Reorganization energies and spectral densities for electron transfer problems in charge transport materials
Various contributions to the outer reorganization energy of an electron transfer system and their theoretical and computational aspects have been discussed.
Multifaceted aspects of charge transfer
Charge transfer is vital for life on Earth and makes our modern ways of living possible.
Asymmetric reactions induced by electron spin polarization
Spin polarized electrons can control asymmetric electrochemical reactions.
Nanoparticles influence miscibility in LCST polymer blends: from fundamental perspective to current applications
Polymer blending is an effective method that can be used to fabricate new versatile materials with enhanced properties.
Theoretical model for predicting thermoelectric properties of tin chalcogenides
Accelerated prediction of thermoelectric properties by a simple theoretical modelling.
Soft XAS as an in situ technique for the study of heterogeneous catalysts
Perspectives on the use of soft X-ray absorption spectroscopy as a tool to rationally develop new heterogeneous catalysts.
Quantum state and surface-site-resolved studies of methane chemisorption by vibrational spectroscopies
Infrared spectroscopic methods enable quantum-state-specific and surface-site-selective studies of methane chemisorption on stepped platinum surfaces.
Large cluster ions: soft local probes and tools for organic and bio surfaces
Large cluster projectiles boost molecular sensitivity in mass spectrometry and open new avenues for physical characterization and nanofabrication.
Piecewise linearity, freedom from self-interaction, and a Coulomb asymptotic potential: three related yet inequivalent properties of the exact density functional
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.
Orientational ordering in heteroepitaxial water ice on metal surfaces
Sum frequency generation spectroscopy uncovers the orientational ordering in crystalline ice films of water grown on Pt(111) and Rh(111).
Morphology control, spectrum modification and extended optical applications of rare earth ion doped phosphors
This review summarizes the morphology control strategy, phase transfer theory, spectrum modulation, and extended optical applications of RE3+-doped phosphors.
Rotational–vibrational resonance states
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.
Hexagonal rare-earth manganites and ferrites: a review of improper ferroelectricity, magnetoelectric coupling, and unusual domain walls
In this review, the multiferroic properties, vortex domain patterns and non-stoichiometric effect in hexagonal rare-earth manganites and ferrites are discussed.
Metal–organic framework-based nanomaterials for photocatalytic hydrogen peroxide production
Metal–organic frameworks act as efficient photocatalysts for visible-light driven hydrogen peroxide production in a single-phase system and two-phase system.
Probing radical–molecule interactions with a second generation energy decomposition analysis of DFT calculations using absolutely localized molecular orbitals
Proper treatment of intermolecular complexes formed by radicals and closed-shell molecules in energy decomposition analysis of DFT calculations.
Single-molecule functionality in electronic components based on orbital resonances
A gateable single-molecule diode and resonant tunneling diode are realized using molecular orbital engineering in multi-site molecules.
Intramolecular vibrational energy redistribution and the quantum ergodicity transition: a phase space perspective
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.
Universal crossed beam imaging studies of polyatomic reaction dynamics
Crossed-beam imaging studies of polyatomic reactions show surprising dynamics not anticipated by extrapolation from smaller model systems.
Tumbling with a limp: local asymmetry in water's hydrogen bond network and its consequences
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.
DFT modelling of explicit solid–solid interfaces in batteries: methods and challenges
Density Functional Theory (DFT) calculations of electrode material properties in high energy density storage devices like lithium batteries have been standard practice for decades.
What is “many-body” dispersion and should I worry about it?
“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.
Designing water splitting catalysts using rules of thumb: advantages, dangers and alternatives
Breaking the OH–OOH scaling relation does not necessarily enhance water splitting electrocatalysis. Seeking “electrocatalytic symmetry” is a suitable alternative.
The challenging playground of astrochemistry: an integrated rotational spectroscopy – quantum chemistry strategy
Astrochemistry: toward the molecular complexity in the interstellar medium.
High throughput sequencing of in vitro selections of mRNA-displayed peptides: data analysis and applications
High-throughput sequencing (HTS) of mRNA display selection of functional peptides.
Probing ultracold chemistry using ion spectrometry
Reactions between KRb molecules at sub-microkelvin temperatures were probed using ion spectrometry.
Approaches to mid-infrared, super-resolution imaging and spectroscopy
Modern microscopy to access super-resolution infrared absorption of materials.
A review of mathematical representations of biomolecular data
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.
Spin-flip methods in quantum chemistry
This perspective discusses, theory, applications, and recent developments of spin-flip methods in quantum chemistry.
From atoms to aerosols: probing clusters and nanoparticles with synchrotron based mass spectrometry and X-ray spectroscopy
Synchrotron radiation provides insight into spectroscopy and dynamics in clusters and nanoparticles.
Solubilization power of surfactant-free microemulsions
An octanol/ethanol/water surfactant-free microemulsion solvates hydrophobic propane in small octanol/ethanol aggregates similar to traditional micelles.
Light and electric field induced unusual large-scale charge separation in hybrid semiconductor objects
Charge separation can be achieved over very long distances in semiconductors by combining bipolar electrochemistry with UV irradiation.
Rationalising the influence of solvent choice on the porosity of conjugated microporous polymers
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 for quantum chemical calculations on quantum computers
A probabilistic spin annihilation method based on the quantum phase estimation algorithm is presented for quantum chemical calculations on quantum computers.
Synergistic effect of two action sites on a nitrogen-doped carbon catalyst towards acetylene hydrochlorination
In this work, the dynamic reaction pathways of nitrogen-doped carbon catalysts are investigated in acetylene hydrochlorination.
Site-dependent selectivity in oxidation reactions on single Pt nanoparticles
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.
New insights into the radiolytic stability of metal(IV) phosphonate hybrid adsorbent materials
The dependence of radiolytic stability on both the organic and inorganic components of hybrid materials is explained.
A neutron irradiation-induced displacement damage of indium vacancies in α-In2Se3 nanoflakes
The discovery of layered two-dimensional (2D) ferroelectric materials has promoted the development of miniaturized and highly integrated ferroelectric electronics.
Excimer-origin CPL vs. monomer-origin magnetic CPL in photo-excited chiral binaphthyl-ester-pyrenes: critical role of ester direction
1 exhibited opposite Py excimer-origin CPL in chloroform and PMMA film. 2 exhibited mirror-symmetric Py-monomer-origin MCPL.
In cell Gd3+-based site-directed spin labeling and EPR spectroscopy of eGFP
A newly synthesized Gd3+ chelate complex allows in cell spin labeling and detection of eGFP by EPR spectroscopy.
Structural characterization of molybdenum–dinitrogen complex as key species toward ammonia formation by dispersive XAFS spectroscopy
Dispersive XAFS (DXAFS) was used for the structural characterization of a hardly-isolatable molybdenum–dinitrogen complex bearing a PNP-type pincer ligand.
Temperature effects on the ionic conductivity in concentrated alkaline electrolyte solutions
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 characterisation of radical polyinterhalogen molecules
Spectroscopic characterisations of the radical polyinterhalogen molecules IF2 and I2F are reported using anion photoelectron spectroscopy.
Controlling the emission frequency of graphene nanoribbon emitters based on spatially excited topological boundary states
Graphene nanoribbons (GNRs) with atomically precise heterojunction interfaces are exploited as nanoscale light emitting devices with modulable emission frequencies.
Linear free energy relationships for transition metal chemistry: case study of CH activation with copper–oxygen complexes
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.
Real-time degradation dynamics of hydrated per- and polyfluoroalkyl substances (PFASs) in the presence of excess electrons
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.
Combining site-directed spin labeling in vivo and in-cell EPR distance determination
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.
On the development of a gold-standard potential energy surface for the OH− + CH3I reaction
We develop the first accurate full-dimensional ab initio PES for the OH− + CH3I SN2 and proton-transfer reactions treating the failure of CCSD(T) at certain geometries.
The nanoscopic principles of capacitive ion sensing interfaces
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.
In situ environmental TEM observation of two-stage shrinking of Cu2O islands on Cu(100) during methanol reduction
A distinct two-stage reduction of Cu2O islands under methanol is revealed via combined in situ ETEM, statistical analysis, and DFT calculations.
Structure and dynamics of the molten alkali-chloride salts from an X-ray, simulation, and rate theory perspective
Molten salts are of great interest as alternative solvents, electrolytes, and heat transfer fluids in many emerging technologies.
Nuclear spin-induced optical rotation of functional groups in hydrocarbons
Systematic correlation between molecular structure and nuclear spin-induced optical rotation is demonstrated in the case of hydrocarbon molecules.
Establishing the accuracy of density functional approaches for the description of noncovalent interactions in biomolecules
Biomolecules have complex structures, and noncovalent interactions are crucial to determine their conformations and functionalities.
Accessing distributions of exchange and dipolar couplings in stiff molecular rulers with Cu(II) centres
Novel approaches to quantitatively analyse distributed exchange couplings are described and tested on experimental data sets for stiff synthetic molecules.
Quantifying active diffusion in an agitated fluid
Single-particle tracking reveals an enhanced diffusional motion of tracer beads when agitating the surrounding fluid with miniaturized magnetic stir bars. Signatures of the stirring are mostly encoded in correlation functions of the particle motion.
Regio- and stereoselectivity in the CYP450BM3-catalyzed hydroxylation of complex terpenoids: a QM/MM study
The selective oxidation of C–H in artemisinin by P450BM3 variants was disclosed by combining QM/MM and MD simulations.
Interplay between two radical species in the formation of periodic patterns during a polymerization reaction
Interplay between initiator and monomer radicals forms periodic precipitation of polymers.
Structural investigation of doubly-dehydrogenated pyrene cations
The first infrared predissociation spectra of the pyrene and doubly-dehydrogenated pyrene cations (C16H10˙+; Py+ and C16H8˙+; ddPy+) are presented. The vibrationally resolved spectrum of ddPy+ is dominated by absorption features from two isomers.
Low-power STMAS – breaking through the limit of large quadrupolar interactions in high-resolution solid-state NMR spectroscopy
The STMAS NMR experiment reported requires significantly lower rf fields and allows acquisition of high-resolution spectra for large quadrupolar interactions.
Net negative contributions of free electrons to the thermal conductivity of NbSe3 nanowires
More free electrons from depinning the charge density wave in NbSe3 nanowires lead to an unexpected reduction of thermal conductivity.
Hydrophobic solvation increases thermal conductivity of water
The rearrangement of the H-bond network in bulk water induced by a small concentration of ethanol is not only reflected in the frequency of the libration band of water, but also in a surprising increase of its thermal conductivity.
High-resolution vacuum ultraviolet photodynamic of the nitrogen dioxide dimer (NO2)2 and the stability of its cation
Mass-selected TPES of the dimer N2O4 is recorded and its VUV photodynamics shows the dimer cation N2O4+ is unstable.
Understanding alkali metal cation affinities of multi-layer guanine quadruplex DNA
Stabilizing solvent effects and electrostatic repulsion are responsible for the constant alkali metal cation affinity in multi-layer guanine quadruplexes.
Structural characterization of supramolecular hollow nanotubes with atomistic simulations and SAXS
Self-assembled nanostructures arise when building blocks spontaneously organize into ordered aggregates that exhibit different properties compared to the disorganized monomers.
Unraveling the mechanisms of S-doped carbon nitride for photocatalytic oxygen reduction to H2O2
First-principles calculations reveal the mechanisms of thermodynamically feasible process for the selective oxygen photoreduction to H2O2 in the S-doped melon-based carbon nitride.
New insights into O and OH adsorption on the Pt–Co alloy surface: effects of Pt/Co ratios and structures
Our DFT study shows how the composition and surface electronic structure of Pt–Co alloys affect the adsorption of O and OH.
Unraveling the local structure and luminescence evolution in Nd3+-doped LiYF4: a new theoretical approach
On the basis of our newly developed WEPMD method, we predicted some promising laser channels in the region of visible and near-infrared spectra for Nd3+-doped LiYF4 laser crystals.
Acetylation of graphite oxide
Unlike many methods of chemical modification of Graphite Oxide (GO) reported during 1930–1960 and re-studied in much detail over the last decade, acetylation somehow escaped attention and remained almost completely unexplored.
Adsorption-induced clustering of CO2 on graphene
At high surface-coverages, CO2 molecules adsorbed on a graphene sheet can form clusters due to favorable quadrupole–quadrupole interactions.
Magnetic studies of polylactic-co-glicolic acid nanocapsules loaded with selol and γ-Fe2O3 nanoparticles
The coexistence of superparamagnetism, interacting superparamagnetism and giant diamagnetism is evidenced from the magnetic behavior of selol-loaded PLGA magnetic nanocapsules.
The electronic structure of the aqueous permanganate ion: aqueous-phase energetics and molecular bonding studied using liquid jet photoelectron spectroscopy
Liquid-jet photoelectron spectroscopy revealed the electronic structure of MnO4−(aq), O-ligand–water interactions, and aqueous-phase energetics of MnO4−(aq)/MnO4˙(aq.).
About this collection
Welcome to our online rolling collection of the hottest work published in PCCP. Here we feature all the 2020 PCCP articles highlighted as HOT by the handling editor or our referees. Congratulations to all the authors whose articles are featured.