Opportunities and challenges in energy and electron transfer of nanocluster based hybrid materials and their sensing applications
This feature article highlights the recent advances of luminescent metal nanoclusters (MNCs) for their potential applications in healthcare and energy-related materials because of their high photosensitivity, thermal stability, low toxicity, and biocompatibility.
Quantum approaches to vibrational dynamics and spectroscopy: is ease of interpretation sacrificed as rigor increases?
The subject of this Perspective is quantum approaches, beyond the harmonic approximation, to vibrational dynamics and IR spectroscopy.
The canonical behavior of the entropic component of thermodynamic effective molarity. An attempt at unifying covalent and noncovalent cyclizations
The statistically corrected entropic component of effective molarity (EMS*) complies with the “canonical” values expressed by the log plot of EMS* vs. the number n of single bonds in the ring product.
Surface and interface design for heterogeneous catalysis
Recent progresses in catalytic nanocrystals with uniform and well-defined structures, in situ characterization techniques, and theoretical calculations are facilitating the innovation of efficient catalysts via surface and interface designs, including crystal phase design, morphology/facet design, and size design, followed by controlled synthesis.
A perspective on quantum mechanics and chemical concepts in describing noncovalent interactions
Since quantum mechanical calculations do not typically lend themselves to chemical interpretation, analyses of bonding interactions depend largely upon models (the octet rule, resonance theory, charge transfer, etc.). This sometimes leads to a blurring of the distinction between mathematical modelling and physical reality.
Two dimensional boron nanosheets: synthesis, properties and applications
As a material generating increasing interest, boron nanosheets have been reviewed from the perspective of their synthesis, properties, application and possible research directions.
Explicit vs. implicit electronic polarisation of environment of an embedded chromophore in frozen-density embedding theory
A comparison of strategies to account for environment polarisation in Frozen Density Embedding Theory (FDET).
Towards the SMART workflow system for computational spectroscopy
Is it possible to convert highly specialized research in the field of computational spectroscopy into robust and user-friendly aids to experiments and industrial applications?
Block copolymer self-assembly in ionic liquids
Recent developments in block copolymer self-assembly in ionic liquids are reviewed from both fundamental and applied aspects.
Superatom chemistry: promising properties of near-spherical noble metal clusters
Atomic angular moments are nearly quenched in bonded structures, but superatoms in cylindrical environments develop molecular orbital moments.
Photoinduced charge transfer by one and two-photon absorptions: physical mechanisms and applications
We review photoinduced charge transfer in organic solar cells without and with an external electric field and then we introduce the visualization methods of the transition density, charge difference density and transition density matrix for the analysis of the photoinduced charge transfer in a neutral system and a charged system excited by one-photon and two-photon absorption.
What's in a name? ‘Coinage-metal’ non-covalent bonds and their definition
Isomorphism among angular geometries of halogen- and ‘coinage metal’-bonded complexes of water.
Is a cross-β-sheet structure of low molecular weight peptides necessary for the formation of fibrils and peptide hydrogels?
Using both theory and experiment, we identify two oligomer structures formed by tripeptides in aqueous solutions.
Understanding the ionic conductivity maximum in doped ceria: trapping and blocking
Ionic conductivity is systematically predicted by only a few migration energies from first-principles DFT calculations combined with Kinetic Monte Carlo simulations.
Multi-fuel surrogate chemical kinetic mechanisms for real world applications
The most important driving force for development of detailed chemical kinetic reaction mechanisms in combustion is the desire by researchers to simulate practical systems.
On the prediction of core level binding energies in molecules, surfaces and solids
Core level binding energies, measured by X-ray photoelectron spectroscopy providing unique information regarding the chemical environment of atoms in a system, can be estimated by a diversity of state-of-the-art accurate methods here detailed.
Necessary and sufficient conditions for the successful three-phase photocatalytic reduction of CO2 by H2O over heterogeneous photocatalysts
Artificial photosynthesis has recently drawn an increasing amount of attention due to the fact that it allows for direct solar-to-chemical energy conversion.
New tricks for old dogs: improving the accuracy of biomolecular force fields by pair-specific corrections to non-bonded interactions
Recent advances in parallel computing have pushed all-atom molecular dynamics simulations into an untested territory. This article reviews the applications of the NBFIX approach for testing and improving molecular dynamics force fields and discuses the implications of the NBFIX corrections for simulations of various biomolecular systems.
Mechanisms ruling the partition of solutes in ionic-liquid-based aqueous biphasic systems – the multiple effects of ionic liquids
The partition of solutes in ionic-liquid-based aqueous biphasic systems is due a multiple effect resulting from both solute–solvent and specific solute–ionic-liquid interactions.
Molecular cocrystals: design, charge-transfer and optoelectronic functionality
This perspective article primarily focuses on the research work related to optoelectronic properties of organic charge transfer cocrystals.
Spectroscopy of prospective interstellar ions and radicals isolated in para-hydrogen matrices
The p-H2 matrix-isolation technique coupled with photolysis in situ or electron bombardment produces protonated or hydrogenated species important in astrochemistry.
Field-, strain- and light-induced superconductivity in organic strongly correlated electron systems
In this perspective, our recent progress in the development of novel SC organic FETs was reviewed, in which organic strongly correlated electron materials were utilised as channel materials.
Magnetic order and enhanced exchange in the quasi-one-dimensional molecule-based antiferromagnet Cu(NO3)2(pyz)3
The magnetic properties of Cu(NO3)2(pyz)3 demonstrate ideal one-dimensional Heisenberg antiferromagnetic behaviour owing to the local environment of Cu2+ ions.
Density functional theory calculations and thermodynamic analysis of bridgmanite surface structure
Bridgmanite surface structure variations as a function of chemical potentials of Mg and O at the upper most of the Earth's lower mantle condition (∼660 km).
Rotation-tunneling spectrum of the water dimer from instanton theory
A linearly-scaling path-integral method is developed to calculate rotation-tunneling spectra, and is applied to the water dimer.
Visible light-triggered fluorescence and pH modulation using metastable-state photoacids and BODIPY
Small changes in the pH gradient play a critical role in numerous biological and chemical pathways.
Electron transfer characteristics of 2′-deoxy-2′-fluoro-arabinonucleic acid, a nucleic acid with enhanced chemical stability
The non-biological nucleic acid 2′F-ANA may be of use in nanobiotechnology because it combines greater chemical stability than DNA with comparable charge conduction properties.
An Ab initio study on the photophysics of tris(salicylideneaniline)
Sequential excited-state proton transfers result in multiple band fluorescence spectrum.
Probing ultrafast dynamics during and after passing through conical intersections
Time-resolved photoelectron spectroscopy using vacuum-UV probe pulses enables observing ultrafast dynamics during and after passing through conical intersections.
Simultaneous activity and surface area measurements on single mesoporous nanoparticle aggregates
The underpotential deposition of hydrogen and the hydrogen evolution reaction is studied at individual mesoporous nanoparticles. This work shows how the electroactive surface area and catalytic activity of these individual particles can be simultaneously measured.
Relationship between electron–phonon interaction and low-frequency Raman anisotropy in high-mobility organic semiconductors
Raman spectroscopy and calculations probe the impact of low-frequency vibrations in anisotropic electron–phonon interaction.
Reliable and computationally affordable prediction of the energy gap of (TiO2)n (10 ≤ n ≤ 563) nanoparticles from density functional theory
Suitable and practical way to estimate Ogap of TiO2 nanoparticles containing up to thousands of atoms from computationally affordable relativistic all-electron calculations with a numerical atomic centered orbital basis set.
Glass formation of a DMSO–water mixture probed with a photosynthetic pigment
We demonstrate an experimental method for probing the glass transition of hydrogen-bonded liquids and for identifying their dynamic heterogeneities.
Vibrational quantum graphs and their application to the quantum dynamics of CH5+
The first application of quantum-graph theory to molecular vibrations helps understand the low-energy vibrational quantum dynamics of CH5+.
The impact of tensorial temperature on equilibrium thermodynamics
By studying a sessile water droplet, it is shown that tensorial temperature leads to the wrong thermodynamics.
Probing heterogeneity of NIR induced secondary fluorescence from DNA-stabilized silver nanoclusters at the single molecule level
Heterogeneities of NIR induced secondary fluorescence from individual DNA-stabilized silver nanoclusters probed by time-correlated single photon counting.
Intermediate length-scale chirality related to the vibrational circular dichroism intensity enhancement upon fibril formation in a gelation process
The VCD intensity enhancement occurring upon fibril formation arises from the second out of the three hierarchical tiers of chirality.
The very long-term physical aging of glassy polymers
The thermodynamic state of polymer glasses aged over 30 years reveals the existence of a metastable state with partial equilibrium recovery.
Planar pentacoordinate carbon in CGa5+ derivatives
A single isoelectronic substitution by a smaller sized element, Be, is enough to stabilize a CGa5+ cluster with a planar pentacoordinate carbon at the centre.
Thermal equilibration between excited states or solvent effects: unveiling the origins of anomalous emissions in heteroleptic Ru(II) complexes
Thermal equilibration between excited states or solvent effects: unveiling the origins of anti-Kasha emissions in heteroleptic [Ru(H)(CO)(N^N)(tpp)2]+ complexes.
Cascade sensitization of triplet–triplet annihilation based photon upconversion at sub-solar irradiance
Cascade sensitization of optically dark triplets allows to increase by 20% the light output in triplet–triplet annihilation based photon upconversion.
Liquid–liquid phase coexistence in lipid membranes observed by natural abundance 1H–13C solid-state NMR
Solid-state NMR is used to detect liquid–liquid phase coexistence from randomly oriented lipid membranes with natural abundance of isotopes.
Zeolites with isolated-framework and oligomeric-extraframework hafnium species characterized with pair distribution function analysis
PDF analysis enabled the visualization and identification of framework and extraframework HfOx species in the post-synthetically produced *BEA zeolites.
A molecular quantum switch based on tunneling in meta-D-phenol C6H4DOH
The concept of a molecular quantum switch is introduced from realistic, quantitative wavepacket analyses of tunneling switching in m-D-phenol.
Collective thermal transport in pure and alloy semiconductors
Suppressing collective effects from momentum-conserving phonon collisions cause fast drop in thermal conductivity at small semiconductor alloy impurity concentrations.
Directing the mechanism of CO2 reduction by a Mn catalyst through surface immobilization
Immobilization of a Mn polypyridyl CO2 reduction electrocatalyst on nanocrystalline TiO2 electrodes yields an active heterogeneous system and also significantly triggers a change in voltammetric and catalytic behaviour, relative to in solution.
First-principles study of intrinsic defects in formamidinium lead triiodide perovskite solar cell absorbers
Based on first-principles calculations, the intrinsic defects in FAPbI3 are investigated systematically. It is found that antisites FAI and IFA create deep levels in the band gap which can act as recombination centers.
Coordination numbers for unraveling intrinsic size effects in gold-catalyzed CO oxidation
Geometry-based reactivity descriptors, e.g., regular, generalized, and orbitalwise coordination numbers, were used for unraveling intrinsic size effects of Au nanocatalysts towards CO oxidation.
Inducing chemical reactivity on specific sites of a molecule using the Coulomb interaction exerted by a low energy electron
Site-specificity in the resonant attachment of low energy electrons to molecular targets is used for engineering chemical reactivity.
Maxwell-Hall access resistance in graphene nanopores
A novel finite-size scaling ansatz allows all-atom simulations to dissect the relative contributions of pore and access resistance in nanopores.
Ultrafast coherent vibrational dynamics in dimethyl methylphosphonate radical cation
Coherent vibrational dynamics drive dissociation of dimethyl methylphosphonate (DMMP) radical cation.
An organoferroelasticity driven by molecular conformational change
We describe ferroelasticity in an organic crystal and its potential utility for damping led by the nature of molecular components.
The first successful observation of in-cell NMR signals of DNA and RNA in living human cells
The first observation of NMR signals of DNA/RNA introduced into living human cells by means of pore formation by SLO and resealing.
The effect of regioisomerism on the photophysical properties of alkylated-naphthalene liquids
Novel alkylated naphthalene liquids with a correlation among the 1- and 2-regioisomeric chemical structures and their photophysical, calorimetric and rheological properties are presented.
The C-terminal cytidine deaminase domain of APOBEC3G itself undergoes intersegmental transfer for a target search, as revealed by real-time NMR monitoring
The deamination activity of A3G-CTD was first increased, but then decreased, which indicated that A3G undergoes the intersegmental transfer.
Spatially resolved ultrasound diagnostics of Li-ion battery electrodes
This work describes the use of spatially acoustic techniques to identify the condition of electrodes in a commercial lithium-ion battery.
Solving the Schrödinger equation of hydrogen molecules with the free-complement variational theory: essentially exact potential curves and vibrational levels of the ground and excited states of the Σ symmetry
The Schrödinger equation of hydrogen molecules was solved essentially exactly and systematically for calculating the potential energy curves of the electronic ground and excited states of the 1Σg, 1Σu, 3Σg, and 3Σu symmetries.
Hydrogen adsorption on transition metal carbides: a DFT study
This work investigates the hydrogenation of the surfaces of those materials and its relationship with the catalytic behaviour of these materials.
Can microsolvation effects be estimated from vacuum computations? A case-study of alcohol decomposition at the H2O/Pt(111) interface
Activation and reaction energies of alcohol decomposition at Pt(111) are barely modified by a PCM, in contrast to adding a single water molecule, whose effect can be predicted based on vacuum computations.
Femtosecond electronic relaxation and real-time vibrational dynamics in 2′-hydroxychalcone
Electronic relaxation, proton transfer and instantaneous vibrational frequency change after the impulsive excitation by a deep ultraviolet 9 fs pulse were studied.
Assessing relative humidity dependent photoacoustics to retrieve mass accommodation coefficients of single optically trapped aerosol particles
Photoacoustic spectroscopy is a standout technique widely used for absorption measurements of atmospheric aerosols. Here we investigate the relative humidity dependence of photoacoustics and its implication for evaporation kinetics.
Molecular dynamics investigation of the local structure in iron melts and its role in crystal nucleation during rapid solidification
Nucleation process of a bcc crystal after the formation of an MRO cluster.
General existence of flexural mode doublets in nanowires targeting vectorial sensing applications
Generally existing flexural mode doublets in silicon nanowires.
Rovibrational quantum dynamics of the vinyl radical and its deuterated isotopologues
Rotational–vibrational states up to 3200 cm−1, beyond the highest-lying stretching fundamental, are computed variationally for the vinyl radical (VR), H2CβCαH, and the following deuterated isotopologues of VR: CH2CD, CHDCH, and CD2CD.
Interfacial premelting of ice in nano composite materials
We present a quantitative description of ice premelting in permafrost model systems. Experimental data on the interfacial premelting in ice/clay nano composites was obtained by high energy X-ray diffraction.
Theoretical insight into joint photodynamic action of a gold(I) complex and a BODIPY chromophore for singlet oxygen generation
Inclusion of a heavy gold atom in a peripheral position of BODIPY is enough to promote ISC.
Double resonance rotational spectroscopy of He–HCO+
The ground state of He–HCO+ is investigated using a recently developed double resonance technique, consisting of a rotational transition followed by a vibrational transition into a dissociative state.
Spectroscopy of a rotating hydrogen molecule in carbon nanotubes
Computing the energy levels of molecular hydrogen rotating in carbon nanotubes of increasing size.
Surfactant-enhanced heterogeneity of the aqueous interface drives water extraction into organic solvents
Liquid/liquid extraction (LLE) is one of the most industrially relevant separations methods. Adsorbed surfactant is demonstrated to enhance interfacial heterogeneity and lead to water protrusions that form the basis for transport into the organic phase.
Production of HO2 and OH radicals from near-UV irradiated airborne TiO2 nanoparticles
Production of HO2 radicals is observed directly following the near-UV irradiation of airborne TiO2 nanoparticles.
About this collection
Welcome to our online rolling collection of the hottest work published in PCCP. Here we feature all the 2018 PCCP articles highlighted as HOT by the handling editor or our referees. Congratulations to all the authors whose articles are featured.