Themed collection 2021 PCCP HOT Articles

Attenuated total reflectance ultraviolet spectroscopy can facilitate access to ionic liquid/solid substrate interfaces in an electrochemical environment.

The transport of charge carriers throughout an active conjugated polymer (CP) host, characterized by a heterogeneous morphology of locally varying degrees of order and disorder, profoundly influences the performance of CP-based electronic devices.

This perspective provides accounts on recent studies regarding the role of vibrations toward energy transfers in photosynthetic complexes. The latest developments in simulation techniques are also reviewed with an outlook to future directions.

Rotational action spectroscopy is an experimental method in which rotational spectra of molecules, typically in the microwave to sub-mm-wave domain of the electromagnetic spectrum (∼1–1000 GHz), are recorded by action spectroscopy.

We review the past and present investigations on ZBBs, discuss the key problems and technical challenges, and propose perspectives for the future, with the focus on materials and chemistry.

High-resolution electron energy loss spectroscopy is a powerful tool to investigate surface excitations (vibrations of chemisorbed atoms and molecules, phonons, plasmons). Here, a perspective on the status and the future perspectives of HREELS is presented.

Graphene, due to its atomic layer structure, has the highest room temperature thermal conductivity k for all known materials and many excellent thermal properties.

The role of the intermolecular charge transfer state during ultrafast intersystem crossing in compact chromophores is revealed by spectroscopy and theoretical investigations.

The conversion of diffusive forms of energy (electrical and light) into short, compact chemical bonds by catalytic reactions regularly involves moving a carrier from an environment that favors delocalization to one that favors localization.

This Perspective discusses recent advances in constructing high fidelity diabatic potential energy matrices for nonadiabatic systems and the associated quantum dynamics.

Synchrotron-based X-ray spectroscopies have been key tools in the discovery, understanding, and development of battery materials. In this Perspective review, their state-of-the-art is highlighted, with special emphasis on future trends and needs.

Perspectives on advancing our understanding of two-dimensional materials using coherent anti-Stokes (CARS), stimulated (SRS) and tip-enhanced (TERS) Raman spectroscopy techniques.

In this perspective, we propose digital-intellectual materials design as the fifth stage of materials design and present its overview of microporous polymers.

Non-ideal aqueous electrolyte solutions have been studied since the start of the application of thermodynamics to chemistry in the late 19th century.

This perspective highlights the significance of regulating Li₂S deposition and the related methods in improving the performance of lithium–sulfur batteries.

Microscopic origins of transcriptional bursting phenomena are discussed from the physical–chemical point of view.

Due to their unique reversible polarization, 2D ferroelectrics are promising for nanodevice applications in ferroelectric field effect transistors, diodes and tunnel junctions.

This Perspective provides a critical summary of the current state of the art in the synthesis and properties of polyheptazine single-layer carbon nitride (SLCN).

Kinetics of triplet–triplet annihilation photon upconversion is organized from the basics for non-experts and experts. From self-consistent analyses of the tangled photophysical events, many important and useful relations are derived and summarized.

Representative methods of surface-selective phase-sensitive sum frequency generation spectroscopy are reviewed in terms of interferometer implementation for optical heterodyne detection.

A general “four-pillar strategy” (theory, simulation, machine learning and augemented reality/virtual reality) to integrate computational and experimental spectroscopy.

Modern multireference methods open up the possibility to treat complicated transition metal systems on a physically sound basis.

Two views of the computed electrostatic potential on the 0.001 au surface of 2,4,6-trifluoro-1,3,5-triazine. Red is the most positive color range, while blue is the most negative.

Recent developments of electron spin dynamics in organic molecular systems studied by time-resolved electron paramagnetic spectroscopy are summarized.

Computational approaches for analyzing the homogeneous nucleation of sheared simple liquids are reviewed. We examine underlying mechanisms and effects of flow. The experimental scope and sheared nucleation of polymers and glasses are also covered.

This prospective provides a brief overview of the working principles of various optoelectronic devices and the structure–property relationships in phenothiazine.

A catalog summary and capacity comparison of ECESDs.

How solvation obstructs charge sharing and limits the size of covalently bound core anions in clusters.

Machine learning algorithms can facilitate the reaction prediction in heterogeneous catalysis.

Pulsed laser strategies (i.e. pulsed laser ablation and fragmentation in liquid) have been reviewed with a focus on the synthesis and processing of amorphous metal nanoparticles. The possible formation criteria and mechanism have been discussed.

We review new light source developments and data analysis considerations relevant to the time-resolved photoelectron imaging technique. Case studies illustrate how these themes may enhance understanding in studies of excited state molecular dynamics.

In this Perspective, the authors review the interplay between structure and charge-transport properties of mesoporous metal oxides, with an emphasis on applications in electrochemical energy storage, catalysis and gas sensing.

The theoretical description of dissociative chemisorption of isolated molecules on metal surfaces is discussed. Emphasis is put on methods that deliver chemical accuracy for the dissociative chemisorption probability S₀, so that Δ ≤ 1 kcal mol⁻¹.

We shed light on the compositional, surface engineering and crystallization kinetics manipulations for FAPbI₃ followed by a proposition for unified testing protocols in order to scale-up the solar cells from the lab to the market.

A review on ultrafast photoinduced processes in molecule-based magnets with an emphasis on Prussian blue analogues.

This work highlights the challenges and problems when modelling inorganic–organic interfaces and provides practical tips and suggestions for efficient calculations.

In the elastic regime, GIFAD is equivalent to TEAS with an effective energy E_⊥ between 1 meV and 1 eV providing a high sensitivity to topology and to attractive forces. The inelastic regime merges to the classical limit and is still in development.

In this Perspective we present the state of the art of creating mixed metal clusters in the superfluid droplet environment and their investigation through a successful interplay between experimental characterization and theoretical modelling.

Solid-state synchronous luminescence spectroscopy (SS-SLS) is a novel high-resolution method to study the absorption and emission of light, electronic structure, and reactions of nanocrystalline semiconductors.

A mini-review of microfluidic technologies for the generation and manipulation of biomimetic nano-assemblies, including perspectives for future research directions.

Recent progress in the development of thermal interface materials.

Review of principles and limitations of viscosity models for ionic liquids and their mixtures focusing on the use of inappropriate mixing rules for molten salts.

The correlation between electronic densities and active molecular vibrations drives the spin–vibronic mechanism of ultrafast decays in coordination chemistry.

Thermal enhancement of upconversion luminescence in lanthanide-doped nanocrystals are summarized and the enhancement mechanism is discussed in detail with a fresh perspective.

We present a method based on Ampère–Maxwell's integral law for calculating strengths of magnetically induced ring currents.

A threshold photoelectron spectrum of HBNH is reported, recorded using synchrotron radiation.

CRISPR-Cas12a target search and cleavage on force-stretched λ-DNA using optical tweezers.

Direct comparison of bandgaps of GaSb zinc blende and wurtzite polytypes (0.75 and 0.84 eV, respectively) by means of valence electron energy-loss spectroscopy (VEELS) in a transmission electron microscope (TEM).

The parameters of the (3,−3) critical point in the localized orbital locator topology reflect the changes in the size, density and electron energy of the nitrogen lone pair and correlate with the complexation energy.

In this report, the strong-dependence of low-frequency (terahertz) vibrational dynamics on weak and long-range forces in crystals is leveraged to determine the bulk magnetic configuration of iron phosphate – a promising material for cathodes in lithium ion batteries.

We have developed a new NMR spectroscopic method to rigorously quantify the interaction between a low water-solubility drug and its target protein by accurate estimation of precipitation using quantitative NMR (qNMR).

The high catalytic activity of RuO₂(110) towards the oxygen evolution reaction is explained theoretically by considering an alternate reaction pathway for this catalyst.

Ehrenfest dynamics study describing the photoinduced charge transfer in metalloid gold nanoclusters.

The large vibrational deactivation, experimentally found in low-energy O + N₂ collisions, is quantitatively reproduced only using a vibronic mechanism.

Steric effects on solute diffusion in flexible polymer gels can be described by a very simple mathematical rule.

This work presents a small matrix decomposition of the modular path integral for spin arrays or molecular aggregates, which leads to an iterative treatment with respect to the units that comprise the system and the propagation time.

The dissociation process of spherical sII mixed methane–propane hydrate particles in liquid hydrocarbon was investigated via microsecond-long molecular dynamics simulations.

A hotter paramagnet relaxes to a ferromagnetic state faster than a colder one, resembling the counter-intutive Mpemba effect in water-ice transition.

Quadruple bonding in heavier main group elements is not known albeit having four valence orbitals accessible for bonding.

We report different polaron trap depths in hematite and akageneite measured by transient XUV reflection–absorption spectroscopy.

In sulfur containing liquid crystal dimers we find that at the transition to the N_TB phase the positional correlation length drops. The nanoscale periodicity was also observed in the upper range of a smectic phase that forms below the N_TB state.

A prior dealumination was proven effective to modify the structure of the initial FAU and consequently facilitate its conversion to the AEI. Based on the obtained results, we proposed a scheme of the interzeolite conversion from FAU to AEI.

Four different conformers have been revealed in the supersonic expansion for the amino acid and supramolecular synthone L-DOPA (see figure), rejecting its previously reported conformational restriction. The role of the N-H···π interactions have been thoroughly described.

Natural reaction orbitals, a new molecular orbital analysis method, enable automated extraction of reactive orbitals and analysis of electron transfer.

TPES spectroscopy is used to unveil the complex vibronic structure of 9-methyladenine cations.

A new method is proposed to record photoelectron spectra based on the well-established pulsed-field-ionization zero-kinetic-energy photoelectron spectroscopy technique and inspired by the data treatment employed in slow photoelectron spectroscopy.

Topological effects are key in driving nano-bio interface phenomena: the symmetry of the lipid membrane (cubic or lamellar) dictates the interaction mechanism, while nanoparticles shape (sphere or rod) modulates the interaction strength.

Electrolyte buffering species are shown to act as oxygen donor in the carbon monoxide electrooxidation

Significant differences are observed in liquid-water's lowest electron binding energy with increasing solute concentration in archetypal aqueous solutions. For NaI_(aq) and TBAI_(aq), the energy changes extend to +0.3 eV and −0.7 eV, respectively.

Emergent calcium battery electrolytes in ethereal solvents exhibit concentration-dependent ion correlations involving significant second-shell interactions. These interactions have a strong influence on both conductivity and metal cycling efficiency.