Research articles

Stacking aromatic molecules through π–π interactions is a useful strategy to create ordered layers of small molecules, but the weak and non-directional nature of these forces creates a challenge in achieving long-range structural ordering. Here, a rigid molecular template that facilitates the creation of a non-collapsible void between two parallel π-faces is designed, and a central N–H motif is shown to increase the thermodynamic stability of self-dimerized assemblies and host–guest complexes via N–H…N hydrogen bonds.

Tropolones harbor a non-benzenoid aromatic scaffold and display a wide-range of bioactivities, however, the cyclic derivatives of aminotroponimines remain underexplored. Here, the authors develop a one-pot synthesis of N^Alkyl/C^Aryl-substituted cyclic-aminotropiminium carboxylate derivatives with promising anticancer properties.

Organic thin film transistors are potent sensors, but their charge transport layers (CTL) need to be carefully designed to reach desired analyte responses. Here, the authors show that zinc phthalocyanine sensors with a CTL thickness of 200 Å and low crystallinity are most susceptible to physical alterations upon exposure to analytes, resulting in large electrical changes and a low detection limit of 40 ppb for Δ9-tetrahydrocannbinol vapor.

On-surface synthesis is a useful tool to produce extended macrocyclic structures with atomic precision, with only one type of macrocycle typically formed through on-surface coupling reactions. Here, distinct domains of four-, six- and eight-membered tetraphenylethylene-based macrocycles are synthesized on Ag(111) as segregated large-area mono-component crystals.

Controlling the thermal expansion of a material is of importance for material longevity in applications with fluctuating temperatures. Here, the impact of nanoparticle loading on the thermal expansion behaviour of a pillared metal–organic framework is explored using variable temperature powder X-ray diffraction, and a significant reduction in the thermal stress is observed.

Hydroamidation of unactivated alkenes is an efficient way to introduce nitrogen-based functional groups to alkenes, however the regioselectivity requires directing groups. Here, the authors report the ligand-controlled NiH-catalyzed anti-Markovnikov intermolecular hydroamidation of unactivated alkenes with dioxazolones for the direct synthesis of N-alkyl amides.

Infrared spectroscopy-based diffraction tomography has a high potential to be used for 3D reconstruction of intact samples, however, the inverse problem is highly non-linear and remains challenging. Here, the authors solve full-wave inverse scattering problems using deep convolutional neural networks and perform 3D spectral reconstruction by diffraction tomography from scatter-distorted IR spectra.

Studies of ion-specific effects on oligopeptides are largely dependent on model peptides and experimental sensitivities. Here, the authors study the ion-specific effects on L-alanyl-L-alanine by combining dielectric relaxation, ¹H-NMR and 2D infrared spectroscopy.

Mass spectrometry is a powerful approach for untargeted lipidomics, however, the unambiguous determination of double bond positions remains challenging. Here, the authors present an approach for double bond position-resolved untargeted lipidomics using a combination of oxygen attachment dissociation and computational mass spectrometry to accurately annotate the biologically relevant lipidome.

Tuning the metal core and ligand environment of atomically precise nanoclusters enables the correlation of structural and electrocatalytic properties at an atomic level. Here, single-atom doping and ligand tuning of atomically precise copper clusters is shown to be an effective route to tuning CO₂ electroreduction activity and selectivity.

Several essential brain micro-environments like pH, salt, and metal ions play a vital role in modulating the amyloid-ß fibrillation, however, the cooperative modulation of these variables remains poorly understood. Here, the authors investigate multivariate effects of pH, ionic strength, and Zn²⁺ ions on Aß₄₀ peptide fibrillation.

Metal-organic frameworks with desirable properties can be designed through careful choice of linker and node combinations, but achieving the synthesis of a desired MOF is complex and dependent on many experimental variables. Here, a genetic algorithm combined with experimental feedback and confirmation is used to obtain the optimal microwave-assisted synthesis conditions for a porphyrin-based aluminium MOF (Al-PMOF), achieving excellent crystallinity and a close to 80% yield in only the 2^nd generation.

The AAA+ ATPase p97 protein is thought to be a potential anticancer target, but direct targeting on its ATPase function has not proven to be a successful strategy in clinical trials due to lack of selectivity. Here, the authors use biolayer interferometry-based fragment screening to identify ligands for the development of protein-protein interaction inhibitors by targeting the SHP-motif as a cofactor binding site in the N-domain of p97.

The gem-difluoroethylene moiety is considered as a valuable building block in organic synthesis, but methods to introduce it into small molecules are generally limited to specific substrates. Here, the authors demonstrate that a gem-difluorovinyl iodonium salt enables the direct difluoroethylation reactions of a diverse range of N- and O-nucleophiles.

Heterodehydrohelicenes exhibit attractive chiroptical properties, but their direct construction by asymmetric synthesis remains very challenging. Here, the authors report the electrochemical sequential synthesis of azaoxadehydro[7]helicenes from arenols through oxidative hetero-coupling followed by dehydrative cyclization and intramolecular C–C bond formation.

Combining conjugated polymers with transition-metal-based metal-organic frameworks offers an opportunity to produce efficient photocatalytic materials. Here, exposed active sites and efficient charge transfer lead to hydrogen evolution rates of up to 2438 µmol g⁻¹ h⁻¹ for composites of anisotropic phenanthroline-based ruthenium polymers grafted on titanium-based MOFs.

Indistinguishable hydrogen nuclei exhibiting long-time and large-scale collision and repulsion dynamics are inherently hard to accurately describe. Here, the authors develop a non-empirical quantum molecular dynamics method that enables real-time molecular dynamics simulations of hydrogen molecules with nuclear quantum rotation satisfying the nuclear spin statistics of the quantum rotor.

Oriented attachment of nanoscale building blocks into hierarchical structures offers vast opportunities to engineer nanomaterial structure-property relationships. Here, the misalignment of crystal plane orientations between iron oxide nanoclusters is shown to govern their magneto–optical properties and magnetic heating functions.

Chromia is an important additive used in uranium dioxide fuel fabrication, but its incorporation mechanism is still not fully understood. Here, the authors use X-ray absorption spectroscopy, including both near edge and extended fine structure regions, to resolve the local structure and valence state of chromium, as divalent, in uranium dioxide.

High-resolution molecular spectroscopy provides invaluable insight into the quantum properties of molecules, but high-resolution rovibronic spectroscopy has largely been limited to relatively small systems owing to the difficulty in preparing translationally and rotationally cold samples for large and complex systems. Here, the authors demonstrate that buffer-gas cooling may be an effective strategy to obtain high-resolution rovibronic spectroscopy results for large gas-phase molecules.