Twisted Phenanthro[9,10-d]imidazole Derivatives as Non-doped Emitters for Efficient Electroluminescent Devices with Ultra-Deep Blue Emission and High Exciton Utilization Efficiency

Herein, two deep-blue emissive molecules ( SAF-PI and SAF-DPI ) are designed and synthesized using spiro[acridine-9,9’-fluorene] as a donor (D) substituted with 2-(3-methylphenyl)-1-phenyl-phenanthro[9,10-d]imidazole as an acceptor (A), forming twisted D−A and A−D−A structures, respectively. The photophysical studies and density functional theory (DFT) calculations reveal that both molecules exhibit hybridized local excited and charge transfer (HLCT) characteristics with deep blue emission color. They are effectively applied as non-doped emitters in OLEDs. Particularly, SAF-PI -based device achieves the high-definition television (HDTV) standard blue color emission peaked at 428 nm with CIE coordinate of (0.156, 0.053), a narrow full width at half maximum of 55 nm, a maximum external quantum efficiency (EQE_max) of 4.57% and an exciton utilization efficiency of 65%.     

Focal Point Evaluation of Energies for Tautomers and Isomers for 3-hydroxy-2-butenamide: Evaluation of Competing Internal Hydrogen Bonds of Types -OH…O=, -OH…N, -NH…O=, and CH…X (X=O and N)

The title compound is a small molecule with many structural variations; it can illustrate a variety of internal hydrogen bonds, among other noncovalent interactions. Here we examine structures displaying hydrogen bonding between carbonyl oxygen and hydroxyl H; between carbonyl oxygen and amino H; hydroxyl H and amino N; hydroxyl O and amino H. We also consider H-bonding in its tautomer 2-oxopropanamide. By extrapolation algorithms applied to Hartree-Fock and correlation energies as estimated in HF, MP2, and CCSD calculations using the cc-pVNZ correlation-consistent basis sets (N = 2, 3, and 4) we obtain reliable relative energies of the isomeric forms. Assuming that such energy differences may be attributed to the presence of the various types of hydrogen bonding, we attempt to infer relative strengths of types of H-bonding. The Atoms in Molecules theory of Bader and the Local Vibrational Modes analysis of Cremer and Kraka are applied to this task. Hydrogen bonds are ranked by relative strength as measured by local stretching force constants, with the stronger =O…HO- > NH…O= > -OH…N well separated from a cluster > NH…O= ≈ >NH…OH ≈ CH…O= of comparable and intermediate strength. Weaker but still significant interactions are of type CH…N which is stronger than CH…OH.     

An infrared small target detection algorithm based on high-speed local contrast method

Small-target detection in infrared imagery with a complex background is always an important task in remote sensing fields. It is important to improve the detection capabilities such as detection rate, false alarm rate, and speed. However, current algorithms usually improve one or two of the detection capabilities while sacrificing the other. In this letter, an Infrared (IR) small target detection algorithm with two layers inspired by Human Visual System (HVS) is proposed to balance those detection capabilities. The first layer uses high speed simplified local contrast method to select significant information. And the second layer uses machine learning classifier to separate targets from background clutters. Experimental results show the proposed algorithm pursue good performance in detection rate, false alarm rate and speed simultaneously.     

Probing the Local Reaction Environment During High Turnover Carbon Dioxide Reduction with Ag-Based Gas Diffusion Electrodes

Discerning the influence of electrochemical reactions on the electrode microenvironment is an unavoidable topic for electrochemical reactions that involve the production of OH⁻ and the consumption of water. That is particularly true for the carbon dioxide reduction reaction (CO₂RR), which together with the competing hydrogen evolution reaction (HER) exert changes in the local OH⁻ and H₂O activity that in turn can possibly affect activity, stability, and selectivity of the CO₂RR. We determine the local OH⁻ and H₂O activity in close proximity to a CO₂-converting Ag-based gas diffusion electrode (GDE) with product analysis using gas chromatography. A Pt nanosensor is positioned in the vicinity of the working GDE using shear-force-based scanning electrochemical microscopy (SECM) approach curves, which allows monitoring changes invoked by reactions proceeding within an otherwise inaccessible porous GDE by potentiodynamic measurements at the Pt-tip nanosensor. We show that high turnover HER/CO₂RR at a GDE lead to modulations of the alkalinity of the local electrolyte, that resemble a 16 m KOH solution, variations that are in turn linked to the reaction selectivity.     

Charge redistribution and a shortening of the Fe—As bond at the quantum critical point of SmO1–xFxFeAs

Many researchers have pointed out that there is a quantum critical point (QCP) in the F‐doped SmOFeAs system. In this paper, the electronic structure and local structure of the superconductive FeAs layer in SmO_1–xF_xFeAs as a function of the F‐doping concentration have been investigated using Fe and As K‐edge X‐ray absorption spectroscopy. Experiments performed on the X‐ray absorption near‐edge structure showed that in the vicinity of the QCP the intensity of the pre‐edge feature at the Fe‐edge decreases continuously, while there is a striking rise of the shoulder‐peak at the As edge, suggesting the occurrence of charge redistribution near the QCP. Further analysis on the As K‐edge extended X‐ray absorption fine structure demonstrated that the charge redistribution originates mostly from a shortening of the Fe—As bond at the QCP. An evident relationship between the mysterious QCP and the fundamental Fe—As bond was established, providing new insights on the interplay between QCP, charge dynamics and the local structural Fe—As bond in Fe‐based superconductors.     

Asymptotically exact a posteriori local discontinuous Galerkin error estimates for the one‐dimensional second‐order wave equation

In this article, we analyze a residual‐based a posteriori error estimates of the spatial errors for the semidiscrete local discontinuous Galerkin (LDG) method applied to the one‐dimensional second‐order wave equation. These error estimates are computationally simple and are obtained by solving a local steady problem with no boundary condition on each element. We apply the optimal L² error estimates and the superconvergence results of Part I of this work [Baccouch, Numer Methods Partial Differential Equations 30 (2014), 862–901] to prove that, for smooth solutions, these a posteriori LDG error estimates for the solution and its spatial derivative, at a fixed time, converge to the true spatial errors in the L²‐norm under mesh refinement. The order of convergence is proved to be , when p‐degree piecewise polynomials with are used. As a consequence, we prove that the LDG method combined with the a posteriori error estimation procedure yields both accurate error estimates and superconvergent solutions. Our computational results show higher convergence rate. We further prove that the global effectivity indices, for both the solution and its derivative, in the L²‐norm converge to unity at rate while numerically they exhibit and rates, respectively. Numerical experiments are shown to validate the theoretical results. © 2014 Wiley Periodicals, Inc. Numer Methods Partial Differential Eq 31: 1461–1491, 2015     

A local parallel superconvergence method for the incompressible flow by coarsening projection

In this article, we investigate a local parallel superconvergence method by coarsening projection for the incompressible Stokes flow. The method is a combination of the local superconvergence technique and the given framework of local parallel method. For the smooth subdomains, the local superconvergence method is applied in a higher order finite dimensional space corresponding to an appropriate coarse mesh on interior domain. Moreover, a useful and flexible local parallel method is designed to obtain the local parallel superconvergence results of presented method, which offset theoretical limitation of the model without the smoothness of the exact solution and a priori regularity of the underlying problem over the whole domain. © 2014 Wiley Periodicals, Inc. Numer Methods Partial Differential Eq 31: 1209–1223, 2015     

Azobenzene‐Functionalized Metal–Organic Polyhedra for the Optically Responsive Capture and Release of Guest Molecules

Stimuli‐responsive metal–organic polyhedra (srMOPs) functionalized with azobenzene showed UV‐irradiation‐induced isomerization from the insoluble trans‐srMOP to the soluble cis‐srMOP, whereas irradiation with blue light reversed this process. Guest molecules were trapped and released upon cis‐to‐trans and trans‐to‐cis isomerization of the srMOPs, respectively. This study provides a new direction in the ever‐diversifying field of MOPs, while laying the groundwork for a new class of optically responsive materials.     

Thermal or Mechanical Stimuli‐Induced Photoluminescence Color Change of a Molecular Assembly Composed of an Amphiphilic Anthracene Derivative in Water

Molecular assemblies that change photoluminescence color in response to thermal or mechanical stimulation without dissociation into the monomeric states in water are described herein. A dumbbell‐shaped amphiphilic compound forms micellar molecular assemblies in water and exhibits yellow photoluminescence derived from excimer formation of the luminescent core, which contains a 2,6‐diethynylanthracene moiety. Annealing of the aqueous solution induces a photoluminescence color change from yellow to green (λ_{em, max}=558→525 nm). The same photoluminescence color change is also achieved by rubbing the yellow‐photoluminescence‐emitting molecular assemblies adsorbed on glass substrates with cotton wool in water. The observed green photoluminescence is ascribed to micelles that are distinct from the yellow‐photoluminescence‐emitting micelles, on the basis of transmission electron microscopy observations, atomic force microscopy observations, and dynamic light scattering measurements. We examined the relationship between the structure of the molecular assemblies and the photophysical properties of the anthracene derivative in water before and after thermal or mechanical stimulation and concluded that thermal or mechanical stimuli‐induced slight changes of the molecular‐assembled structures in the micelles result in the change in the photoluminescence color from yellow to green in water.     

Enhanced Anticancer Efficacy by ATP‐Mediated Liposomal Drug Delivery

A liposome‐based co‐delivery system composed of a fusogenic liposome encapsulating ATP‐responsive elements with chemotherapeutics and a liposome containing ATP was developed for ATP‐mediated drug release triggered by liposomal fusion. The fusogenic liposome had a protein–DNA complex core containing an ATP‐responsive DNA scaffold with doxorubicin (DOX) and could release DOX through a conformational change from the duplex to the aptamer/ATP complex in the presence of ATP. A cell‐penetrating peptide‐modified fusogenic liposomal membrane was coated on the core, which had an acid‐triggered fusogenic potential with the ATP‐loaded liposomes or endosomes/lysosomes. Directly delivering extrinsic liposomal ATP promoted the drug release from the fusogenic liposome in the acidic intracellular compartments upon a pH‐sensitive membrane fusion and anticancer efficacy was enhanced both in vitro and in vivo.