An easy-to-access, near-UV-emitting linearly extended B,Ndoped heptacene with high thermal stability is designed and synthesized in good yields. This compound exhibits thermally activated delayed fluorescence (TADF) at ambient temperature from a multiresonant (MR) state and represents a rare example of a non-triangulene-based MR-TADF emitter. At lower temperatures triplet−triplet annihilation dominates. The compound simultaneously possesses narrow, deep-blue emission with CIE coordinates of (0.17, 0.01). While delayed fluorescence results mainly from triplet−triplet annihilation at lower temperatures in THF solution, where aggregates form upon cooling, the TADF mechanism takes over around room temperature in solution when the aggregates dissolve or when the compound is well dispersed in a solid matrix. The potential of our molecular design to trigger TADF in larger acenes is demonstrated through the accurate prediction of ΔE ST using correlated wave-function-based calculations. On the basis of these calculations, we predicted dramatically different optoelectronic behavior in terms of both ΔE ST and the optical energy gap of two constitutional isomers where only the boron and nitrogen positions change. A comprehensive structural, optoelectronic, and theoretical investigation is presented. In addition, the ability of the achiral molecule to assemble on a Au(111) surface to a highly ordered layer composed of enantiomorphic domains of racemic entities is demonstrated by scanning tunneling microscopy.
Previous analytical results on the resilience of unstructured P2P systems have not explicitly modeled heterogeneity of user churn (i.e., difference in online behavior) or the impact of in-degree on system resilience. To overcome these limitations, we introduce a generic model of heterogeneous user churn, derive the distribution of the various metrics observed in prior experimental studies (e.g., lifetime distribution of joining users, joint distribution of session time of alive peers, and residual lifetime of a randomly selected user), derive several closed-form results on the transient behavior of in-degree, and eventually obtain the joint in/out degree isolation probability as a simple extension of the out-degree model in [20].
The synthesis of terpenes is a large field of research that is woven deeply into the history of chemistry. Terpene biosynthesis is a case study of how the logic of a modular design can lead to diverse structures with unparalleled efficiency. This work leverages modern nickel-catalyzed electrochemical sp 2 –sp 3 decarboxylative coupling reactions, enabled by silver nanoparticle–modified electrodes, to intuitively assemble terpene natural products and complex polyenes by using simple modular building blocks. The step change in efficiency of this approach is exemplified through the scalable preparation of 13 complex terpenes, which minimized protecting group manipulations, functional group interconversions, and redox fluctuations. The mechanistic aspects of the essential functionalized electrodes are studied in depth through a variety of spectroscopic and analytical techniques.
Imidazole-substituted metalloporphyrins are valuable for studies of self-assembly and for applications where water solubility is required. Rational syntheses of porphyrins bearing one or two imidazol-2-yl or imidazol-4-yl groups at the meso positions have been developed. The syntheses employ dipyrromethanes, 1-acyldipyrromethanes, and 1,9-diacyldipyrromethanes bearing an imidazole group at the 5-position. The polar, reactive imidazole unit was successfully masked by use of (1) the 2-(trimethylsilyl)ethoxymethyl (SEM) group at the imidazole pyrrolic nitrogen, and (2) a dialkylboron motif bound to the pyrrole of the dipyrromethane and coordinated to the imidazole imino nitrogen. The nonpolar nature of such doubly masked imidazolyl-dipyrromethanes facilitated handling. Selected masked dipyrromethanes were characterized by 11B and 15N NMR spectroscopy. Five distinct methods were examined to obtain trans-A2B2-, trans-AB2C-, and trans-AB-porphyrins. Each porphyrin contained one or two SEM-protected imidazole units. The SEM group could be removed with TBAF or HCl. Two zinc(II) porphyrins and a palladium(II) porphyrin bearing a single imidazole moiety were prepared and subjected to alkylation (with ethyl iodide, 1,3-propane sultone, or 1,4-butane sultone) to give water-soluble imidazolium- porphyrins. This work establishes the foundation for the rational synthesis of a variety of porphyrins containing imidazole units.
Hard magnetic materials with high remnant magnetic moment, Mr, have unique advantages that can achieve bi-directional (push–pull) movement in an external magnetic field. This paper presents the results on the fabrication and testing of novel composite elastic permanent magnet films. The microsize hard barium ferrite powder, NdFeB powder, and different silicone elastomers have been used to fabricate various large elongation hard magnetic films. Three different fabrication methods, screen-coating processing, moulding processing and squeegee-coating processing, have been investigated, and the squeegee-coating process was proven to be the most successful method. The uniform composite elastic permanent magnet films range from 40 µm to 216 µm in thickness have been successfully fabricated. These films were then magnetized in the thickness direction after fabrication. They exhibited permanent magnet behaviour; for instance, the film (0.640 mm3 in volume) made of polydimethyl siloxane (PDMS) and hard barium ferrite powders is measured to give a coercive force, Hc, of 3.24 × 105 A m−1 and Mr of 1.023 × 10−5 A m2, and the film (0.504 mm3 in volume) made of PDMS and NdFeB powders gives 1.55 × 105 A m−1 Hc and 8.081 × 10−5 A m2 Mr. These composite elastic permanent magnet films' mechanical properties, like Young's modulus and deflection force, have been evaluated. To validate the films' Young's modulus, a finite-element computer simulation (ANSYS®) is used and one film is chosen whose Young's modulus (16.60 MPa) is confirmed by the simulation results with ANSYS®. The large elongation composite elastic permanent magnet film provides an excellent diaphragm material, which plays an important role in the micropump or valve. The movement of the 126 µm thick film with 4.5 mm diameter made of PDMS and NdFeB powders has been tested in a 0.21 Tesla external magnetic field. It was proven to have large deflection of 125 µm.
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