Exploiting Covalent Chemical Labeling with Self-Labeling Proteins.

The visualization and manipulation of proteins in live cells are critical for studying complex biological processes. Self-labeling proteins do so by enabling the specific and covalent attachment of synthetic probes, offering unprecedented flexibility in the chemical labeling of proteins in live cells and in vivo. By combining the excellent photophysical properties of synthetic dyes with genetic targetability, these tags provide a modular and innovative toolbox for live-cell and high-resolution fluorescence imaging.

Electrolyte Effects in Membrane-Electrode-Assembly CO Electrolysis.

Membrane-electrode-assembly (MEA)-based CO electrolysis (COE) has demonstrated the capability to produce C products with high faradaic efficiency at ampere-level current densities. However, most studies on COE have achieved performance benchmarks under strongly alkaline conditions (e.g.

Impact of processing atmosphere on nanoscale properties of highly efficient CsMAFAPbI perovskite solar cells.

The fabrication process of triple-cation-halide organic inorganic perovskites must be tightly controlled to make high-efficiency solar cells. After precursor deposition, the amount of oxygen and moisture during the annealing process is important but not always well-monitored and understood. In this study, CsMAFAPbI perovskite films were annealed in different environments, namely N, O and air, to systematically explore the relationship between the evolution of PbI, the grain boundary band bending and the optoelectronic properties.

Functionalized Phenyl Methanaminium Salts Provide Highly Stable Perovskite Solar Cells.

One of the leading approaches to enhancing the performance and stability of perovskite solar cells (PSCs) involves passivating the perovskite surface and grain boundaries with large ammonium salts. Here, we report the synthesis of furan-, thiophene-, and selenophene-functionalized phenyl methanaminium iodide salts (, , and ) and their application as passivating agents on 3D [(CsFAMA)Pb(IBrCl)] perovskite. The -passivated PSCs performed the best and achieved a power conversion efficiency (PCE) of 23.

Magnetically and optically active edges in phosphorene nanoribbons.

Nanoribbons, nanometre-wide strips of a two-dimensional material, are a unique system in condensed matter. They combine the exotic electronic structures of low-dimensional materials with an enhanced number of exposed edges, where phenomena including ultralong spin coherence times, quantum confinement and topologically protected states can emerge. An exciting prospect for this material concept is the potential for both a tunable semiconducting electronic structure and magnetism along the nanoribbon edge, a key property for spin-based electronics such as (low-energy) non-volatile transistors.

Bulk Measurement of Membrane Permeability for Random Cyclic Peptides in Living Cells to Guide Drug Development.

Cyclic peptides are attractive for drug discovery due to their excellent binding properties and the potential to cross cell membranes. However, by far, not all cyclic peptides are cell permeable, and measuring or predicting their membrane permeability is not trivial. In this work, we assessed the membrane permeability of thioether-cyclized peptides, a widely used format in drug discovery.

Aldehyde-Stabilization Strategies for Building Biobased Consumer Products around Intact lignocellulosic Structures.

Dwindling fossil resources and their associated environmental concerns have increased interest in biobased products. In particular, many approaches to convert lignocellulosic biomass into small-molecule building blocks are being explored via thermal, chemical, and biological processes. Depending on their structure, these molecules can be used as direct (i.

Pd-Catalyzed Strain-Releasing Dyotropic Rearrangement: Ring-Expanding Amidofluorination of Methylenecyclobutanes.

Under the Pd(II)/Pd(IV) catalytic cycle, the cyclization of pent-4-en-1-amine derivatives typically yields either pyrrolidines or piperidines depending on the N-protecting group. We report herein an unprecedented Pd(II)-catalyzed oxidative domino process that converts readily accessible N-protected 2-(2-amidoethyl)-1-methylenecyclobutane derivatives to 1-fluoro-2-azabicyclo[3.2.

Single-Grain High-Efficiency Full-Visible-Spectrum White Emitters.

Full-visible-spectrum emission phosphors are promising candidates for next-generation white light-emitting diodes (WLEDs), overcoming the complex and high costs of traditional mixed phosphors. However, their practical application is hindered by low luminescence efficiency. In this regard, a generalization strategy is developed that involves creating heterostructure interfaces to prevent detrimental energy transfer processes, thereby boosting efficiency.

Quantum interference observed in state-resolved molecule-surface scattering.

Although the dynamics of collisions between a molecule and a solid surface are ultimately quantum mechanical, decohering effects owing to the large number of interacting degrees of freedom typically obscure the wavelike nature of these events. However, a partial decoupling of internal molecular motion from external degrees of freedom can reveal striking interference effects despite significant momentum exchange between the molecule and the bath of surface vibrations. We report state-prepared and state-resolved measurements of methane scattering from a room-temperature gold surface that demonstrate total destructive interference between molecular states related by a reflection symmetry operation.

Predicting Toxicity toward Nitrifiers by Attention-Enhanced Graph Neural Networks and Transfer Learning from Baseline Toxicity.

Assessing chemical environmental impacts is critical but challenging due to the time-consuming nature of experimental testing. Graph neural networks (GNNs) support superior prediction performance and mechanistic interpretation of (eco-)toxicity data, but face the risk of overfitting on the typically small experimental data sets. In contrast to purely data-driven approaches, we propose a mechanism-guided transfer learning strategy that is highly efficient and provides key insights into the underlying drivers of (eco-)toxicity.

Nanowire morphology control in Sb metal-derived antimony selenide photocathodes for solar water splitting.

We report a facile method to enhance the photoelectrochemical (PEC) performance of SbSe photocathodes by controlling the growth of bilayer SbSe consisting of vertically oriented nanorods on a compact SbSe layer. SbSe thin films with controllable nanorod diameters were achieved by manipulating the substrate temperatures during metallic Sb thin film deposition. The lower temperature-derived SbSe photocathode, with a larger nanorod diameter (202 ± 48 nm), demonstrated a photocurrent density of -15.

Dipolar Carbazole Ammonium for Broadened Electric Field Distribution in High-Performance Perovskite Solar Cells.

Perovskite solar cells (PSCs) with ammonium passivation exhibit superior device performance and stability. Beyond typical chemical passivation, ammonium salts control the electronic structure of perovskite surfaces, yet the molecular structure-property relationship requires further understanding, especially the dipole effect. Here, we employed carbazole and its halogenated counterpart as the functional group of ammonium salts.

Ultrathin liquid sheets: water gets in shape for VUV absorption.

We present absorption spectra of thin, free-flowing liquid sheets in the vacuum ultraviolet energy range using a gas-squeezed liquid jet. Compared to liquid flow cells, operation without transmission windows eliminates restrictions on the energy range. The temperature of the water sheet is estimated at 0 ± 3 °C, at the verge of the supercooled regime.

Characterization of the glutathione redox state in the Golgi apparatus.

Redox homeostasis is crucial for cell function, and, in eukaryotic cells, studying it in a compartmentalized way is essential due to the redox variations between different organelles. The redox state of organelles is largely determined by the redox potential of glutathione, E, and the concentration of its reduced and oxidized species, [GS]. The Golgi apparatus is an essential component of the secretory pathway, yet little is known about the concentration or redox state of GSH in this organelle.

SiR-XActin: A fluorescent probe for imaging actin dynamics in live cells.

Imaging actin-dependent processes in live cells is important for understanding numerous biological processes. However, currently used natural-product based fluorescent probes for actin filaments affect the dynamics of actin polymerization and can induce undesired cellular phenotypes. Here, we introduce SiR-XActin, a simplified jasplakinolide-based, far-red fluorescent probe that enables bright and photostable staining in various cell types without requiring genetic modifications.

Perovskite heteroepitaxy for high-efficiency and stable pure-red LEDs.

Ultrasmall CsPbI perovskite quantum dots (QDs) are the most promising candidates for realizing efficient and stable pure-red perovskite light-emitting diodes (PeLEDs). However, it is challenging for ultrasmall CsPbI QDs to retain their solution-phase properties when they assemble into conductive films, greatly hindering their device application. Here we report an approach for in situ deposit stabilized ultrasmall CsPbI QD conductive solids, by constructing CsPbI QD/quasi-two-dimensional (quasi-2D) perovskite heteroepitaxy.

Tailored Lattice-Matched Carbazole Self-Assembled Molecule for Efficient and Stable Perovskite Solar Cells.

Self-assembled monolayer molecules have been widely employed as interfacial transport materials in inverted perovskite solar cells (PSCs), demonstrating high efficiency and improved device stability. However, self-assembling monolayer (SAM) molecules often suffer from aggregation and weak interactions with the perovskite layer, resulting in inefficient charge transfer and significant energy losses, ultimately limiting the power conversion efficiency and long-term stability of perovskite solar cells. In this work, we developed a series of novel skeleton-matching carbazole isomer SAMs based on the following key design principles: (1) introducing a benzene ring structure to distort the molecular skeleton of the SAM, thereby preventing aggregation and achieving a uniform distribution on fluorine-doped tin oxide (FTO) substrates; (2) strategically incorporating methoxy groups onto the benzene ring at different positions (ortho, meta, and para).

Chiral light-matter interactions in solution-processable semiconductors.

Chirality is a fundamental property widely observed in nature, arising in objects without a proper rotation axis, therefore existing as forms with distinct handedness. This characteristic can profoundly impact the properties of materials and can enable new functionality, especially for spin-optoelectronics. Chirality enables asymmetric light and spin interactions in materials, with widespread potential applications ranging from energy-efficient displays, holography, imaging, and spin-selective and enantio-selective chemistry to quantum information technologies.

Plasmonic Hot-Carrier Engineering at Bimetallic Nanoparticle/Semiconductor Interfaces: A Computational Perspective.

Plasmonic catalysis employs plasmonic metals such as Ag, Au, Cu, and Al, typically in combination with semiconductors, to drive diverse redox chemical reactions. These metals are good at harnessing sunlight, owing to their strong absorption cross-sections and tunable absorption peaks within the visible range of the solar spectrum. Unfortunately, facilitating plasmon-induced hot-carrier separation and subsequently harvesting them to improve catalytic efficiencies has been a problem at monometallic particle-semiconductor interfaces.

Surface Functionalization of Nanocarriers with Anti-EGFR Ligands for Cancer Active Targeting.

Active cancer targeting consists of the selective recognition of overexpressed biomarkers on cancer cell surfaces or within the tumor microenvironment, enabled by ligands conjugated to drug carriers. Nanoparticle (NP)-based systems are highly relevant for such an approach due to their large surface area which is amenable to a variety of chemical modifications. Over the past decades, several studies have debated the efficiency of passive targeting, highlighting active targeting as a more specific and selective approach.

Total Synthesis of Discobahamin A and Putative Structure of Discobahamin B via an Isocyanide-based Macrocyclization Reaction.

We report in this paper the first total synthesis of discobahamin A, a 24-membered macrocyclopeptide containing an α-keto amide functional group. We assign the absolute configuration of 2-hydroxy-3-methylpentanoic acid (Hmp), the side chain capping the N-terminus of the macrocycle, as the (2S, 3S) stereoisomer. A novel macrocyclization strategy was developed, utilizing an intramolecular Passerini reaction between ω-isocyano aldehyde and acetic acid.

Structural basis of SIRT7 nucleosome engagement and substrate specificity.

Chromatin-modifying enzymes target distinct residues within histones to finetune gene expression profiles. SIRT7 is an NAD-dependent deacylase often deregulated in cancer, which deacetylates either H3 lysine 36 (H3K36) or H3K18 with high specificity within nucleosomes. Here, we report structures of nucleosome-bound SIRT7, and uncover the structural basis of its specificity towards H3K36 and K18 deacylation, combining a mechanism-based cross-linking strategy, cryo-EM, and enzymatic and cellular assays.

Asymmetric Synthesis of Inherently Chiral Tetraoxacalix[2]arene[2]pyridines via SAr-Based Cross-Cyclotetramerization.

Potassium phosphate-promoted cross-cyclotetramerization of 2,6-dichloro-3-nitropyridine 1 with resorcinol derivatives 2 gave rise to thermodynamically favored 1,3-alternate tetraoxacalix[2]arene[2]pyridines and kinetically controlled 1,2-alternate isomers. The kinetic product could convert into its 1,3-alternate conformational isomer by a macrocycle to macrocycle conversion pathway. Enantiomerically enriched C-symmetric inherently chiral tetraoxacalix[2]arene[2]pyridines were synthesized via a Cinchonine-derived chiral phase-transfer catalyst (PTC).