Themed collection 2022 PCCP HOT Articles

Some key articles that have recently shown the potential of self-assembly for artificial photosynthesis are discussed; it is shown that emerging properties derived from self-assembly can be useful for designing efficient photocatalytic systems.

The enthusiasm for research on liquid crystal random lasers (LCRLs) is driven by their unusual optical properties and promising potential for broad applications in manufacturing, communications, medicine and entertainment.

The mechanics-based design of lithium-ion batteries during the preparation stage and the cycling stage is reviewed. The general problems currently being faced are summarized, followed by the outlook of possible solutions.

In this paper, the history, present status, and future of density-functional theory (DFT) is informally reviewed and discussed by 70 workers in the field, including molecular scientists, materials scientists, method developers and practitioners.

Two roads in the electric–dipole revolution in chiral measurements.

Lithium (Li) metal is strongly considered to be the ultimate anode for next-generation high-energy-density rechargeable batteries. Carbon materials and their composites with excellent structure tunability and properties have shown great potential applications in Li metal anodes.

In this perspective article, main trends of angle-resolved molecular photoelectron spectroscopy in the laboratory up to the molecular frame, in different regimes of light-matter interactions, are highlighted with emphasis on foundations and most recent applications.

The methodological advances made in recent years have significantly extended the range and dimensionality of noncovalently bound molecular complexes for which full-dimensional quantum calculations of their rovibrational states are feasible.

In this review, we discuss the recent progress in developing geminal-based theories for challenging problems in quantum chemistry.

Biexcitons dominate the optical responses of lead halide perovskite nanocrystals and provide a unique way to control and improve the optical gain.

A comprehensive perspective of the n → π* non-covalent interaction obtained using various experimental and theoretical approaches is presented.

Gold nanobipyramids (AuBPs) with narrow size distribution and high monodispersity possess more advantageous plasmonic properties and have been a promising template to fabricate anisotropic multi-metallic nanostructures.

Differential Dynamic Microscopy (DDM) is a relatively new technique which measures the dynamics of suspended particles using a dynamic light scattering formalism.

This article provides atomistic insight into the dynamic microsolvation processes occurring in differential mobility spectrometry (DMS), which can be used to (1) reproduce an ion's DMS behaviour, and (2) predict an ion's condensed-phase properties.

In this perspective, we discuss the current state of the art of time-resolved photoelectron spectroscopy to probe nonadiabatic dynamics, including ab initio approaches for its simulation and new experimental efforts.

Velocity correlated cluster emission (VCCE) effect: all large clusters emitted from a given target following a fullerene ion impact move with nearly the same velocity. A hot moving precursor is proposed as the source of the outgoing clusters.

Mixed ionic-electronic conduction is a critical feature in a wide range of emerging electrochemical devices based on conjugated polymers exploiting transport, coupling, and charge carrier concentration modulation of both electronic and ionic charges.

The efficiency of a 2D photocatalyst is largely dependent on the excited state charge carrier behavior at short time scale, which can be accessed and used for the betterment of the photocatalyst via only transient absorption spectroscopy.

This perspective demonstrates the novelty of the understanding, fabrication, notification and outlook of the free-standing cathodic interlayer in Li-S batteries.

Paramagnetic NMR observables provide accurate long-range structural information and act as a loupe on the metal coordination site.

Many experiments that utilize beams of incident atoms colliding with surfaces as a probe of surface properties are carried out at large energies, high temperatures and with large mass atoms.

In this article, we review the theoretical methods used to simulate and analyze grazing-incidence fast atom and molecule diffraction, focusing on their weaknesses and strengths, as well as the theoretical challenges that still need to be addressed.

Anharmonic effects are important in adsorbed molecules even as harmonic calculations continue to dominate computed vibrational spectra in applications. We consider perspectives of application of anharmonic methods to adsorbed molecules.

Nanoheaters: FCC solid spherical nanocrystal assemblies either dispersed in solution or internalized in tumor cells.

Green's function approaches facilitate efficient and accurate calculations of X-ray spectra that include key many-body effects.

This perspective article reviews specific challenges associated with photoemission spectroscopy of bulk liquid water, aqueous solutions, water droplets and water clusters.

Deep eutectic solvents (DESs) have emerged as a new class of green, designer and biocompatible solvents, an alternative to conventional organic solvents and ionic liquids (ILs) which are comparatively toxic and non-biodegradable.

An overview of the OCEAN code for calculating near-edge X-ray spectroscopy, including X-ray absorption and resonant inelastic X-ray scattering, using the Bethe-Salpeter equation approach.

Objections are raised against the straight-line behavior of the energy for fractional electron number and its basis in thermodynamical (grand canonical ensemble) considerations. It is not “the exact DFT for noninteger electron systems”.

This perspective reviews the historical explanations for specific ion effects, and explores the frontiers of the field before summarising its challenges and opportunities.

All-atom simulations can provide molecular-level insights into the dynamics of gas-phase, condensed-phase and surface processes.

Free-base porphyrins on TiO₂(110) anchor to O_br rows, where they capture diluted hydrogen underneath and favour outdiffusion of Ti interstitials by self-metalation; Ti metalated species may also capture oxygen from hydroxyl adsorbates on Ti_5f rows.

The first theory blind challenge addressing the effect of microsolvation on water vibrations is launched.

A tabletop pulsed laser can launch a hypervelocity flyer plate to create high temperatures and pressures in a nanosecond in an array of solid or liquid samples.

Computational modelling complements experimental biochemical studies on DNA adduct mutagenicity by providing structural insights for a diverse set of lesions resulting from tobacco products.

This perspective article reviews experimental and theoretical works where rare gas clusters and helium nanodroplets are used as a nanoreactor to investigate chemical dynamics in a solvent environment.

Small-molecule materials showing ambipolar transistor properties are reviewed.

The study of reactions relevant to heterogeneous catalysis on metal clusters with full control over the number of constituent atoms and elemental composition can lead to a detailed insight into the interactions governing catalytic functionality.

This personal account describes my motivation for each previous subject on metal nanoclusters, what type of research I want to perform, and how I consider the outlook of the field.

We summarise methodologies, challenges and opportunities for theoretical modelling to advance current understanding of electromagnetic bioeffects for biomedicine and industry.

Electron diffraction of clusters doped in superfluid helium droplets is an in situ technique for cluster synthesis and atomic structure determination. Both neutral and ionic nanoclusters can be investigated with proper care of the helium background.

A new combination of coarse-grained modeling and finite element calculations enable rapid and accurate characterization of DNA transport through nanostructures of diverse geometries.

Palladium clusters enhance the hydrogen storage of nanoporous carbons.

Photoelectron spectroscopy has evolved into a powerful tool for physical chemistry and molecular physics. Some recent examples are highlighted in this perspective.

In this article, we review recent first principles, anharmonic studies on the molecular vibrations of gaseous formic acid in its monomer form.

Graphene oxide consists of diverse surface chemistry which allows tethering GO with additional functionalities and tuning its intrinsic properties. This review summarizes recently advanced methods to covalently modify GO for specific applications.

Photoelectron–photoion(s) coincidence, PEPICO, experiments with synchrotron radiation have become one of the most powerful tools to investigate dissociative photoionization thanks to their selectivity.

This review provides an overview of the significant progresses that occur on lithium metal anodes for lithium metal batteries. Some modification strategies and in situ characterization approaches are discussed.

Polymer nanodielectrics with high breakdown strength (E_b), high energy density (U_e) and low energy loss have great potential to be used as capacitive energy storage materials of high-voltage film capacitors in modern electrical and electronic equipment, such as smart grids, new energy vehicles and pulse powered weapons.

In this review, we take heteroatom-bridged heteroaromatic calixarene, cucurbituril and cyclodextrin as examples, and summarize the recent progress in the molecular recognition and self-assembly of macrocyclic host molecules by multiscale modelling.

Minireview on ultrasmall subnanometer clusters driving chemical transformations in heterogeneous catalysis, electrocatalysis and photocatalysis.

The shortest reaction path is not always that of lowest activation energy.

This tutorial review presents the theory, models, and protocols for the simulation of electrochemical properties of nanoelectrocatalysts with complex morphologies using the finite element method.

We put a spotlight on IR spectroscopic investigations in materials science by providing a critical insight into the state of the art, covering both fundamental aspects, examples of its utilisation, and current challenges and perspectives focusing on the solid state.

First-row TMOs have remarkable properties that are appealing in materials design for technological applications. Their electronic structure can be modelled with DFT, but this requires careful considerations due to strong correlation effects of 3d orbitals.

This tutorial review provides an introduction to multiscale modelling of complex chemical, physical and biological processes through case studies, aimed at beginning researchers and more senior colleagues who are changing direction to focus on multiscale aspects of their research.

Unprecedented intermolecular aggregation of pyrene at micromolar concentration level within neat lanthanide metal based-deep eutectic solvents.

The preparation of graphdiyne via the self-coupling reaction of hexakis(bromoethynyl)benzene (hBEP) with alkynyl bromide groups is reported, where the reaction can proceed moderately in 12 h at room temperature.

Despite the expected influence of heteroatom substitution in carbon materials, no technologically significant effect was identified for H₂ physisorption energies.

Recent developments in new synthesis techniques have allowed the production of precise monodisperse metal clusters composed of a few atoms. The study of these clusters represents a challenge for theoretical investigations.

The controversial tetrahedral intermediate of the reaction between acetyl chloride and ethanol was detected using novel methodology. The results demonstrate that the reaction proceeds via an addition/elimination mechanism.

Efficient prediction of the partition coefficient (log P) between polar and non-polar phases could shorten the cycle of drug and materials design.

Quantum chemical calculations show that ligated metal oxide anions can convert methane to methanol efficiently and facilitate the release of methanol from the metal center preventing its further oxidation.

A chemical reaction between epoxy and amine compounds at an outermost solid interface was studied by sum-frequency generation spectroscopy, X-ray and neutron reflectivity and a full atomistic molecular dynamics simulation.

The TiO₂-nanoparticle scaffold suppresses ion accumulation in mesoporous perovskite solar cells by reducing the electrostatic interaction between the conductive substrate and the perovskite active layer.

Water devoid RF pulses designed by an evolutionary algorithm and AI improve solvent suppression and increase the NMR spectra sensitivity.

The film-growth model predicts a morphology-driven dual-layer structure due to slowing down of electron diffusion through the SEI.

Helium atom scattering experiments on a “holey” silica bilayer film reveal that the bending rigidity of the material, extracted from phonon dispersion curves, decreases with decreasing material density.

A complete core–shell B₉₆ is highly symmetric (T_h) and stable, and exhibits a superatomic electronic configuration and spherical aromaticity.

Nucleophilicities N_R–B of molecules R–B (R = F, Cl, Br, I, CN, NC, CH₃, SiH₃, CF₃, H) are determined from the equilibrium dissociation energies D_e of 70 hydrogen-bonded complexes R–B⋯HX (X = F, Cl, Br, I, HCN, HCCH, HCP).