Organic light-emitting diodes (OLEDs) have their performance limited by the number of emissive singlet states created upon charge recombination (25%). Recently, a novel strategy has been proposed, based on thermally activated up-conversion of triplet to singlet states, yielding delayed fluorescence (TADF), which greatly enhances electroluminescence. The energy barrier for this reverse intersystem crossing mechanism is proportional to the exchange energy (ΔEST ) between the singlet and triplet states; therefore, materials with intramolecular charge transfer (ICT) states, where it is known that the exchange energy is small, are perfect candidates. However, here it is shown that triplet states can be harvested with 100% efficiency via TADF, even in materials with ΔEST of more than 20 kT (where k is the Boltzmann constant and T is the temperature) at room temperature. The key role played by lone pair electrons in achieving this high efficiency in a series of ICT molecules is elucidated. The results show the complex photophysics of efficient TADF materials and give clear guidelines for designing new emitters.
Matrix stiffening with downstream activation of mechanosensitive pathways is strongly implicated in progressive fibrosis; however, pathologic changes in extracellular matrix (ECM) that initiate mechano-homeostasis dysregulation are not defined in human disease. By integrated multiscale biomechanical and biological analyses of idiopathic pulmonary fibrosis lung tissue, we identify that increased tissue stiffness is a function of dysregulated post-translational collagen cross-linking rather than any collagen concentration increase whilst at the nanometre-scale collagen fibrils are structurally and functionally abnormal with increased stiffness, reduced swelling ratio, and reduced diameter. In ex vivo and animal models of lung fibrosis, dual inhibition of lysyl oxidase-like (LOXL) 2 and LOXL3 was sufficient to normalise collagen fibrillogenesis, reduce tissue stiffness, and improve lung function in vivo. Thus, in human fibrosis, altered collagen architecture is a key determinant of abnormal ECM structure-function, and inhibition of pyridinoline cross-linking can maintain mechano-homeostasis to limit the self-sustaining effects of ECM on progressive fibrosis.
The efficient synthesis and photophysical properties of a series of ambipolar donor-acceptor-donor systems is described where the acceptor is dibenzothiophene S,S-dioxide and the donor is fluorene, carbazole, or arylamine. The systems exhibit intramolecular charge transfer (ICT) states (of variable ICT character strengths) leading to fluorescence emission ranging from deep blue to green with moderate to high photoluminescence quantum yields. The emission properties can be effectively tuned by systematically changing the position of substitution on both donor and acceptor units (which affects the extent of conjugation) and the redox potentials of the donor units. The results are supported by cyclic voltammetric data and TD-DFT calculations.
A metal-catalyst-free growth method of carbon nanotubes (CNTs) has been developed using chemical vapor deposition of CNTs on carbon-implanted SiGe islands on Si substrates. From scanning electron microscopy and Raman measurements, the fabricated CNTs are identified as single-walled CNTs with a diameter ranging from 1.2 to 1.6 nm. Essential parts of the substrate preparation after CVD SiGe growth and carbon implant are a chemical oxidization by hydrogen peroxide solution and a heat treatment at 1000 °C prior to CNT growth. We believe that these processes enhance surface decomposition and assist the formation of carbon clusters, which play a role in seeding CNT growth. The growth technique is a practical method of growing metal-free CNTs for a variety of applications, while at the same time opening up the prospect of merging CNT devices into silicon very-large-scale-integration technology.
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