Themed collection 2019 PCCP HOT Articles

Two novel strategies for computational design and discovery of two-dimensional transition-metal free electro-catalysts are reviewed.

Periodical structures induced by pulsed lasers are a unique phenomenon when pulsed lasers irradiate on some material surfaces.

Ionic liquids (ILs) represent as solvents or co-solvents for protein stabilization and refolding. Thus, ILs are replacement to toxic organic solvents in chemical, biotechnology and biomedical applications.

Water is an intriguing substance. It shows sharp and reversible transitions between amorphous ices and, possibly, a liquid–liquid phase transition. Here, we discuss how this behavior is altered by the addition of solutes, such as salts and alcohols.

A cavity or excluded-volume structure best explains the experimental properties of the aqueous or “hydrated” electron.

Scanning probe microscopy techniques providing mechanistic insights into chemical reactions induced by localized surface plasmon on the basis of real-space observations.

This perspective summarizes our recent efforts in the application of gas-phase characterization methods to ligand-protected Au/Ag clusters chemically synthesized with atomic precision.

Transient reflection, photoreflectance and attenuated total reflection spectroscopy are developed to understand the ultrafast interfacial dynamics of solar conversion materials.

Ionic surfactants can be combined with various functional groups through electrostatic interaction, resulting in a series of thermotropic liquid crystals (TLCs).

We survey and assess current knowledge regarding the primary photochemistry of hydrocarbon molecules and radicals.

This article discusses applications of Bayesian machine learning for quantum molecular dynamics.

The electrocatalytic oxidation of water coupled to the reduction of carbon dioxide, to make carbon based products, or the reduction of protons to provide hydrogen, offers a sustainable route to generating useful fuels.

Two-dimensional oxide-on-metal materials: concepts, methods, and link to technological applications, with 5 subtopics: structural motifs, robustness, catalysis, ternaries, and nanopatterning.

This review summarizes the recent progress in chirality manipulation on 2D supramolecular crystal engineering.

We review recent efforts to model nonradiative recombination in semiconductor nanoparticles through conical intersections, focusing on the reasons for and consequences of the locality of such intersections.

We review the state-of-the-art of determining the electronic structure of nanocrystals in thin films by electrochemistry and emphasize the benefits of correlating electrochemical with spectroscopic methods to this end.

The pump pulse initiates intracluster charge transfer, creating transient nucleobase anions that model DNA damage pathways induced by low-energy electron attachment.

Electrochemical hydrogenation of a carboxylic acid using water as a hydrogen source is an environmentally friendly synthetic process for upgrading bio-based chemicals.

Quantum-chemical exciton analysis allows for quantitative, yet facile characterization of excited-state electronic structure and advanced multi-parameter benchmarking.

Non-covalent interactions as tools for modifying molecular properties.

The statistically corrected entropic component of effective molarity (EM_S*) complies with the “canonical” values expressed by the log plot of EM_S* vs. the number n of single bonds in the ring product.

A tunnelling controlled reaction is studied with semiclassical transition state theory, rationalising the results of experiment.

The structure and dynamics of the ordered CO ad-layer on MgO surfaces is determined by combining theoretical quantum-mechanical calculations and experimental infrared spectroscopic measurements.

Step-scan FTIR-spectroscopy reveals the bimolecular reaction in the ferrioxalate photochemistry, which builds the molecular-level foundation of the Hatchard–Parker actinometer.

Boron compounds usually exhibit Lewis acidity at the boron center due to the presence of vacant p-orbitals. But using Zintl-ion based groups (Ge₉Y₃, Y = H, CH₃, BO, CN), we can alter Lewis acid nature of B to a Lewis base.

We developed a multi-layer energy-based fragment (MLEBF) method within the many-body energy expansion framework.

Electron acceptors built upon the para-benzoquinone (pBQ) electro-phore are ubiquitous in nature.

We present the first quantitative measurements of hydrate formation probability, nucleation rate and growth on a water droplet suspended within a high pressure natural gas by acoustic levitation.

Dynamic Nuclear Polarization (DNP) can increase the sensitivity of Nuclear Magnetic Resonance (NMR), but it is challenging in the liquid state at high magnetic fields.

Weak n→π* and C–H⋯O interactions determine the structure of pyridine–acetaldehyde adduct. The n→π* distance oscillates with the methyl group internal rotation which acts as a sort of molecular balance to explore the n→π* interaction energy.

The symmetrically substituted diallyl disulfide adopts an asymmetric conformation in the gas phase, as observed in the rotational spectrum.

The structure of liquid water promotes the formation of ice in which the content of the cubic structure is higher than the content of the hexagonal structure.

The electrical double layer structure formed in an ionic liquid electrolyte was determined by combining the neutron reflectivity and deuterium labelling techniques.

Room-temperature triplet dynamic nuclear polarization (triplet-DNP) of nanocrystals dispersed in water is achieved for the first time.

In this communication the prediction of a two-dimensional carbon nitride allotrope (CN) featuring a 1 : 1 stoichiometry is considered.

An unusual blue shift in excimer fluorescence with increasing temperature was observed from a crystal with a discrete π–π anthracene dimer.

We present the photoelectron spectroscopy of the simplest Criegee intermediate, CH₂OO, close to the first ionization energy.

Tadpole-shaped single-chain nanoparticles (TSCNPs) are useful soft building blocks for nanotechnology composed of a flexible polymer chain tethered to an intramolecularly folded single-chain nanoparticle.

The facet-dependent strain effects on the hydrogen evolution reaction catalyzed by CoP were studied using density functional theory methods.

Here we report a combined use of THz-EPR and paramagnetic NMR spectroscopy for obtaining a detailed electronic structure of a high-spin cobalt(II) complex.

The ordering of endohedral clusterfullerenes Sc₃N@C₈₀ and YSc₂N@C₈₀ co-crystallized with Ni(OEP) and isolated complexes with Ni(OEP) have been investigated theoretically.

The quantum magnet KOsO₄ has been characterized by a combination of X-ray and neutron diffraction techniques. This represents the first structural and magnetic characterization of a simple Os⁷⁺, S = 1/2 oxide system.

In current materials science and technologies, surface effects on carrier and spin dynamics in functional materials and devices are of great importance.

We investigate the structural evolution of Cu(OH)₂ nanoparticle-derived electrodes under CO₂ electroreduction conditions and its effect on their electrocatalytic performance.

The activation of parahydrogen by a metal-free P–P biradicaloid leads to ¹H and ³¹P nuclear spin hyperpolarization.

Solubility parameter theories can be used to model the degree of polymer functionalization of MWCNTs in different solvent media.

The reaction between atomic oxygen and chloride anion in aqueous solutions exposed to cold plasma was investigated experimentally and computationally.

A time-domain laser experiment resolved spectra for benzene with single-MHz resolution, a 100-fold improvement on literature data.

Salts of fullerene C₆₀˙⁻ (1) and endometallofullerene Sc₃N@I_h-C₈₀˙⁻ (2) radical anions with the Bu₃MeP⁺ cation were obtained. These radical anions form Kagome lattices with equilateral fullerene triangles. The strong antiferromagnetic coupling of spins in 1 and 2 without magnetic ordering down to 1.5–1.9 K indicates strong spin frustration.

Evolution of water's structural dynamics from ambient liquid to supercritical dense liquid-like and dilute gas-like conditions.

The TiO₂–Pt–water interface is of great relevance in photocatalysis where Pt is widely used as a co-catalyst for enhancing hydrogen evolution in aqueous TiO₂.

Addition of NaNO₂ and/or NaNO₃ to the α-Al(OH)₃–NaOH–H₂O system leads to significant enhancement of α-Al(OH)₃ solubility.

We develop intuitive metrics for quantifying complex nucleating systems under confinement.

Our recently developed statistical model for molecular fragmentation (SMF) is used to study the decomposition of propane and to predict thermodynamically controlled yields of products as a function of excitation energy deposited into propane.

A liquid cell was designed for coherent diffractive imaging measurements at high tilt angles and tested at SACLA.

The iterative subspace algorithm to solve the CCSD complex linear response equations has been modified to include a core–valence separation projection step to overcome convergence problems. Illustrative results are reported for XAS, XCD, XES and RIXS.

A novel quantum-classical approach demonstrates that dynamic disorder, as induced by a liquid polar solvent, boosts RET efficiency.

Thermo-sensitive aqueous polymers undergo a coil-to-globule transition on heating, with drastic chemical and structural changes. We performed molecular dynamics simulations for PVCL in water to study the driving forces for the polymer's collapse.

Homochiral encounters of vicinal diols are blocked from relaxing to the heterochiral global minimum dimer structure in supersonic jet expansions.

Mass selected slow photoelectron spectra (SPES) of three boron-containing reactive species, BH₂, BH, and BF were recorded by double imaging photoion–photoelectron coincidence spectroscopy (i²PEPICO) using synchrotron radiation.

Solid methane doped by beryllium is superconducting at low pressures and its critical temperature can reach 30 K.

A detailed mechanism of TAM photolysis was studied and includes photoionization of the TAM radical with the formation of carbocation and further conversion of the carbocation under aerobic conditions into quinone-methide and under anaerobic conditions supposedly into an aromatic carbene.

SnC/As heterostructures in different configurations are extraordinary photocatalysts for water splitting even under infrared light.

Five tunnelling rearrangement pathways in water pentamer are responsible for the ground-state tunnelling splitting pattern of 320 states.

The thermal decomposition of VX has been studied computationally. The VX reactions have higher barriers and slower rates than the GB reaction. It is predicted that VX completely decomposes in 2 s at temperatures above 750 K.

A simple approach based on first principles leads to investigation of the origins of dendritic growth.

The synthesis of high quality MnBi₂Te₄ crystals as the first intrinsic antiferromagnetic topological insulator to unearth exotic topological quantum phenomena.

Photocatalytic materials are a potentially effective remediation technology for indoor air purification.

A disordered spacer layer (red) allows to form an ordered CO₂ layer (green), which is not influenced by the substrate.

In this work, we employ large-scale coarse-grained molecular dynamics (CGMD) simulations to study the three-dimensional line edge roughness associated with line and space patterns of chemo-epitaxially directed symmetric block copolymers.