Articles in 2020

Strong spin-spin interactions between surface-deposited magnetic molecules are desirable for quantum computing applications. Here the authors use scanning tunneling microscopy and spectroscopy to investigate the spin-spin interactions between neighbouring porphyrazine-derivatives on Au(111).

Compound crystallization is typically achieved from supersaturated solutions over time, through melting, or via sublimation. Here the authors show how a 10-fs laser pulse vaporizes a sample of thioglucoside without heating to produce a solvent-free single crystal from an undersaturated solution.

How small molecules could have accumulated within hypothetical protocells on the early Earth is an open question. Here automated microfluidic experiments provide evidence for abiotic accumulation of small molecules within cell-sized liposomes under hydrodynamic flow evoking a surface-mediated mechanism.

Two-dimensional covalent organic frameworks (2D COFs) are commonly synthesised through dynamic covalent chemistry, as it allows for thermodynamic ‘error correction' which enhances crystallinity. Here a crystalline 2D COF with amine and hydroxyl functional groups within the pores is synthesised through kinetically-controlled reactions.

High-nuclearity lanthanide clusters can exhibit interesting properties such as magnetism, but the mechanisms by which they assemble are poorly understood. Here, the formation of two dysprosium nanoclusters containing 30 or 60 atoms is followed over time by mass spectrometry and proposed to follow a seven-step assembly mechanism.

Strained alkenes are valuable reagents for rapid and selective labeling of biomolecules but may undergo side-reactions. Here direct excitation of an azobenzene generates a strained nitrogen-nitrogen double bond in situ which reacts with a photochemically-generated nitrile imine, allowing the labeling of live cells with spatiotemporal control.

To understand the self-assembly of semiconductor nanocrystals, the formation mechanism of two-dimensional superlattices needs to be deciphered. Here the authors observe lead selenide nanocrystal organization at the ethylene glycol-air interface combining in-situ grazing-incidence small -and-wide-angle X-ray scattering, X-ray reflectivity and analytical calculations to obtain a three-dimensional picture of the adsorption geometry of the nanocrystals.

The interface friction on solid surfaces is generally regarded as consistent with the wetting behaviour. Here the authors use molecular dynamics simulations and experiments to show that a small surface charge difference causes a change in the solid/water friction coefficient of over an order of magnitude, while the contact angles stay similar.

Tumor cells express high levels of integrins, which can be labeled using cyclic peptides, but selective labeling of target cells can be a challenge. Here in situ ligation of strongly binding cyclic peptides with weakly binding glycans allows discrimination of cancerous and non-cancerous cells which both express integrins on the surface.

Zeolites are industrially important heterogeneous catalysts with promising applications in acid-catalysed conversion. Here the relationship between the distribution of aluminium atoms in the ZSM-5 framework with the mechanism of ethanol dehydration is elucidated using FT-IR spectroscopy.

Flexible supercapacitors are versatile energy storage devices owing to their light weight, flexibility and high power density. Here a scalable, flexible, tubular supercapacitor possessing the diameter of an electrical wire is presented.

Although a geologically important mineral, the atomic-scale structure of ferrihydrite remains unresolved. Here the authors combine X-ray total scattering and reverse Monto Carlo to evaluate the two principal contending models, explicitly considering the material’s complex nanocomposite structure.

Ab initio prediction of aqueous pKa values is complicated by the presence of tautomerisable moieties. Here a model based on a small number of easily-calculated bond lengths is shown to accurately predict the pKas of 1,3-dicarbonyls including industrially significant herbicides.

The folding and conformational dynamics of proteins can be studied using optical tweezers with the aid of DNA handles. Here this assay is extended to simultaneously visualize the binding of complexing partners while monitoring the induced conformational changes on the protein.

Accurate prediction of protein-ligand binding is limited by our ability to model solvation. Here, in addition to protein and ligand information, density maps for hydration site occupancy are used to train a convolutional neural network in order to predict binding poses more accurately compared to common scoring functions.

Water trapped in nanoscale spaces shows unique properties due to confinement effects. Here the authors observe an exotic state of water in the hydrophilic nanopores of porous coordination polymers.

The origin of the excellent photoluminescence properties of embedded cesium lead halide perovskite nanocrystals remains to be fully understood. Here the authors visualize lattice alignments in dual-phase Cs₄PbBr₆ and CsPb₂Br₅ composites synthesized by sonochemistry and find that the CsPbBr₃ nanocrystals are responsible for the luminescence.

Cations influence the electrostatic, chemical and mechanical properties of lipid bilayers. Here, label-free second harmonic microscopy shows that cation-induced transient ordering of water also plays a role in driving membrane curvature fluctuations, linking molecular hydration to macroscopic properties.

Computational methods are a powerful tool for rapidly searching the optoelectronic property space of organic molecules. Here the property landscape of around 250,000 arenes and quinones is systematically explored, providing guidance for the design of new functional organic molecules.

Collision theory predicts the spectral peak of the sodium D-line to have a red-shift dependent on pressure and temperature. Using the serendipitous presence of sodium in octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine (HMX), the authors calibrate the D-line shift up to 1.5 GPa during deflagration.