle for using these steels in sustainable energy production. Hydrogen embrittlement involves hydrogen-defect interactions at multiple-length ...scales. However, the challenge of measuring the precise location of hydrogen atoms limits our understanding. Thermal desorption spectroscopy can identify hydrogen retention or trapping, but data cannot be easily linked to the relative contributions of different microstructural features. We used cryo-transfer atom probe tomography to observe hydrogen at specific microstructural features in steels. Direct observation of hydrogen at carbon-rich dislocations and grain boundaries provides validation for embrittlement models. Hydrogen observed at an incoherent interface between niobium carbides and the surrounding steel provides direct evidence that these incoherent boundaries can act as trapping sites. This information is vital for designing embrittlement-resistant steels.
Lithium incorporation in kesterite Cu2ZnSn(S,Se)4 (CZTSSe) materials has been experimentally proven effective in improving electronic quality for application in photovoltaic devices. Herein, a ...feasible and effective solution‐based lithium post‐deposition treatment (PDT), enabling further efficiency improvement on the high‐performance baseline is reported and the dominant mechanism for this improvement is proposed. In this way, lithium is uniformly incorporated into grain interiors (GIs) without segregation at grain boundaries (GBs), which can occupy the Zn sites with a high solubility in the CZTSSe matrix, producing high density of LiZn antisites with shallower acceptor levels than the intrinsic dominant defect (CuZn antisites). As a result, CZTSSe absorber with better p‐type doping is obtained, leading to a pronounced enhancement in fill factor and a corresponding gain in open‐circuit voltage and short‐circuit current and consequently a significant efficiency boost from 9.3% to 10.7%. This work provides a feasible alternative alkali‐PDT treatment for chalcogenide semiconductors and promotes a better understanding of the mechanism of Li incorporation in kesterite materials.
A feasible solution‐based post‐deposition treatment is developed for the incorporation of Li into the grain interior of kesterite Cu2ZnSn(S,Se)4 materials for high performance solar cells. In this way, the dominant CuZn antisites of Cu2ZnSn(S,Se)4 are replaced with shallower LiZn antisites, resulting in significantly promoted p‐type conductivity and minority carrier lifetime and thereby pronounced improvement of efficiency from 9.3% to 10.7%.
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FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK