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Hirudin is a widely studied model for folding of disulfide-rich proteins, which folds through a slow pathway with highly heterogeneous intermediates and scrambled isomers before it reaches its native state. Here the effect of native and non-native diselenide bridges on the kinetics, yield, and heterogeneity of hirudin folding are systematically explored.
Dioxygen protein sensors undergo structural distortions upon binding, but the role of heme distortion in allostery is unclear. Here heme distortion in a bacterial dioxygen sensor is studied using picosecond time-resolved electronic absorption spectroscopy and shown to control the allosteric equilibrium.
The crystallization processes of titanates are central to the fabrication of optical and electrical crystals and glasses, but their rich polymorphism is not fully understood. Here, authors identify when and how polymorphic selection takes place during the crystallization of an undercooled barium titanate melt using aerodynamic levitation, in situ time resolved high energy X-ray diffraction and ab initio molecular dynamics simulations.
Molecular dynamics simulation can reveal conformational dynamics of host-guest complexes, but simulating larger systems can be challenging. Here a modular approach allows simulation of a neocarcerand whose complexation is enabled by the guest-induced barrier for decomplexation.
Polymerisation induced self assembly can lead to unusual morphology and dynamics of resultant structures. Here the mechanism of the collective dynamics of a self-assembled polymer system under light irradiation, including self-replication, is eludicated.
Fatty acid membranes are implicated in several hypotheses about the origins of life, but whether their stability towards extremes of temperature, pressure, and ionic strength is sufficient to enable primitive biochemistry remains unclear. Here branched and linear alkanes are shown to stabilise a common model primordial membrane towards high temperatures and pressures
Cyclodiphosphazane macrocycles have demonstrated promising host-guest chemistry, but synthetic routes to highorder versions are lacking. Here the authors synthesise high-order oxygen-bridged phosphazane macrocycles via a modular cyclisation strategy.
Dearomatisation of indoles allows efficient access to indolines, but often is incompatible with electron-withdrawing substituents. Here a photoredox Giese-type dearomatisation of indoles yields 2,3-disubstituted indolines bearing electron-withdrawing groups.
DNA templating is a useful strategy to control the positioning and aggregation of molecular dyes on a sub-nanometer scale, but sub-angstrom control is desirable for the precise tailoring of excitonic properties. Here, the authors show that templating squaraine dyes functionalized with rotaxane rings promotes an elusive oblique packing arrangement and extended excited-state lifetimes.
Efficient autoxidation of organic compounds typically requires that they possess double bonds or oxygen-containing moieties, which is why alkanes were thought to contribute little to atmospheric organic aerosol formation. Here, mass spectrometry shows significant autoxidation of alkanes under both atmospheric and combustion conditions.
Portable liquid chromatography instruments enable a myriad of applications in field research. Here a handportable system incorporating a broadband absorption detector is used to separate and classify polycyclic aromatic hydrocarbons from environmental water samples based solely on spectral fingerprinting.
Recent works have highlighted the role of energy sources in driving nonequilibrium behaviours in chemical reaction networks. Here, the authors theoretically describe linear reaction networks with thermal gradients to highlight the basic rules governing most favourable states, relating them to kinetic and dissipation rates.
Despite strong demand for their clinical use, the synthesis of heparin oligosaccharides as anticoagulants remains challenging. Here, a mild and scalable formal synthesis of Fondaparinux pentasaccharide is presented through [Au]/[Ag]-catalyzed glycosidations.
Collision geometries are hard to control, making transition states in chemical reaction hard to study. Here the authors show that a linear transition state leads to formation of reaction product ‘knocked-on’ along the continuation of the direction of reagent approach.
Cyanide anions exist in interstellar space, but the vibrationally or electronically excited states above the electron autodetachment threshold of CN- are assumed to have no contributions to cosmic CN-. Here, the authors report long-lived, superexcited CN- from the dissociative electron attachment to cyanogen bromide.
Methacrolein oxide is one of the ozonolysis products of isoprene present in our atmosphere, but its relevance under humid conditions is not fully understood. Here, UV-vis spectroscopy and reaction kinetics studies show much longer lifetimes of anti-methacrolein oxide than previously thought, suggesting much higher steady-state concentrations and higher impact on the oxidation of atmospheric SO2.
Nano-sized catalysts are useful for electrocatalytic nitrogen reduction, but loading the particles on electrode substrates can limit catalytic performance. Here, the authors report nitrogen to ammonia electroreduction mediated by silver nanodots dispersed in an aqueous solution.
Molten salt electrolytes are widely used in energy storage and conversion, but our understanding of conductivity trends remains incomplete. Here, computational approaches are used to determine ionic electrical mobilities, local structures, and kinetics, unravelling the origins of conductivity in molten lithium halide salts.
Methyl vinyl ketone oxide is an important Criegee intermediate formed during the ozonolysis of isoprene, but its formation and resonance stabilization remain poorly characterized. Here, transient infrared spectroscopy of the syn-trans-conformer shows a stronger O‒O stretching band at 948 cm-1 that confirms the stabilization.
Under-coordinated corner and edge sites often dictate oxide properties, however, information about their atomic-scale structure and chemical nature is often missing. Here, a combined experimental and theoretical study of the ZnO(10-14) surface reveals stable, long-range ordered, non-polar facets of ZnO, with a high step-density and uniform termination.