ChemRxiv

Balancing bathochromic shift and narrowband emission remains a long-standing bottleneck for multiple resonance (MR) emitters, especially for indolocarbazole (ICz)-based systems with limited spectral tunability. Herein, the study proposes a synergistic regional aromaticity (SRA) strategy that harmonically integrates localized and delocalized aromaticity to address this trade-off, enabling the cons…

Intermetallic catalysts offer a unique platform for the hydrogenation reaction of acetylene, as their well-defined crystal structures and precise stoichiometry enable atomic-level control over active-site composition, geometry, and electronic structure. In ternary intermetallics, the addition of a third element in varying amounts can alter the crystal structure, thereby changing the stable crysta…

The electrochemical CO2 reduction reaction (CO2RR) relies on precise control of the catalyst and electrolyte environment so that an electric field from the Helmholtz-layer acts on reaction intermediates. Despite established benchmarking protocols, achieving reproducible performance remains difficult even for planar Cu under nominally identical conditions. We show that planar Cu operated at a fixe…

The tyrosine kinase expressed in hepatocellular carcinoma (TEC) family comprises five non-receptor tyrosine kinases – BTK, ITK, BMX, TXK, and TEC – with key roles in immune signalling. Although BTK and ITK have been extensively studied, selective inhibitors for TEC, TXK, and BMX remain scarce. Recently, we identified 7-azaindole-based covalent BMX inhibitors with potent inhibitory activity and ro…

The performance of Pt-based oxygen reduction reaction (ORR) catalysts is governed not only by adsorption energetics but also by the thermodynamic accessibility of near-surface structures and the resulting adsorbate coverage. Here, we combine a density-functional-theory-trained cluster expansion model with semi-grand-canonical and kinetic Monte Carlo simulations to resolve the structure–activity r…

The utilization of hot electrons surpasses the Shockley-Queisser limit, and fundamental understanding of hot electrons provides design principles for photo-energy conversion materials. Although the effect of donor-acceptor distance on electron transfer from the lowest excitonic state in quantum dots (QDs) to the acceptor has been studied (cold electron transfer), that of hot electron transfer sti…

Despite the long-standing recognition that ultrahigh molecular weight (UHMW) polymers give rise to chain-length-derived emergent material properties, the synthesis of functional UHMW polymers remains synthetically challenging due to oxygen-mediated radical quenching and chain growth limitations in conventional polymerization methodologies. In this study, we introduce an enzyme-deoxygenated photoi…

For nearly three decades, benchmarking density functional theory (DFT) functionals for zeolites and other tetrahedral frameworks has relied almost exclusively on average Si-O bond lengths. This practice assumes that accurate reproduction of bond lengths implies correct overall framework geometry. In this work, it is demonstrated that this assumption can be systematically misleading due to error c…

Surface nanobubbles are nanoscopic gaseous domains that reside at solid–liquid interfaces and exhibit anomalous stability against diffusive dissolution. Despite similarities in size and composition to bulk nanobubbles, the physicochemical mechanisms governing their interfacial persistence remain incompletely understood. Here, molecular dynamics simulations employing the polarizable SWM4-NDP water…

Methylorubrum species are prominent members of the plant phyllosphere, where they are exposed to fluctuating environmental conditions, including intense ultraviolet (UV) radiation. To mitigate such stressors, these bacteria commonly synthesise carotenoids as an oxidative protection. In this study, we investigated the carotenoid production of two closely related methylotrophic strai ns, Methylorub…

The intensity of a photon released from cyanine dye on a labeled oligonucleotide is heavily influenced by the adjacent sequence. This phenomenon could have profound effects in biotechnologies that rely on fluorescently labeled DNA based materials such as PCR, DNA-PAINT, and FISH. For instance, the selection of a DNA probe could result in a lower Signal-to-Noise ratio necessitating further data pr…

Strain-release cycloaddition chemistry of bicyclo[1.1.0]butanes (BCBs) has emerged as a powerful platform for the construction of saturated bridged frameworks. Despite remarkable advances in formal (2+2), (3+2), and (4+2) annulation reactions, higher-order annulation manifolds of BCBs remain under explored. Herein, we report the first formal (4+3) strain-release annulation of BCBs with indole-der…

Ion-selective ligand-functionalized polymer membranes (LFPMs) are promising materials for critical mineral (CM) industrial wastewater refining, but the effect of ligand identity on LFPM selectivity remains poorly described. We developed a dual–mode sorption (DMS) model for cation partitioning to quantitatively describe how ligand identity modulates cation selective partitioning in LFPMs. In this …

A chiral multiporphyrin receptor was prepared by covalent attachment of six zinc tetraphenylporphyrin units to a biotin[6]uril sulfoxide scaffold through flexible amide-linked side chains. In non-coordinating solvents, the conjugate adopts a propeller-like, C3-symmetric conformation in which three π–π-stacked porphyrin pairs are arranged helically around the chiral macrocyclic core, producing a s…

To have the most efficient simplified quantum chemistry method to compute excited states and response properties for all-atom quantum mechanical (AQM) methodologies, this contribution introduces the ηXsTD-DFT family of methods for which the exact integral simplified time-dependent density functional theory (XsTD-DFT) is adapted considering the resolution of identity (RI) approximation with a mini…

Polyglutamine (polyQ) diseases are neurodegenerative disorders caused by CAG repeat expansions and are characterized by a clinical pathogenic threshold typically observed between 35 and 39 glutamine residues. While this threshold is well established from genetic and clinical studies, its molecular and thermodynamic origin remains unclear. Here, we performed all-atom molecular dynamics (MD) simula…

Biology makes use of specialised proteins, the Aquaporins, to facilitate rapid water transport across cell membranes whilst strictly excluding salt, enabling maintenance of homeostasis. Whilst attempts have been made to use these properties in water purification and desalination, issues with stability, scalability, and cost have restricted their impact. Recent attention has focussed on building a…

Ilmenite, TiFeO 3 , is an earth-abundant mineral commonly used as a feedstock for TiO 2 , Ti, and Fe via reduction. One reduction product currently being explored is TiFe, an intermetallic compound capable of reversible, near-ambient hydrogen storage. Here, we use first-principles calculations coupled with CALPHAD thermodynamic modeling to evaluate how the kinetics and thermodynamics of point def…

Extreme fast charging in lithium-ion batteries is limited by their poor charge acceptance at high C-rates. In this work, we use overpotential component analysis to decouple ohmic, kinetic and transport related voltage losses during fast charging. The concentration gradients developed as a result of fast charging are identified as the primary culprit in poor charge acceptance, so we study carbonat…

Coarse-grained (CG) molecular dynamics enables the simulation of large biomolecular systems over extended timescales, but recovering atomistic detail from CG representations remains a significant challenge. Here, we present BackMapNet, a generalised and computationally e!cient framework for protein backmapping. The method adopts a staged reconstruction strategy for backbone and side-chain predict…