Themed collection 2020 PCCP HOT Articles

Anion PE spectroscopy and DFT calculations reveal molecular and electronic structural features of cluster models for catalysis.

This article presents development of first principle based Beyond Born–Oppenheimer theory and its applications in conjunction with Jahn–Teller theory.

DFT calculated structures, vibrational frequencies, and energies provide insights into the reaction/proton pumping cycle of cytochrome c oxidase.

Solvation effects are essential for defining the shape of vibrational circular dichroism (VCD) spectra.

Halide perovskites possess unusual phonon and thermal properties, which lead to unique thermo-optical responses very different from those of conventional inorganic semiconductors.

Different forms of energy conversion based on superhydrophobic surfaces.

Significant enhancements of binding constants for molecular recognition are observed at the air–water interface, which would be related to molecular recognition in biomolecular systems.

Polyelectrolyte complexes (PECs) exhibit varying dynamic responses depending upon the ionic strength, water content, temperature, pH, and molecular weight.

We review an atomistic, fully polarizable approach to accurately predict the chiroptical properties of molecular systems in aqueous solution, by retaining all relevant physico-chemical interactions.

An overview of catalysis related to hydrogen spillover, surface protonics, analysis techniques for hydrogen migration, and low-temperature catalysis using surface protonics are summarized.

Two-dimensional materials are now excelling in yet another arena of ultrafast photonics, including optical modulation through optical limiting/mode-locking, photodetectors, optical communications, integrated miniaturized all-optical devices, etc.

Various contributions to the outer reorganization energy of an electron transfer system and their theoretical and computational aspects have been discussed.

Charge transfer is vital for life on Earth and makes our modern ways of living possible.

Spin polarized electrons can control asymmetric electrochemical reactions.

Polymer blending is an effective method that can be used to fabricate new versatile materials with enhanced properties.

Accelerated prediction of thermoelectric properties by a simple theoretical modelling.

Perspectives on the use of soft X-ray absorption spectroscopy as a tool to rationally develop new heterogeneous catalysts.

Infrared spectroscopic methods enable quantum-state-specific and surface-site-selective studies of methane chemisorption on stepped platinum surfaces.

Large cluster projectiles boost molecular sensitivity in mass spectrometry and open new avenues for physical characterization and nanofabrication.

Three properties of the exact energy functional of DFT are important in general and for spectroscopy in particular, but are not necessarily obeyed by approximate functionals. We explain what they are, why they are important, and how they are related yet inequivalent.

Sum frequency generation spectroscopy uncovers the orientational ordering in crystalline ice films of water grown on Pt(111) and Rh(111).

This review summarizes the morphology control strategy, phase transfer theory, spectrum modulation, and extended optical applications of RE³⁺-doped phosphors.

All molecular systems possess a significant number of rovibrational resonance states accessible via spectroscopic and scattering experiments, which can also be computed and rationalized by a variety of first-principles quantum-chemical techniques.

In this review, the multiferroic properties, vortex domain patterns and non-stoichiometric effect in hexagonal rare-earth manganites and ferrites are discussed.

Metal–organic frameworks act as efficient photocatalysts for visible-light driven hydrogen peroxide production in a single-phase system and two-phase system.

Proper treatment of intermolecular complexes formed by radicals and closed-shell molecules in energy decomposition analysis of DFT calculations.

A gateable single-molecule diode and resonant tunneling diode are realized using molecular orbital engineering in multi-site molecules.

The onset of facile intramolecular vibrational energy flow can be related to features in the connected network of anharmonic resonances in the classical phase space.

Crossed-beam imaging studies of polyatomic reactions show surprising dynamics not anticipated by extrapolation from smaller model systems.

Ab initio molecular dynamics simulations of ambient liquid water and energy decomposition analysis have recently shown that water molecules exhibit significant asymmetry between the strengths of the two donor and/or the two acceptor interactions.

Density Functional Theory (DFT) calculations of electrode material properties in high energy density storage devices like lithium batteries have been standard practice for decades.

“Many-body” dispersion can refer to two distinct phenomena, here termed electronic and atomic many-body effects, both of which cause the dispersion energy to be non-additive.

Breaking the OH–OOH scaling relation does not necessarily enhance water splitting electrocatalysis. Seeking “electrocatalytic symmetry” is a suitable alternative.

Astrochemistry: toward the molecular complexity in the interstellar medium.

High-throughput sequencing (HTS) of mRNA display selection of functional peptides.

Reactions between KRb molecules at sub-microkelvin temperatures were probed using ion spectrometry.

Modern microscopy to access super-resolution infrared absorption of materials.

Recently, machine learning (ML) has established itself in various worldwide benchmarking competitions in computational biology, including Critical Assessment of Structure Prediction (CASP) and Drug Design Data Resource (D3R) Grand Challenges.

This perspective discusses, theory, applications, and recent developments of spin-flip methods in quantum chemistry.

Synchrotron radiation provides insight into spectroscopy and dynamics in clusters and nanoparticles.

An ultrathin Al₂O₃ layer deposited between RuN3 and ZIF-67 by ALD can finely control the energy transfer efficiency between them.

Electronegativity equalization is examined after understanding an atom-in-a-molecule as an open quantum system, characterized by a variable fluctuating number of electrons whose average is set through charge-constrained electronic structure calculations.

An octanol/ethanol/water surfactant-free microemulsion solvates hydrophobic propane in small octanol/ethanol aggregates similar to traditional micelles.

Charge separation can be achieved over very long distances in semiconductors by combining bipolar electrochemistry with UV irradiation.

A design strategy for high surface area CMPs is to choose a solvent that minimises miscibility of solvent and reactants.

A probabilistic spin annihilation method based on the quantum phase estimation algorithm is presented for quantum chemical calculations on quantum computers.

In this work, the dynamic reaction pathways of nitrogen-doped carbon catalysts are investigated in acetylene hydrochlorination.

Site-dependent selectivity in oxidation reactions on Pt nanoparticles was identified by conducting IR nanospectroscopy measurements while using allyl-functionalized N-heterocyclic carbenes (allyl-NHCs) as probe molecules.

The dependence of radiolytic stability on both the organic and inorganic components of hybrid materials is explained.

The discovery of layered two-dimensional (2D) ferroelectric materials has promoted the development of miniaturized and highly integrated ferroelectric electronics.

1 exhibited opposite Py excimer-origin CPL in chloroform and PMMA film. 2 exhibited mirror-symmetric Py-monomer-origin MCPL.

A newly synthesized Gd³⁺ chelate complex allows in cell spin labeling and detection of eGFP by EPR spectroscopy.

Dispersive XAFS (DXAFS) was used for the structural characterization of a hardly-isolatable molybdenum–dinitrogen complex bearing a PNP-type pincer ligand.

Reactive molecular dynamics simulations show how ion-paring, cross-correlated ion motions and proton transfer contribute to the ionic conductivity in concentrated NaOH solutions at elevated temperatures.

Spectroscopic characterisations of the radical polyinterhalogen molecules IF₂ and I₂F are reported using anion photoelectron spectroscopy.

Graphene nanoribbons (GNRs) with atomically precise heterojunction interfaces are exploited as nanoscale light emitting devices with modulable emission frequencies.

We propose a computational framework for developing Taft-like linear free energy relationships to characterize steric effects on the catalytic activity of transition metal complexes.

Per- and polyfluoroalkyl substances (PFASs) are harmful man-made chemicals that have contaminated several drinking water resources worldwide. Our work provides the first real-time assessment of PFAS degradation in the presence of excess electrons.

Non-canonical amino acid incorporation via amber stop codon suppression and in vivo site-directed spin labeling allow in-cell EPR distance determination in E. coli.

We develop the first accurate full-dimensional ab initio PES for the OH⁻ + CH₃I S_N2 and proton-transfer reactions treating the failure of CCSD(T) at certain geometries.

Herein we discuss the operational principles of molecular interfaces that specifically recruit ions from an electrolyte solution and report this in a reagentless capacitive manner.

A distinct two-stage reduction of Cu₂O islands under methanol is revealed via combined in situ ETEM, statistical analysis, and DFT calculations.

Using chiral tosylates as model systems we evaluate the effect of diffuse and polarization functions on the quality of predicted VCD and IR spectra. Polarization functions on sulfur are shown to be important to reliable determine ACs using VCD.

Nanocomposite absorbers possess a simple structure and tailorable absorption in the mid-infrared (MIR) region achieved by manipulating structural parameters.

Mixing ionic liquids (ILs) with cosolvents can extend the practical applications of ILs and overcome the drawbacks of neat ILs. Studies on the structure and hydrogen-bond interaction properties of IL–cosolvent mixtures is essential for chemical applications.

The segregation tendency of an impurity in a semiconductor nanowire can be tuned by adjusting the Fermi level position.

This research provides an atomic-level insight into the synergic contribution of mono- and divalent ions to interfacial environment of calcite surfaces exposed to electrolyte solutions containing organic compounds.

The lifetime of a localised singlet diradical with bulky substituents was extended using the dynamic solvent effect and reached an almost bottleable timescale of ∼2 s under extremely viscous conditions induced by high pressure.

The motion of the confined doxorubicin drug molecule exhibits an interesting combination of anomalous diffusion features.

This work analyzes rotational–vibrational spectra of scattering resonances in four ozone isotopomers in relation to the symmetry-driven isotope effect.