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The ability to precisely engineer nanostructures is crucial for a wide range of applications in areas such as electronics, optics, and biomedical sciences. Here, the authors present an approach for templated growth of gold nanoparticle assemblies leveraging the weak van der Waals forces between metal atoms and small molecular templates in superfluid helium.
Large classes of metal clusters are expected to have dipole-allowed electronic transitions in the near-infrared, but precise experimental characterization of such low-lying states is lacking. Here, the authors probe cationic cobalt clusters of 4 to 15 atoms using IR photofragmentation spectroscopy with krypton as a messenger atom to show that low-lying electronic excited states are responsible for the size-dependent radiative decay of these highly excited clusters.
Photolysis can induce the homolytic cleavage of chemical bonds through the excited state under specific irradiation wavelengths, producing free radical species. Here, the authors report the photoinduced homolysis of electronegative interelement bonds (N–Cl, N–F, and O–Cl bonds) using light with wavelengths longer than that predicted for the S0–Sn or S0–Tn transitions, initiating diverse radical reactions.
Data-driven computational methods have demonstrated promising potential in predicting compound activities from chemical structures, however, unbiased practical applications remain challenging due to the lack of proper benchmarking methods. Here, the authors develop a benchmark termed CARA to eliminate the biases in current compound activity data by using new train-test splitting schemes and evaluation metrics, revealing accurate and informative model performances.
Membranization of coacervate microdroplets can stabilize coacervates and enable the construction of hierarchical protocells by using various interfacial layers. Here, the authors demonstrate the modulation of interfacial membrane fluidity and thickness of dextran-bound coacervate protocells by adjusting the molecular weight of dextran or through enzymatic hydrolysis, achieving control over colloidal stability, interfacial molecular transport and cell-protocell interactions.
Enzymes play an important role in organic synthesis thanks to their high selectivity, however, such selectivity limits their substrate scope and hampers their wide application. Here, the authors report an approach to rationally select enzymes with proposed functionalities based on sequence analysis, exploring the substrate scope of 4-phenol oxidases by in silico sequence-function correlation analysis.
Ion channels are known to be important actors in cellular signaling, and their functions correlate to their conformational states, however, detailed function–conformation relationships remain underexplored. Here, the authors use a molecular modeling-based approach to assess water and ion conductivity along with pore hydrophobicity and residue packing to characterize the ion channel structural intermediates, revealing three major states of vanilloid-subfamily transient receptor potential channels.
Droplet interface bilayers can be used as a model of artificial membranes for synthetic biology and drug delivery applications, however, their accessibility using non-invasive techniques remains challenging. Here, the authors develop an in-situ bilayer manipulation of encapsulated droplet interface bilayers in hydrogel capsules, generated by high-order emulsification in monolithic 3D-printed microfluidic devices.
Extraterrestrial carbon gives insights into the origin of life and processes that took place billions of years ago in our solar system. Here, the authors provide an overview of what is known and of unanswered questions with a meteoritical focus.
Quasi-liquid layers on the surface of water ice significantly affect its distinctive chemical and physical properties, but a molecular-level understanding of these heterogeneous layers is missing. Here, the authors use molecular dynamics simulations and machine learning analyses to show that the quasi-liquid layers resemble supercooled water.
Brønsted basicity can be greatly enhanced by the mechanical entanglement of two or more interlocked molecular subunits within catenanes and rotaxanes. Here, the authors discuss the development of such mechanically interlocked superbases, and outline challenges and opportunities for future directions of research.
Optical filter materials are used across scientific disciplines for imaging or spectroscopy, but inexpensive and eco-friendly alternatives remain underexplored. Here, the authors exploit the localized surface plasmon resonance of metal nanoparticles embedded in edible gelatine for modular light filters working in the ultraviolet to near-infrared range.
Peptide-like foldamers are known to be controlled by amide backbone hydrogen bonding, however, the influence of functional groups forming individual hydrogen-bond networks remains underexplored. Here, the authors report peptide-like α-γ heterofoldamers consisting of alternating α,β,γ-triamino acids, forming ordered secondary structures and folding in both organic and aqueous environments.
Ultra-high molecular weight (UHMW) polymers exhibit exceptional mechanical properties and have found extensive applications, however, it remains challenging to produce them with a low dispersity. Here, the authors develop ultrasound-initiated copolymerization of diverse monomers, generating UHMW polymers with low dispersity within 15 min.
Solution NMR spectroscopy provides rich structural information on biomolecules, however, its resolution becomes limited when molecular size increases, due to short-lived nuclear magnetic responses to electromagnetic radiation. Here, the authors sustain long-lived coherences for the aliphatic protons of glycine residues within protein lysozyme, yielding substantial through-space magnetization transfers, and mapping interacting atoms in the protein structure.
Plasma-activated chemical transformations promise efficient syntheses of vital chemicals such as ammonia, however, reaction pathways are often unknown and quantum state-resolved information is lacking. Here, the authors use quantum cascade laser dual-comb spectroscopy to study non-thermal plasma-activated ammonia synthesis with rotational and vibrational state resolution, quantifying state-specific number densities via broadband spectral analysis.
Tandem mass spectrometry spectra contain structural information of analyzed small molecules, however structural annotation and prediction from MS spectra remain challenging. Here, the authors combine the fragmentation tree models with a deep-learning transformer module, to annotate the fragmentation peaks and generate de novo molecular structures from a low-resolution mass spectrometer.
The anthraquinone process is currently the predominant method for large-scale H2O2 production, but the reaction’s high energy consumption and hazardous waste generation spur the search for alternatives. Here, the authors investigate the two-electron oxygen reduction reactivities of metal-free non-porous, micro-, and mesoporous carbon catalysts to elucidate the impacts of porous structures, finding mesoporous structures show the highest H2O2 production selectivity.
Graphene quantum dots have versatile properties, but their luminescence can be quenched when the dots aggregate. Here, the authors immobilize graphene quantum dots on 2D MOF sheets and demonstrate their photoluminescence in suspension and as a dry powder, and show their application in copper ion sensing.