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A simple descriptor for energetics at fcc-bcc metal interfacesFeb 08 2018We develop a new and user-friendly method for calculating interface energies from first-principles. Our approach avoids problems that derive from the numerical differences between bulk and slab calculations, such as the number of k-points along the direction ... More

Fabrication and characterization of pH responsive nanoprobes based on ion current rectificationFeb 08 2018In this study, we investigated the ionic current rectification of glass nanopipettes modified with bovine serum albumin - glutaraldehyde (BSA-GA) artificial membrane using solutions with various pHs. Ionic current rectification is a phenomenon that is ... More

Transient dynamics of electric double layer capacitors: Exact expressions within the Debye-Falkenhagen approximationFeb 08 2018We revisit a classical problem of theoretical electrochemistry: the response of an electric double layer capacitor (EDLC) subject to a small, suddenly-applied external potential. We solve the Debye-Falkenhagen equation to obtain exact expressions for ... More

Relativistic coupled-cluster theory analysis of energies, hyperfine structure constants, and dipole polarizabilities of Cd$^{+}$Feb 08 2018Roles of electron correlation effects in the determination of attachment energies, magnetic dipole hyperfine structure constants and electric dipole (E1) matrix elements of the low-lying states in the singly charged cadmium ion (Cd$^+$) have been analyzed. ... More

Magnetic Isotope Effect in the Uranium Isotopes SeparationFeb 07 2018When uranyl nitrate is photolysed in the water solution, light isotope ${}^{235}{\rm U}$ is separated from isotope ${}^{238}{\rm U}$ ; an enrichment factor $K = 1.04$ . The initial samples were depleted by a light isotope of uranium ${}^{235}{\rm U}$ ... More

Towards Understanding the Structure, Dynamics and Bio-activity of Diabetic Drug MetforminFeb 07 2018Small molecules are often found to exhibit extraordinarily diverse biological activities. Metformin is one of them. It is widely used as anti-diabetic drug for type-two diabetes. In addition to that, metformin hydrochloride shows anti-tumour activities ... More

Catalytic membrane reactor model as a laboratory for pattern emergence in reaction-diffusion-advection mediaFeb 07 2018Reaction-diffusion-advection media on semi-infinite domains are important in chemical, biological and ecological applications, yet remain a challenge for pattern formation theory. To demonstrate the rich emergence of nonlinear traveling waves and stationary ... More

Stability of boron-doped graphene/copper interface: DFT, XPS and OSEE studiesFeb 07 2018Two different types of boron-doped graphene/copper interfaces synthesized using two different flow rates of Ar through the bubbler containing the boron source were studied. X-ray photoelectron spectra (XPS) and optically stimulated electron emission (OSEE) ... More

Catalysis by metallic nanoparticles in solution: Thermosensitive microgels as nanoreactorsFeb 07 2018Metallic nanoparticles have been used as catalysts for various reactions, and the huge literature on the subject is hard to overlook. In many applications, the nanoparticles must be affixed to a colloidal carrier for easy handling during catalysis. These ... More

Fidelity of bacterial translation initiation: a stochastic kinetic modelFeb 06 2018During the initiation stage of protein synthesis, a ribosomal initiation complex (IC) is assembled on a messenger RNA (mRNA) template. In bacteria, the speed and accuracy of this assembly process are regulated by the complementary activities of three ... More

Restoring size consistency of approximate functionals constructed from the adiabatic connectionFeb 06 2018Approximate exchange-correlation functionals built by modeling in a non-linear way the adiabatic connection (AC) integrand of density functional theory have many attractive features, being virtually parameters-free and satisfying different exact properties, ... More

Interlocking mechanism between molecular gears attached to surfacesFeb 06 2018While molecular machines play an increasingly significant role in nanoscience research and applications, there remains a shortage of investigations and understanding of the molecular gear (cogwheel), which is an indispensable and fundamental component ... More

Jellium with gap model applied to Orbital-Free Density Functional TheoryFeb 05 2018We construct a non-local kinetic energy functional having a density-independent kernel based on the linear response of the jellium-with-gap model. This functional has the correct physics for metals, semiconductors, and insulators in the low momentum limit ... More

Hybrid 2D Black Phosphorus/Polymer Materials: New Platforms for Device FabricationFeb 04 2018Hybrid materials, containing a 2D filler embedded in a polymeric matrix, are an interesting platform for several applications, because of the variety of properties that the filler can impart to the polymer matrix when dispersed at the nanoscale. Moreover, ... More

Lipid-protein interaction induced domains: kinetics and conformational changes in multicomponent vesiclesFeb 03 2018The spatio-temporal organization of proteins and the associated morphological changes in membranes are of importance in cell signaling. Several mechanisms that promote the aggregation of proteins at low cell surface concentrations have been investigated ... More

Origin of the size-dependence of the equilibrium van der Waals binding between nanostructuresFeb 03 2018Nanostructures can be bound together at equilibrium by the van der Waals (vdW) effect, a small but ubiquitous many-body attraction that presents challenges to density functional theory. How does the binding energy depend upon the size or number of atoms ... More

Quantum correction to thermodynamic properties of Li_2, Na_2 and Cs_2 dimersFeb 02 2018We have calculated the quantum correction(QC) in the vibrational partition function and thermodynamic state functions, e.g., internal energy, specific heat, free energy and entropy by using improved Manning-Rosen(MR) potential for Li_2, Na_2 and Cs_2 ... More

Optimized cell geometry for buffer-gas-cooled molecular-beam sourcesJan 31 2018We have designed, constructed, and commissioned a cryogenic helium buffer-gas source for producing a cryogenially-cooled molecular beam and evaluated the effect of different cell geometries on the intensity of the produced molecular beam, using ammonia ... More

Lie Algebraic approach to molecular spectroscopy: Diatomic to polyatomic moleculesJan 31 2018Interacting dipole ($p$) bosons along with scalar ($s$) bosons, based on the ideas drawn from the interacting boson model of atomic nuclei, led to the development of the vibron model based on $U(4)$ spectrum generating algebra for diatomic molecules. ... More

Non-Orthogonal Multi-Slater Determinant Expansions in Auxiliary Field Quantum Monte CarloJan 31 2018The Auxiliary-Field Quantum Monte Carlo (AFQMC) algorithm is a powerful quantum many-body method that can be used successfully as an alternative to standard quantum chemistry approaches to compute the ground state of many body systems, such as molecules ... More

Dynamic Chemical Model for H2/O2 Combustion Developed Through a Community WorkflowJan 30 2018Feb 03 2018Elementary-reaction models for H2/O2 combustion were evaluated and optimized through a collaborative workflow, establishing accuracy and characterizing uncertainties. Quantitative findings were the optimized model, the importance of $\text{H}_2 + \text{O}_2(1\Delta) ... More

Assessment of interaction-strength interpolation formulas for gold and silver clustersJan 30 2018The performance of functionals based on the idea of interpolating between the weak and the strong-interaction limits the global adiabatic-connection integrand is carefully studied for the challenging case of noble-metal clusters. Different interpolation ... More

Density-Wavefunction Mapping in Degenerate Current-Density-Functional TheoryJan 29 2018We show that the particle density, $\rho(\mathbf{r})$, and the paramagnetic current density, $\mathbf{j}^{p}(\mathbf{r})$, are not sufficient to determine the set of degenerate ground-state wave functions. This is a general feature of degenerate systems ... More

Temperature-Dependence of the Solid-Electrolyte Interphase Overpotential: Part I. Two Parallel Mechanisms, One Phase TransitionJan 28 2018It has been shown recently that the overpotential originating from ionic conduction of alkali-ions through the inner dense solid-electrolyte interphase (SEI) is strongly non-linear. An empirical equation was proposed to merge the measured resistances ... More

Molecular Dynamics of Lithium Ion Transport in a Model Solid Electrolyte InterphaseJan 26 2018Li+ transport within a solid electrolyte interphase (SEI) in lithium ion batteries has challenged molecular dynamics (MD) studies due to limited compositional control of that layer. In recent years, experiments and ab initio simulations have identified ... More

Identification of the fragment of the 1-methylpyrene cation by mid-IR spectroscopyJan 26 2018The fragment of the 1-methylpyrene cation, C17H11+, can exist in two isomeric forms, 1-pyrenemethylium PyrCH2+ and the tropylium containing species PyrC7+. We measured the infrared (IR) action spectrum of cold C17H11+ tagged with Ne using a cryogenic ... More

Ultrafast extreme ultraviolet photoemission without space chargeJan 24 2018Feb 02 2018Time- and Angle-resolved photoelectron spectroscopy from surfaces can be used to record the dynamics of electrons and holes in condensed matter on ultrafast time scales. However, ultrafast photoemission experiments using extreme-ultraviolet (XUV) light ... More

Strontium and Barium in Aqueous Solution and a Potassium Channel Binding SiteJan 24 2018Ion hydration structure and free energy establish criteria for understanding selective ion binding in potassium K+ ion channels, and may be significant to understanding blocking mechanisms as well. Recently, we investigated the hydration properties of ... More

Atom-molecule collisions, spin relaxation, and sympathetic cooling in an ultracold spin-polarized Rb($^2\mathrm{S}$)-SrF$(^2Σ^+)$ mixtureJan 24 2018We explore the suitability of ultracold collisions between spin-polarized SrF($^2\Sigma^+$) molecules and Rb($^2$S) atoms as elementary steps for the sympathetic cooling of SrF($^2\Sigma^+$) molecules in a magnetic trap. To this end, we carry out quantum ... More

Why does hydronium diffuse faster than hydroxide in liquid water?Jan 24 2018Proton transfer via hydronium and hydroxide ions in water is ubiquitous. It underlies acid-base chemistry, certain enzyme reactions, and even infection by the flu. Despite two-centuries of investigation, the mechanism underlying why hydronium diffuses ... More

Role of Internal Motions and Molecular Geometry on the NMR Relaxation of HydrocarbonsJan 23 2018The role of internal motions and molecular geometry on $^1$H NMR relaxation times $T_{1,2}$ in hydrocarbons is investigated using MD (molecular dynamics) simulations of the autocorrelation functions for in{\it tra}molecular $G_R(t)$ and in{\it ter}molecular ... More

Molecular mechanism of lytic polysaccharide monooxygenasesJan 23 2018The lytic polysaccharide monooxygenases (LPMOs) are copper metalloenzymes that can enhance polysaccharide depolymerization through an oxidative mechanism and hence boost generation of biofuel from e.g. cellulose. By employing density functional theory ... More

Quantized Self-Assembly of Discotic Rings in a Liquid Crystal Confined in NanoporesJan 23 2018Disklike molecules with aromatic cores spontaneously stack up in linear columns with high, one-dimensional charge carrier mobilities along the columnar axes making them prominent model systems for functional, self-organized matter. We show by high-resolution ... More

Adaptive parallelism with RMI: Idle high-performance computing resources can be completely avoidedJan 22 2018In practice, standard scheduling of parallel computing jobs almost always leaves significant portions of the available hardware unused, even with many jobs still waiting in the queue. The simple reason is that the resource requests of these waiting jobs ... More

Comparison of Single-Ion Molecular Dynamics in Common SolventsJan 22 2018Laying a basis for molecularly specific theory for the mobilities of ions in solutions of practical interest, we report a broad survey of velocity autocorrelation functions (VACFs) of Li$^+$ and PF$_6{}^-$ ions in water, ethylene carbonate, propylene ... More

Relativistic Normal Coupled-Cluster Theory for Accurate Determination of Electric Dipole Moments of Atoms: First application to $^{199}$Hg atomJan 22 2018Recent relativistic coupled-cluster (RCC) calculations of electric dipole moments (EDMs) of diamagnetic atoms due to parity and time-reversal violating (P,T-odd) interactions, that are essential ingredients for probing new physics beyond the standard ... More

Chemically stabilized epitaxial wurtzite-BN thin filmJan 22 2018We report on the chemically stabilized epitaxial w-BN thin film grown on c-plane sapphire by pulsed laser deposition under slow kinetic condition. Traces of no other allotropes such as cubic (c) or hexagonal (h) BN phases are present. Sapphire substrate ... More

Transport of secondary electrons through coatings of ion-irradiated metallic nanoparticlesJan 21 2018Feb 05 2018The transport of low-energy electrons through the coating of a radiosensitizing metallic nanoparticle under fast ion irradiation is analyzed theoretically and numerically. As a case study, we consider a poly(ethylene glycol)-coated gold nanoparticle of ... More

Anisotropy enhanced X-ray scattering from solvated transition metal complexesJan 20 2018Time-resolved X-ray scattering patterns from photoexcited molecules in solution are in many cases anisotropic at the ultrafast time scales accessible at X-ray Free Electron Lasers (XFELs). This anisotropy arises from the interaction of a linearly polarized ... More

Ehrenfest statistical dynamics in chemistry: study of decoherence effects and of its equilibrium distributionJan 18 2018We investigate decoherence, pointer states and the equilibrium distribution in the Ehrenfest Statistical Dynamics (ESD) model by considering ensembles of trajectories of simple but realistic molecular models, consisting of two classical cores and one ... More

Controlling polyelectrolyte adsorption onto carbon nanotubes by tuning ion-image interactionsJan 17 2018Understanding and controlling polyelectrolyte adsorption onto carbon nanotubes is a fundamen- tal challenge in nanotechology. Polyelectrolytes have been shown to stabilise nanotube suspensions through adsorbing onto the nanotube surface, and polyelectrolyte-coated ... More

Accurate millimetre and submillimetre rest frequencies for $cis$- and $trans$-dithioformic acid, HCSSHJan 16 2018A better understanding of sulphur chemistry is needed to solve the interstellar sulphur depletion problem. A way to achieve this goal is to study new S-bearing molecules in the laboratory, obtaining accurate rest frequencies for an astronomical search. ... More

Applying machine learning techniques to predict the properties of energetic materialsJan 15 2018Jan 18 2018We present a proof of concept that machine learning techniques can be used to predict the properties of CNOHF energetic molecules from their molecular structures. We focus on a small but diverse dataset consisting of 109 molecular structures spread across ... More

All-solid flexible fiber-shaped lithium ion batteriesJan 15 2018We propose fabrication of the fiber-shaped lithium ion batteries assembled by twisting a cathode filament together with an anode filament. The cathode filament is fabricated by depositing a LiFePO4 (LFP)-composite layer onto a steel-filled polyester conductive ... More

The heteronuclear limit of strong-field ionization: HeH$^+$Jan 15 2018A sophisticated setup for measuring laser-induced fragmentation of an ion beam of helium hydride and an isotopologue at various wavelengths and intensities enables us to study the dynamics of this most fundamental polar molecule. In contrast to the prevailing ... More

Bohmian pathways into chemistry: A brief overviewJan 15 2018Perhaps because of the popularity that trajectory-based methodologies have always had in Chemistry and the important role they have played, Bohmian mechanics has been increasingly accepted within this community, particularly in those areas of the theoretical ... More

Solvophobic and solvophilic contributions in the water-to-aqueous guanidinium chloride transfer free energy of model peptidesJan 15 2018We study the solvation free energy of two different conformations (helix and extended) of two different peptides (deca-alanine and deca-glycine) in two different solvents (water and aqueous guanidinium chloride, GdmCl). The free energies are obtained ... More

Interpretation of the vibrational spectra of glassy polymers using coarse-grained simulationsJan 12 2018Jan 16 2018The structure and vibrational density of states (VDOS) of polymer glasses are investigated using numerical simulations based on the classical Kremer-Grest bead-spring model. We focus on the roles of chain length and bending stiffness, the latter being ... More

Reaction mechanism of hydrogen activation by frustrated Lewis pairsJan 11 2018Typically, a Lewis acid and a base react with each other and form classic acid base adducts. The neutralization reaction is however prevented by the introduction of bulky substitutes and this interesting finding leads to a new concept called frustrated ... More

Recent Advances in Computational Modeling of ThrombosisJan 06 2018The study of thrombosis is crucial to understand and develop new therapies for diseases like deep vein thrombosis, diabetes related strokes, pulmonary embolism etc. The last two decades have seen an exponential growth in studies related to the blood clot ... More

Lithiation of Silicon Anode based on Soft X-ray Emission Spectroscopy: A Theoretical StudyJan 06 2018Due to its exceptional lithium storage capacity silicon is considered as a promising candidate for anode material in lithium-ion batteries (LIBs). In the present work we demonstrate that methods of the soft X-ray emission spectroscopy (SXES) can be used ... More

PHOENICS: A universal deep Bayesian optimizerJan 04 2018In this work we introduce PHOENICS, a probabilistic global optimization algorithm combining ideas from Bayesian optimization with concepts from Bayesian kernel density estimation. We propose an inexpensive acquisition function balancing the explorative ... More

Probing resonant energy transfer in collisions of ammonia with Rydberg helium atoms by microwave spectroscopyJan 04 2018We present the results of experiments demonstrating the spectroscopic detection of F\"{o}rster resonance energy transfer from NH$_3$ in the $X\,^1A_1$ ground electronic state to helium atoms in 1s$n$s\,$^3$S$_1$ Rydberg levels, where $n=37$ and $n=40$. ... More

Quantum Monte Carlo calculations of van der Waals interactions between aromatic benzene ringsJan 03 2018The magnitude of finite-size effects and Coulomb interactions in quantum Monte Carlo simulations of van der Waals interactions between weakly bonded benzene molecules are investigated. We assess the impact of the backflow coordinate transformation to ... More

Orientational dependence of the van der Waals interactions for finite-sized particlesJan 03 2018Van der Waals forces as interactions between neutral and polarisable particles act at small distances between two objects. Their theoretical origin lies in the electromagnetic interaction between induced dipole moments caused by the vacuum fluctuations ... More

An experimental water line list at 1950 K in the 6250 -- 6670 \cm\ regionDec 26 2017An absorption spectrum of H$_2$$^{16}$O at 1950 K is recorded in a premixed methane/air flat flame using a cavity-enhanced optical frequency comb-based Fourier transform spectrometer. 2417 absorption lines are identified in the 6250 -- 6670 cm region ... More

Probing frontier orbital energies of (Co9(P2W15)3) polyoxometalate clusters at molecule-metal and molecule-water interfacesDec 25 2017Functionalization of polyoxotungstates with organoarsonate co-ligands enabling surface decoration was explored for the triangular cluster architectures of the composition [CoII9(H2O)6(OH)3(p-RC6H4AsVO3)2({\alpha}-PV2WVI15O56)3]25-({Co9(P2W15)3}, R = H ... More

Non-equilibrium effects on thermal ignition using molecular dynamics simulationsDec 21 2017The present study addresses the role of molecular non-equilibrium effects in thermal ignition problems. We consider a single binary reaction of the form $A+B \rightarrow C+C$. Molecular dynamics calculations were performed for activation energies ranging ... More

MSM/RD: Coupling Markov state models of molecular kinetics with reaction-diffusion simulationsDec 21 2017Molecular dynamics (MD) simulations can model the interactions between macromolecules with high spatiotemporal resolution but at a high computational cost. By combining high-throughput MD with Markov state models (MSMs), it is now possible to obtain statistically ... More

WACSF - Weighted Atom-Centered Symmetry Functions as Descriptors in Machine Learning PotentialsDec 15 2017We introduce weighted atom-centered symmetry functions (wACSFs) as descriptors of a chemical system's geometry for use in the prediction of chemical properties such as enthalpies or potential energies via machine learning. The wACSFs are based on conventional ... More

Step bunching with both directions of the current: Vicinal W(110) surfaces versus atomistic scale modelDec 13 2017Dec 31 2017We report for the first time the observation of bunching of monoatomic steps on vicinal W(110) surfaces induced by step up or step down currents across the steps. Measurements reveal that the size scaling exponent {\gamma}, connecting the maximal slope ... More

Charcoal obtained from cherry stones in different carbonisation atmospheresDec 12 2017Dec 17 2017The exploitation of using agro-industrial residues as the cherry stone to produce charcoal and activated carbon is very relevant nowadays due to the high demand of these materials. This work describes the methods to prepare charcoal from cherry stones ... More

High permittivity processed SrTiO3 for metamaterials applications at terahertz frequenciesNov 28 2017High permittivity SrTiO3 for the realization of all-dielectric metamaterials operating at terahertz frequencies was fabricated. A comparison of different processing routes evidences that Spark Plasma Sintering is the most effective sintering process to ... More

A free energy landscape of the capture of CO2 by frustrated Lewis pairsNov 14 2017Frustrated Lewis pairs (FLPs) are known for its ability to capture CO2. Although many FLPs have been reported experimentally and several theoretical studies have been carried out to address the reaction mechanism, the individual roles of Lewis acids and ... More

Investigating the importance of edge-structure in the loss of H/H2 of PAH cations: the case of dibenzopyrene isomersNov 08 2017We present a detailed study of the main dehydrogenation processes of two dibenzopyrene cation (C24H14+) isomers, namely dibenzo(a,e)pyrene (AE+) and dibenzo(a,l)pyrene (AL+). First, action spectroscopy under VUV photons was performed using synchrotron ... More

A nucleobase-centered coarse-grained representation for structure prediction of RNA motifsNov 02 2017Dec 06 2017We introduce the SPlit-and-conQueR (SPQR) model, a coarse-grained representation of RNA designed for structure prediction and refinement. In our approach, the representation of a nucleotide consists of a point particle for the phosphate group and an anisotropic ... More

A cryofuge for cold-collision experiments with slow polar moleculesOct 16 2017Ultracold molecules represent a fascinating research frontier in physics and chemistry, but it has proven challenging to prepare dense samples at low velocities. Here we present a solution to this goal by a non-conventional approach dubbed cryofuge. It ... More

Effective Polarisability ModelsOct 13 2017Theories for the effective polarisability of a small particle in a medium are presented using different levels of approximation: we consider the virtual cavity, real cavity and the hard-sphere models as well as a continuous interpolation of the latter ... More

Coulomb explosion imaging of concurrent CH$_{2}$BrI photodissociation dynamicsOct 06 2017The dynamics following laser-induced molecular photodissociation of gas-phase CH$_{2}$BrI at 271.6 nm were investigated by time-resolved Coulomb explosion imaging using intense near-IR femtosecond laser pulses. The observed delay-dependent photofragment ... More

Multi-dimensional Tensor Network Simulation of Open Quantum Dynamics in Singlet FissionOct 03 2017We develop a powerful tree tensor network states method that is capable of simulating exciton-phonon quantum dynamics of larger molecular complexes and open quantum systems with multiple bosonic environments. We interface this method with ab initio density ... More

High accuracy calculations of the rotation-vibration spectrum of H$_3^+$Sep 21 2017Calculation of the rotation-vibration spectrum of H3+, as well as of its deuterated isotopologues, with near-spectroscopic accuracy requires the development of sophisticated theoretical models, methods, and codes. The present paper reviews the state-of-the-art ... More

Non-Adiabatic Vibrational Damping of Molecular Adsorbates: Insights into Electronic Friction and the Role of Electronic CoherenceSep 20 2017We present a perturbation approach rooted in time-dependent density-functional theory to calculate electron hole (eh)-pair excitation spectra during the non-adiabatic vibrational damping of adsorbates on metal surfaces. Our analysis for the benchmark ... More

Exact combinatorial approach to finite coagulating systemsSep 16 2017Sep 23 2017The paper outlines an exact combinatorial approach to finite coagulating systems. In this approach, cluster sizes and time are discrete, and the binary aggregation alone governs the time evolution of the systems. By considering the growth histories of ... More

Kinetics of the simplest Criegee intermediate reaction with ozone studied by mid-infrared quantum cascade laser spectrometerSep 07 2017Nov 21 2017The kinetics of CH$_2$OO reaction with ozone has been studied by monitoring CH$_2$OO with time-resolved infrared (IR) absorption spectroscopy, which utilized fast chirped IR pulse train from a quantum cascade laser [J. Chem. Phys. 146, 244302 (2017)]. ... More

Fragmentation of Fullerenes to Linear Carbon ChainsSep 01 2017Small cationic fullerene fragments, produced by electron impact ionization of C60, were mass-selected and accumulated in cryogenic Ne matrixes. Optical absorption spectroscopy of these fragments with up to 18 carbon atoms revealed linear structures. Considering ... More

How Do Methyl Groups Enhance the Triplet Chemiexcitation Yield of Dioxetane?Aug 10 2017Chemiluminescence is the emission of light as a result of a nonadiabatic chemical reaction. The present work is concerned with understanding the yield of chemiluminescence, in particular how it dramatically increases upon methylation of 1,2-dioxetane. ... More

Assessing impacts of discrepancies in model parameters on autoignition model performance: a case study using butanolAug 07 2017Dec 24 2017Side-by-side comparison of detailed kinetic models using a new tool to aid recognition of species structures reveals significant discrepancies in the published rates of many reactions and thermochemistry of many species. We present a first automated assessment ... More

Density Functional Theory of doped superfluid liquid helium and nanodropletsAug 05 2017During the last decade, density function theory (DFT) in its static and dynamic time dependent forms, has emerged as a powerful tool to describe the structure and dynamics of doped liquid helium and droplets. In this review, we summarize the activity ... More

Rovibrational quantum dynamical computations for deuterated isotopologues of the methane-water dimerAug 03 2017Rovibrational states of the four dimers formed by the light and the heavy isotopologues of the methane and the water molecules are computed using a potential energy surface taken from the literature. The general rovibrational energy-level pattern characteristic ... More

Mapping the Free Energy of Lithium Solvation in the Protic Ionic Liquid Ethylammonuim Nitrate: A Metadynamics StudyAug 01 2017Understanding lithium solvation and transport in ionic liquids is important due to their possible application in electrochemical devices. Using first-principles simulations aided by a metadynamics approach we study the free-energy landscape for lithium ... More

Machine Learning for Quantum Dynamics: Deep Learning of Excitation Energy Transfer PropertiesJul 20 2017Understanding the relationship between the structure of light-harvesting systems and their excitation energy transfer properties is of fundamental importance in many applications including the development of next generation photovoltaics. Natural light ... More

High resolution quantum cascade laser spectroscopy of the simplest Criegee intermediate, CH$_2$OO, between 1273 cm$^{-1}$ and 1290 cm$^{-1}$Jun 12 2017Jun 27 2017The region 1273-1290 cm$^{-1}$ of the $\nu$4 fundamental of the simplest Criegee intermediate, CH$_2$OO, has been measured using a quantum cascade laser transient absorption spectrometer, which offers greater sensitivity and spectral resolution (< 0.004 ... More

Structural evolution of CO2 filled pure silica LTA zeolite under high-pressure high-temperature conditionsMay 30 2017The crystal structure of CO2 filled pure SiO2 LTA zeolite has been studied at high pressures and temperatures using synchrotron based x ray powder diffraction. Its structure consists of 13 CO2 guest molecules, 12 of them accommodated in the large alpha ... More

Absence of selection for quantum coherence in the Fenna-Matthews-Olson complex: a combined evolutionary and excitonic studyMay 02 2017We present a study on the evolution of the Fenna-Matthews-Olson bacterial photosynthetic pigment-protein complex. This protein complex functions as an antenna. It transports absorbed photons - excitons - to a reaction center where photosynthetic reactions ... More

How good is the generalized Langevin equation to describe the dynamics of photo-induced electron transfer in fluid solution?Apr 20 2017The dynamics of unimolecular photo-triggered reactions can be strongly affected by the surrounding medium. An accurate description of these reactions requires knowing the free energy surface (FES) and the friction felt by the reactants. Most of theories ... More

Ultrafast charge transfer processes accompanying KLL Auger decay in aqueous KCl solutionMar 31 2017X-ray photoelectron spectroscopy (XPS) and KLL Auger spectra of aqueous KCl solution were measured for the K$^+$ and Cl$^-$ edges. While the XPS spectra of potassium and chloride have similar structures, both exhibiting only weak satellite structures ... More

Experimental measurement of binding energy, selectivity and allostery using fluctuation theoremsMar 30 2017Thermodynamic bulk measurements of binding reactions critically rely on the validity of the law of mass action and the assumption of a dilute solution. Yet important biological systems such as allosteric ligand-receptor binding, macromolecular crowding, ... More

Electro-Oxidation of Ni42 Steel: A highly Active Bifunctional ElectrocatalystMar 21 2017Janus type Water-Splitting Catalysts have attracted highest attention as a tool of choice for solar to fuel conversion. AISI Ni 42 steel was upon harsh anodization converted in a bifunctional electrocatalyst. Oxygen evolution reaction- (OER) and hydrogen ... More

Analytical calculation of the axis angle 2V from extinction measurements on the spindle stageFeb 27 2017A concise derivation of the "Joel equations", which allow for the determination of the axis angle 2V from measurements of extinction directions on a spindle stage, is provided starting from the wave-equation. Only analytic methods and no geometric arguments ... More

A comparison between quantum chemistry and quantum Monte Carlo techniques for the adsorption of water on the (001) LiH surfaceFeb 21 2017May 09 2017We present a comprehensive benchmark study of the adsorption energy of a single water molecule on the (001) LiH surface using periodic coupled cluster and quantum Monte Carlo theories. We benchmark and compare different implementations of quantum chemical ... More

Novel polystyrene-based nanocomposites by phosphorene dispersionFeb 14 2017Polystyrene-based phosphorene nanocomposites were prepared by a solvent blending procedure allowing the embedding of black phosphorus (BP) nanoflakes in the polymer matrix. Raman spectroscopy, X Ray Diffraction and TEM microscopy were employed to characterize ... More

PAH chemistry at eV internal energies. 1. H-shifted isomersFeb 14 2017The PAH family of organic compounds (polycyclic aromatic hydrocarbons), involved in several fields of chemistry, has received particular attention in astrochemistry, where their vibrational spectroscopy, thermodynamic, dynamic, and fragmentation properties ... More

PAH chemistry at eV internal energies. 2. Ring alteration and dissociationFeb 13 2017Apr 19 2017Recognized as important interstellar constituents, polycyclic aromatic hydrocarbons (PAHs) have been intensively studied in astrochemistry and their spectroscopy, thermodynamics, dynamics, and fragmentations are now amply documented. There exists typical ... More

Spectral focusing of broadband silver electroluminescence in nanoscopic FRET-LEDsFeb 13 2017Few inventions have shaped the world like the incandescent bulb. While Edison used thermal radiation from ohmically heated conductors, some noble metals exhibit "cold" electroluminescence (EL) in percolation films, tunnel diodes, electromigrated nanoparticle ... More

Perturbation of Exciton Aggregate Coupling by Optical Excitation in Crystalline Perfluoropentacene FilmsDec 15 2016Carrier multiplication by singlet exciton fission enhances photovoltaic conversion efficiencies in organic solids. This decay of one singlet exciton into two triplet states promises to overcome the Shockley-Queisser limit as up to two electrons may be ... More

Control of Intramolecular Electron Transfer in Perylene Dihydrazides and Perylene Diimides: A Comparative Study by Time-Resolved SpectroscopyDec 15 2016Electron transfer (ET) in molecular donor-acceptor dye systems is crucial for charge transport in organic semiconductors. Classically, ET rates should decrease with increasing donor-acceptor distance while the microscopic mechanism is more complex and ... More

Differentiation between shallow and deep charge trap states on single poly(3-hexylthiophene) chains through fluorescence photon statisticsDec 09 2016Blinking of the photoluminescence (PL) emitted from individual conjugated polymer chains is one of the central observations made by single-molecule spectroscopy (SMS). Important information, e.g., regarding excitation energy transfer, can be extracted ... More

Search for Interstellar monohydric ThiolsDec 08 2016It has been pointed out by various astronomers that very interesting relationship exists between interstellar alcohols and the corresponding thiols (sulfur analogue of alcohols) as far as the spectroscopic properties and chemical abundances are concerned. ... More

Quantum embedding theoriesDec 08 2016In complex systems, it is often the case that the region of interest forms only one part of a much larger system. The idea of joining two different quantum simulations - a high level calculation on the active region of interest, and a low level calculation ... More

Controlling charge transfer in ultracold gases via Feshbach resonancesDec 08 2016We investigate the prospects of controlling charge-exchange in ultracold collisions of heteroisotopic combinations of atoms and ions of the same element. The treatment, readily applicable to alkali or alkanine-earth metals, is illustrated in the process ... More