The Golden Age of Thermally Activated Delayed Fluorescence Materials: Design and Exploitation.

Since the seminal report by Adachi and co-workers in 2012, there has been a veritable explosion of interest in the design of thermally activated delayed fluorescence (TADF) compounds, particularly as emitters for organic light-emitting diodes (OLEDs). With rapid advancements and innovation in materials design, the efficiencies of TADF OLEDs for each of the primary color points as well as for white devices now rival those of state-of-the-art phosphorescent emitters. Beyond electroluminescent devices, TADF compounds have also found increasing utility and applications in numerous related fields, from photocatalysis, to sensing, to imaging and beyond.

Inverse design workflow discovers hole-transport materials tailored for perovskite solar cells.

The inverse design of tailored organic molecules for specific optoelectronic devices of high complexity holds an enormous potential but has not yet been realized. Current models rely on large data sets that generally do not exist for specialized research fields. We demonstrate a closed-loop workflow that combines high-throughput synthesis of organic semiconductors to create large datasets and Bayesian optimization to discover new hole-transporting materials with tailored properties for solar cell applications.

High-Entropy Metal-Organic Frameworks and Their Derivatives: Advances in Design, Synthesis, and Applications for Catalysis and Energy Storage.

As a nascent class of high-entropy materials (HEMs), high-entropy metal-organic frameworks (HE-MOFs) have garnered significant attention in the fields of catalysis and renewable energy technology owing to their intriguing features, including abundant active sites, stable framework structure, and adjustable chemical properties. This review offers a comprehensive summary of the latest developments in HE-MOFs, focusing on functional design, synthesis strategies, and practical applications. This work begins by presenting the design principles for the synthesis strategies of HE-MOFs, along with a detailed description of commonly employed methods based on existing reports.

Femtosecond Spin-State Switching Dynamics of Fe(II) Complexes Condensed in Thin Films.

The tailoring of spin-crossover films has made significant progress over the past decade, mostly motivated by the prospect in technological applications. In contrast to spin-crossover complexes in solution, the investigation of the ultrafast switching in spin-crossover films has remained scarce. Combining the progress in molecule synthesis and film growth with the opportunities at X-ray free-electron lasers, we study the photoinduced spin-state switching dynamics of a molecular film at room temperature.

Thermodynamically inconsistent extreme precipitation sensitivities across continents driven by cloud-radiative effects.

Extreme precipitation events are projected to intensify with global warming, threatening ecosystems and amplifying flood risks. However, observation-based estimates of extreme precipitation-temperature (EP-T) sensitivities show systematic spatio-temporal variability, with predominantly negative sensitivities across warmer regions. Here, we attribute this variability to confounding cloud radiative effects, which cool surfaces during rainfall, introducing covariation between rainfall and temperature beyond temperature's effect on atmospheric moisture-holding capacity.

Simple and versatile electrochemical synthesis of highly substituted 2,1-benzisoxazoles.

A sustainable, general and scalable electrochemical protocol for direct access to 3-(acylamidoalkyl)-2,1-benzisoxazoles by cathodic reduction of widely accessible nitro arenes is established. The method is characterised by a simple undivided set-up under constant current conditions, inexpensive and reusable carbon-based electrodes, and environmentally benign reaction conditions. The versatility of the developed protocol is demonstrated on 39 highly diverse examples with up to 81% yield.

Trp residues near peptide termini enhance the membranolytic activity of cationic amphipathic α-helices.

KIA peptides were designed as a series of cationic antimicrobial agents of different lengths, based on the repetitive motif [KIAGKIA]. As amphiphilic helices, they tend to bind initially to the surface of lipid membranes. Depending on the conditions, they are proposed to flip, insert and form toroidal pores, such that the peptides are aligned in a transmembrane orientation.

Combining simulation models and machine learning in healthcare management: strategies and applications.

Simulation models and artificial intelligence (AI) are largely used to address healthcare and biomedical engineering problems. Both approaches showed promising results in the analysis and optimization of healthcare processes. Therefore, the combination of simulation models and AI could provide a strategy to further boost the quality of health services.

Acetate Shock Loads Enhance CO Uptake Rates of Anaerobic Microbiomes.

Pyrolysis of lignocellulosic biomass commonly produces syngas, a mixture of gases such as CO, CO and H, as well as an aqueous solution generally rich in organic acids such as acetate. In this study, we evaluated the impact of increasing acetate shock loads during syngas co-fermentation with anaerobic microbiomes at different pH levels (6.7 and 5.

Measurement of the electric potential and the magnetic field in the shifted analysing plane of the KATRIN experiment.

The projected sensitivity of the effective electron neutrino-mass measurement with the KATRIN experiment is below 0.3 eV (90 % CL) after 5 years of data acquisition. The sensitivity is affected by the increased rate of the background electrons from KATRIN's main spectrometer.

A Stable Carbon-Centered Radical Showing Six Amphoteric Redox States.

An air- and moisture-stable hydrocarbon radical with four six- and three five-membered rings alternately fused to a heptacycle was obtained by ortho fusion in a suitably ortho,ortho'-substituted diphenylfluorene and subsequent re-establishment of the conjugation. The radical was obtained in five consecutive steps from commercially available starting materials with a total yield of 34 %; key steps are Suzuki couplings and cyclizing SAr reactions. Mesityl substituents at the five-membered rings ensure the stability of the radical.

Isoprene nitrates drive new particle formation in Amazon's upper troposphere.

New particle formation (NPF) in the tropical upper troposphere is a globally important source of atmospheric aerosols. It is known to occur over the Amazon basin, but the nucleation mechanism and chemical precursors have yet to be identified. Here we present comprehensive in situ aircraft measurements showing that extremely low-volatile oxidation products of isoprene, particularly certain organonitrates, drive NPF in the Amazonian upper troposphere.

Atomic-Scale Imaging of Polymers and Precision Molecular Weight Analysis.

Polymer design requires fine control over syntheses and a thorough understanding of their macromolecular structure. Herein, near-atomic level imaging of polymers is achieved, enabling the precise determination of one of the most important macromolecular characteristics: molecular weight. By judiciously designing and synthesizing different linear metal(loid)-rich homopolymers, subnanoscale polymer imaging is achieved through annular dark field-scanning transmission electron microscopy (ADF-STEM), owing to the incorporation of high atoms in the side chain of the monomeric units.

Activation of CH, NH, and N by Tantalum Ions, Clusters and Their Oxides: What Can Be Learnt from Studies of Ions in the Gas Phase.

The emission control of harmful compounds and greenhouse gases and the development of alternative, sustainable fuel sources is a major focus in current research. A solution for this problem lies in the development of efficient catalytic materials. Here, gas phase model systems represent prominent examples for obtaining fundamental insights on reaction properties of prospective catalytic systems.

Stabilisation of a Strontium Hydride with a Monodentate Carbazolyl Ligand and its Reactivity.

The molecular strontium hydride 2 [(Cbz)SrH(L)] (L=benzene, toluene) was isolated and stabilized by employing a sterically demanding carbazole ligand (Cbz=1,8-bis(3,5-ditertbutylphenyl)-3,6-ditertbutylcarbazolyl). Compound 2 was synthesized via phenylsilane metathesis with the corresponding amide (Cbz)SrN(SiMe) and characterized by H NMR, XRD and vibrational spectroscopy methods. We further investigated the stoichiometric reactivity of 2 towards carbon monoxide, azobenzene and trimethylsilylacetylene, showing three distinct reactivity pathways: addition, reduction and deprotonation.

Restraining Planar Gliding in Single-Crystalline LiNiCoMnO Cathodes by Combining Bulk and Surface Modification Strategies.

The delamination cracking from planar gliding along the (003) facets and anisotropic lattice strain perpendicular to the (003) facets inevitable lead to degradation of Ni-rich single-crystal cathode materials, adversely affecting their cyclability. Herein, we rationally design a single-crystal LiNiCoMnO (SC90) cathode with robust chemo-mechanical properties, in which coherently grown MgO octahedra and BO tetrahedra are incorporated into the lattice, and a stabilizing Mg(BO) layer is concurrently formed on the particle surface. Multiscale in/ex situ characterizations and theoretical calculations indicate that introducing the MgO and BO units leads to a "pinning effect" within the layered structure.

Responsive 3D Printed Microstructures Based on Collagen Folding and Unfolding.

Mimicking extracellular matrices holds great potential for tissue engineering in biological and biomedical applications. A key compound for the mechanical stability of these matrices is collagen, which also plays an important role in many intra- and intercellular processes. Two-photon 3D laser printing offers structuring of these matrices with subcellular resolution.

Cyclodextrin-based rotaxanes for polymer materials: challenge on simultaneous realization of inexpensive production and defined structures.

Owing to their dynamic natures, rotaxane-based polymers are attractive motifs for developing stimuli-responsive materials. However, the accurate control of the rotaxane structure, which can be achieved via multistep synthesis, is key to utilizing the material. Concurrently, implementing a scale-up synthesis procedure to exploit the application potential of rotaxane-based polymers induces structural ambiguities, thereby presenting a significant trade-off between realizing inexpensive production and defined structures.

Functionalization of monolithic MOF thin films with hydrocarbon chains to achieve superhydrophobic surfaces with tunable water adhesion strength.

While the accessible pores render an enormous variety of functionalities to the bulk of metal-organic frameworks (MOFs), the outer surfaces exposed by these crystalline materials also offer unique characteristics not available when using conventional substrates. By grafting hydrocarbon chains to well-defined MOF thin films (SURMOFs) prepared using layer-by-layer methods, we were able to fabricate superhydrophobic substrates with static water contact angles over 160°. A detailed theoretical modelling of the hydrocarbon chains grafted on the outer SURMOF surface with well-defined spacing between anchoring points reveals that the grafted hydrocarbon chains behave similarly to polymer brushes during wetting, where conformational entropy is traded with mixing entropy.