Rapid Combinatorial Synthesis and Chromatography Based Screening of Phosphorescent Iridium Complexes for Solution Processing

This work reports the combinatorial synthesis and screening of phosphorescent iridium complexes as solution processable emitters for OLEDs. The approach taken here allows for the rapid synthesis, isolation, spectroscopic characterization and identification of the libraries based on chromatographic methods. Subsequent analysis of the irradiation induced degradation provides insight on the stability of the complexes under continuous excitation. The method is versatile and can easily be applied to other metal complexes or organic dyes for various applications, e.g., in electroluminescence, photovoltaics and sensing.     

Diindenoperylene derivatives: A model to investigate the path from molecular structure via morphology to solar cell performance

Efficient organic electronic devices require a detailed understanding of the relation between molecular structure, thin film growth, and device performance, which is only partially understood at present. Here, we show that small changes in molecular structure of a donor absorber material lead to significant changes in the intermolecular arrangement within organic solar cells. For this purpose, phenyl rings and propyl side chains are fused to the diindenoperylene (DIP) molecule. Grazing incidence X-ray diffraction and variable angle spectroscopic ellipsometry turned out to be a powerful combination to gain detailed information about the thin film growth. Planar and bulk heterojunction solar cells with C60 as acceptor and the DIP derivatives as donor are fabricated to investigate the influence of film morphology on the device performance. Due to its planar structure, DIP is found to be highly crystalline in pristine and DIP:C60 blend films while its derivatives grow liquid-like crystalline. This indicates that the molecular arrangement is strongly disturbed by the steric hindrance induced by the phenyl rings. The high fill factor (FF) of more than 75% in planar heterojunction solar cells of the DIP derivatives indicates excellent charge transport in the pristine liquid-like crystalline absorber layers. However, bulk heterojunctions of these materials surprisingly result in a low FF of only 54% caused by a weak phase separation and thus poor charge carrier percolation paths due to the lower ordered thin film growth. In contrast, crystalline DIP:C60 heterojunctions lead to high FF of up to 65% as the crystalline growth induces better percolation for the charge carriers. However, the major drawback of this crystalline growth mode is the nearly upright standing orientation of the DIP molecules in both pristine and blend films. This arrangement results in low absorption and thus a photocurrent which is significantly lower than in the DIP derivative devices, where the liquid-like crystalline growth leads to a more horizontal molecular alignment. Our results underline the complexity of the molecular structure-device performance relation in organic semiconductor devices.     

Structural Aspects of P2-Type Na0.67Mn0.6Ni0.2Li0.2O2 (MNL) Stabilization by Lithium Defects as a Cathode Material for Sodium-Ion Batteries

A known strategy for improving the properties of layered oxide electrodes in sodium-ion batteries is the partial substitution of transition metals by Li. Herein, the role of Li as a defect and its impact on sodium storage in P2-Na_0.67Mn_0.6Ni_0.2Li_0.2O₂ is discussed. In tandem with electrochemical studies, the electronic and atomic structure are studied using solid-state NMR, operando XRD, and density functional theory (DFT). For the as-synthesized material, Li is located in comparable amounts within the sodium and the transition metal oxide (TMO) layers. Desodiation leads to a redistribution of Li ions within the crystal lattice. During charging, Li ions from the Na layer first migrate to the TMO layer before reversing their course at low Na contents. There is little change in the lattice parameters during charging/discharging, indicating stabilization of the P2 structure. This leads to a solid-solution type storage mechanism (sloping voltage profile) and hence excellent cycle life with a capacity of 110 mAh g^-1 after 100 cycles. In contrast, the Li-free compositions Na_0.67Mn_0.6Ni_0.4O₂ and Na_0.67Mn_0.8Ni_0.2O₂ show phase transitions and a stair-case voltage profile. The capacity is found to originate from mainly Ni³⁺/Ni⁴⁺ and O^2-/O^2-δ redox processes by DFT, although a small contribution from Mn⁴⁺/Mn⁵⁺ to the capacity cannot be excluded.     

Miniaturized Flexible Electronic Systems with Wireless Power and Near‐Field Communication Capabilities

A class of thin, lightweight, flexible, near‐field communication (NFC) devices with ultraminiaturized format is introduced, and systematic investigations of the mechanics, radio frequency characteristics, and materials aspects associated with their optimized construction are presented. These systems allow advantages in mechanical strength, placement versatility, and minimized interfacial stresses compared to other NFC technologies and wearable electronics. Detailed experimental studies and theoretical modeling of the mechanical and electromagnetic properties of these systems establish understanding of the key design considerations. These concepts can apply to many other types of wireless communication systems including biosensors and electronic implants.     

Supramolecular Assembly of Aminoethylene‐Lipopeptide PMO Conjugates into RNA Splice‐Switching Nanomicelles

Phosphorodiamidate morpholino oligomers (PMOs) are oligonucleotide analogs that can be used for therapeutic modulation of pre‐mRNA splicing. Similar to other classes of nucleic acid‐based therapeutics, PMOs require delivery systems for efficient transport to the intracellular target sites. Here, artificial peptides based on the oligo(ethylenamino) acid succinyl‐tetraethylenpentamine (Stp), hydrophobic modifications, and an azide group are presented, which are used for strain‐promoted azide‐alkyne cycloaddition conjugation with splice‐switching PMOs. By systematically varying the lead structure and formulation, it is determined that the type of contained fatty acid and supramolecular assembly have a critical impact on the delivery efficacy. A compound containing linolenic acid with three cis double bonds exhibits the highest splice‐switching activity and significantly increases functional protein expression in pLuc/705 reporter cells in vitro and after local administration in vivo. Structural and mechanistic studies reveal that the lipopeptide PMO conjugates form nanoparticles, which accelerate cellular uptake and that the content of unsaturated fatty acids enhances endosomal escape. In an in vitro Duchenne muscular dystrophy exon skipping model using H2K‐mdx52 dystrophic skeletal myotubes, the highly potent PMO conjugates mediate significant splice‐switching at very low nanomolar concentrations. The presented aminoethylene‐lipopeptides are thus a promising platform for the generation of PMO‐therapeutics with a favorable activity/toxicity profile.     

电容式触摸传感器提升应用设计

好像在突然之间，电容式传感器就无处不在了。它被安装在汽车座位里以控制气囊配置和安全带预紧装置，在洗碗机和干燥机中以校正旋转桶的状态，甚至冰箱也使用其来控制自动去冰过程。但是直到现在，它最大的潜在应用领域还是触摸开关，触摸开关已越来越多地出现在消费电子产品中。