Using anion photoelectron spectroscopy of cluster models to gain insights into mechanisms of catalyst-mediated H2 production from water
Anion PE spectroscopy and DFT calculations reveal molecular and electronic structural features of cluster models for catalysis.
Intriguing structural, bonding and reactivity features in some beryllium containing complexes
We highlighted our contributions to Be chemistry which include bond-stretch isomerism in Be32− species, Be complexes bound with noble gas, CO, and N2, Be based nanorotors, and intriguing bonding situations in some Be complexes.
The role of electron–nuclear coupling on multi-state photoelectron spectra, scattering processes and phase transitions
This article presents development of first principle based Beyond Born–Oppenheimer theory and its applications in conjunction with Jahn–Teller theory.
Coupled transport of electrons and protons in a bacterial cytochrome c oxidase—DFT calculated properties compared to structures and spectroscopies
DFT calculated structures, vibrational frequencies, and energies provide insights into the reaction/proton pumping cycle of cytochrome c oxidase.
Spectroscopic evidence of n → π* interactions involving carbonyl groups
n → π* interactions involving carbonyl groups can be detected in solution by using common spectroscopic methods such as IR, UV-Vis, and NMR if the interactions are relatively strong (>1.5 kcal mol−1).
In silico investigation of Cu(In,Ga)Se2-based solar cells
State-of-the-art methods in materials science such as artificial intelligence and data-driven techniques advance the investigation of photovoltaic materials.
Density functional theory based embedding approaches for transition-metal complexes
Density functional theory based embedding approaches for the description of chemical reactions are reviewed for their applicability to transition metal species.
Assessing cluster models of solvation for the description of vibrational circular dichroism spectra: synergy between static and dynamic approaches
Solvation effects are essential for defining the shape of vibrational circular dichroism (VCD) spectra.
Temperature control in DRIFT cells used for in situ and operando studies: where do we stand today?
Heat transfer limitations in diffuse-reflectance-infrared-Fourier-transform-spectroscopy cells, which can affect the measurement in spectrokinetic studies, have been appraised.
Phonon, thermal, and thermo-optical properties of halide perovskites
Halide perovskites possess unusual phonon and thermal properties, which lead to unique thermo-optical responses very different from those of conventional inorganic semiconductors.
Energy conversion based on superhydrophobic surfaces
Different forms of energy conversion based on superhydrophobic surfaces.
Challenges and prospects of polyatomic ions’ intercalation in the graphite layer for energy storage applications
This review focuses on unraveling the reaction mechanisms of the intercalation of polyatomic ions into GICs by in situ techniques, correlated with computational studies.
Molecular recognition at the air–water interface: nanoarchitectonic design and physicochemical understanding
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.
Emerging trends in the dynamics of polyelectrolyte complexes
Polyelectrolyte complexes (PECs) exhibit varying dynamic responses depending upon the ionic strength, water content, temperature, pH, and molecular weight.
Supramolecular and suprabiomolecular photochemistry: a perspective overview
This review article brings out current research trends in supramolecular and suprabiomolecular photochemistry, highlighting their possible applications in different areas.
Theory and algorithms for chiroptical properties and spectroscopies of aqueous systems
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.
Recent progress in use and observation of surface hydrogen migration over metal oxides
An overview of catalysis related to hydrogen spillover, surface protonics, analysis techniques for hydrogen migration, and low-temperature catalysis using surface protonics are summarized.
Disentangling the liquid phase exfoliation of two-dimensional materials: an “in silico” perspective
In this perspective article, recent advances in molecular simulation techniques have been reviewed to shed light on the complexity of liquid phase exfoliation of 2D materials.
2D materials towards ultrafast photonic applications
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.
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.
Energy dispersive X-ray diffraction (EDXRD) for operando materials characterization within batteries
This review highlights the efficacy of EDXRD as a non-destructive characterization tool in elucidating system-level phenomena for batteries.
Polymer models for the mechanisms of chromatin 3D folding: review and perspective
In this perspective paper, classical physical models for mammalian interphase chromatin folding are reviewed.
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.
Advances and challenges for experiment and theory for multi-electron multi-proton transfer at electrified solid–liquid interfaces
Understanding microscopic mechanism of multi-electron multi-proton transfer reactions at complexed systems is important for advancing electrochemistry-oriented science in the 21st century.
Towards molecular movies with X-ray photon correlation spectroscopy
We highlight perspective research opportunities of making molecular movies of biomolecular condensates and supercooled water using X-ray synchrotrons and XFELs.
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.
Enantiospecificity in achiral zeolites for asymmetric catalysis
We highlight the recent study in using chiral and achiral porous materials for the potential applications in asymmetric catalysis.
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.
Recent advances in MXenes and their composites in lithium/sodium batteries from the viewpoints of components and interlayer engineering
An up-to-date review about MXenes based on their distinguishing properties, namely, large interlayer spacing and rich surface chemistry.
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).
Polymer-based actuators: back to the future
This work demonstrates that polymer-based actuators play a key role in the area of smart materials and devices.
Enzyme-based optical biosensors for organophosphate class of pesticide detection
A systematic review of enzyme based optical detection schemes for the detection and analysis of organophosphate pesticides has been presented.
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.
Polarizable embedding QM/MM: the future gold standard for complex (bio)systems?
We provide a perspective of the induced dipole formulation of polarizable QM/MM, showing how efficient implementations will enable their application to the modeling of dynamics, spectroscopy, and reactivity in complex biosystems.
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.
A revisit of the bond valence model makes it universal
The application of Pauling's principles to any type of chemical bond can be validated using recent quantum chemistry data (bond orders), thus making them universal.
Towards sustainable and efficient p-type metal oxide semiconductor materials in dye-sensitised photocathodes for solar energy conversion
In order to meet the ever-growing global energy demand for affordable and clean energy, it is essential to provide this energy by renewable resources and consider the eco-efficiency of the production and abundance of the utilised materials.
Organic–inorganic hybrid perovskite electronics
Organic–inorganic hybrid perovskite is a leading successor for the next generation of (opto)electronics.
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.
Fragment-based quantum mechanical approach to biomolecules, molecular clusters, molecular crystals and liquids
To study large molecular systems beyond the system size that the current state-of-the-art ab initio electronic structure methods could handle, fragment-based quantum mechanical (QM) approaches have been developed over the past years, and proved to be efficient in dealing with large molecular systems at various ab initio levels.
High-throughput experimentation meets artificial intelligence: a new pathway to catalyst discovery
High throughput experimentation in heterogeneous catalysis provides an efficient solution to the generation of large datasets under reproducible conditions.
Quantum electrocatalysts: theoretical picture, electrochemical kinetic isotope effect analysis, and conjecture to understand microscopic mechanisms
The fundamental aspects of quantum electrocatalysts are discussed together with the newly developed electrochemical kinetic isotope effect (EC-KIE) approach.
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.
Biomolecule–polymer hybrid compartments: combining the best of both worlds
Recent advances in bio/polymer hybrid compartments in the quest to obtain artificial cells, biosensors and catalytic compartments.
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.
Surface chemistry of TiO2 connecting thermal catalysis and photocatalysis
The surface chemistry of small molecules on TiO2 is reviewed with the aim to connect thermal catalysis and photocatalysis.
Hierarchical phenomena in multicomponent liquids: simulation methods, analysis, chemistry
Complex, multicomponent, liquids benefit from a hierarchical understanding of solution speciation, collective organization and dynamics.
Cold and controlled chemical reaction dynamics
State-to-state chemical reaction dynamics, with complete control over the reaction parameters, offers unparalleled insight into fundamental reactivity.
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.
A new horizon for vibrational circular dichroism spectroscopy: a challenge for supramolecular chirality
The development of the solid state and time-step VCD methods opened a new horizon to reveal the mechanism of chirality amplification from microscopic to supramolecular scales.
Intrinsic nature of photocatalysis by comparing with electrochemistry
The kinetics of photocatalysis was discussed based on the calculated surface electric field, the limited electron transfer frequency and the irreversibility.
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.
Toward an understanding of electronic excitation energies beyond the molecular orbital picture
Can we gain an intuitive understanding of excitation energies beyond the molecular picture?
Theory and simulation developments of confined mass transport through graphene-based separation membranes
The perspectives of graphene-based membranes based on confined mass transport from simulations and experiments for water desalination.
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.
Benchmark ab initio and dynamical characterization of the stationary points of reactive atom + alkane and SN2 potential energy surfaces
We review composite ab initio and dynamical methods and their applications to characterize stationary points of atom/ion + molecule reactions.
About this collection
Welcome to our online collection of PCCP Perspective articles. Here we feature PCCP Perspective articles published in 2020.
Perspectives are high profile articles that present an authoritative state-of-the-art account of the selected research field. PCCP Perspectives take a wide variety of forms including personal accounts of research, critical analyses of topics of current interest and essential introductions to a field.
Congratulations to all the authors whose articles are featured and we hope readers enjoy this collection.