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Wyniki wyszukiwania dla: physical organic chemistry
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On the Possibility of the Amphotericin B-Sterol Complex Formation in Cholesterol- and Ergosterol-Containing Lipid Bilayers: A Molecular Dynamics Study
PublikacjaAmphotericin B (AmB) is a well-known membrane-active antibiotic that has been used to treat systemicfungal infections for more than 45 years. Therapeutic application of AmB is based on the fact that it is moreactive against ergosterol-containing membranes of fungal cells than against mammalian membranes withcholesterol. In this paper, we examine the hypothesis according to which the selectivity of the AmB's membraneaction originates...
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Electron attachment and electron iozization of acetic acid clusters embedded in helium nanodroplets
PublikacjaThe effect of incident electrons on acetic acid clusters is explored for the first time. The acetic acid clusters are formed inside liquid helium nanodroplets and both cationic and anionic productsejected in to the gas phase aredetected by mass spectrometry.
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Visible-light-induced photocatalysis through surface Plasmon excitation of gold on titania surfaces
PublikacjaPietnascie komercyjnych probek tlenku tytanu(IV) zostalo zmodyfikowanych zlotem za pomoca fotodepozycji oraz scharakteryzowanych. Fotoaktywnosci proszkow Au/TiO2 zostaly przebadane dla fotodegradacji kwasu octowego i 2-propanolu podczas naswietlania promieniowaniem widzialnym oraz ultrafioletowym. Wykazano, ze fotokatalityczne aktywnosci scisle zaleza od wlasciwosci nanoczastek zlota i tlenku tytanu. Analizy spektrum działania...
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A XAS study of a highly diluted Pt electrocatalyst operating in PEM fuel cells
PublikacjaWe present an X-ray absorption spectroscopy (XAS) study of a low Pt content catalyst layer(Pt loading 0.1 mg c2) operating at the cathode of a proton exchange membrane fuel cell(PEMFC). This catalyst is based on the use of a mesoporous inorganic matrix as a support forthe catalyst Pt nanoparticles. Due to the high Pt dilution, in situ measurements of itsstructural properties by XAS are challenging and suitable experimental strategies...
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Structural properties of hydration shell around various conformations of simple polypeptides
PublikacjaIn this paper we investigate structural properties of water within the solvation shell around the peptide core created by a well-defined conformation of polypeptide chain. The following secondary structures are investigated: linear (straight chain), and three helices PII (polyproline-like), 310, and α. We propose using the two-particle contribution to entropy as a rational measure of the water structural ordering within the solvation...
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Study of Phase Transformation Processes Occurring in the Nanocrystalline Iron/Ammonia/Hydrogen System by the Magnetic Permeability Measurement Method
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Promotion of Photocatalytic Hydrogen Evolution under Visible Light with NiO/C Fabricated via a Super Facile and General Strategy
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A new Apporoach to the Spectral Analysis of Liquid Membrane Oscillators by Gabor Transformation
PublikacjaOcylatory z membrana ciekłą charakteryzują się nieregularnymi oscylacjami. Widma mocy nie mogą być ustalone za pomocą transformacji Fourier'a do oscylacji niestacjonarnej. Zaprezentowano nowe podejście pozwalające tych przypadkach otrzymać widma mocy. Analizę tę zastosowano do oscylatorów z membraną ciekłą, zawierających kationowy surfaktant. Stwierdzono, że obecnośc róznych dodanych substancji do wodnej fazy akceptorowej wpływa...
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Preferential solvation in (amide+alcohol) binary mixtures. Part 2. The N-methylpyrrolidinone+methanol mixture at T = 313.15 K: thermodynamic resultsand molecular dynamics calculations.
PublikacjaBadano zjawisko preferencyjnej solwatacji amidu (N-metylopyrrolidonu) przez metanol wykorzystując dwie uzupełniające się metody: bezpośrednich pomiarów własności termodynamicznych roztworu oraz symulacji komputerowych. W metodzie pierwszej dokonano pomiarów wielkości termodynamicznych takich jak: nadmiarowa energia swobodna mieszania, nadmiarowa objętość mieszania oraz współczynnika ściśliwości izotermicznej mieszaniny,...
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Preferential solvation in (amide+alcohol) binary mixtures. Part 1. The N- methylpyrrolidinone+ethanol mixture at T = 313.15 K: thermodynamic resultsand molecular dynamics calculations.
PublikacjaBadano zjawisko preferencyjnej solwatacji amidu (N-metylopyrrolidonu) przez etanol wykorzystując dwie uzupełniające się metody: bezpośrednich pomiarów własności termodynamicznych roztworu oraz symulacji komputerowych. W metodzie pierwszej dokonano pomiarów wielkości termodynamicznych takich jak: nadmiarowa energia swobodna mieszania, nadmiarowa objętość mieszania oraz współczynnika ściśliwości izotermicznej mieszaniny,...
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Solvation of N-methylformamide by ethanol: a comparison of molecular dynamics calculations with the experimental data
PublikacjaWykonano obliczenia metodami dynamiki molekularnej dla tytułowego układu. Rezultaty porównano z uzyskanymi wcześniej wynikami pomiarów termodynamicznych oraz wnioskami z nich wyciągniętymi.
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Raman spectroscopic study of Ni2+-DNA interactions in aqueous systems
PublikacjaMetodą ramanowskich widm różnicowych określono sposób oddziaływania jonu Ni2+ z DNA(CT) w układach wodnych. Kation Ni(II) koordynuje w pozycjach N7 guaniny (G) i adeniny (A) w powtarzających się sekwencjach GG, AA i GA cząsteczki DNA. Jednocześnie Ni2+ oddziałuje zewnątrz sferowo poprzez cząsteczki wody z grupami fosforanowymi DNA.
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Radiative lifetime of a BODIPY dye as calculated by TDDFT and EOM-CCSD methods: solvent and vibronic effects
PublikacjaThe radiative emission lifetime and associated S1 excited state properties of a BODIPY dye are investigated with TDDFT and EOM-CCSD calculations. The effects of a solvent are described with the polarizable continuum model using the linear response (LR) approach as well as state-specific methods. The Franck–Condon (FC), Herzberg–Teller (HT) and Duschinsky vibronic effects are evaluated for the absorption and emission spectra, and...
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Anionic states of C6Cl6 probed in electron transfer experiments
PublikacjaThis is the first comprehensive investigation on the anionic species formed in collisions of fast neutral potassium (K) atoms with neutral hexachlorobenzene (C6Cl6) molecules in the laboratory frame range from 10 up to 100 eV. In such ion-pair formation experiments, we also report a novel K+ energy loss spectrum obtained in the forward scattering giving evidence of the most accessible electronic states. The vertical electron affinity...
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Determinants of Directionality and Efficiency of the ATP Synthase Fo Motor at Atomic Resolution
PublikacjaFo subcomplex of ATP synthase is a membrane-embedded rotary motor that converts proton motive force into mechanical energy. Despite a rapid increase in the number of high-resolution structures, the mechanism of tight coupling between proton transport and motion of the rotary c-ring remains elusive. Here, using extensive all-atom free energy simulations, we show how the motor’s directionality naturally arises from the interplay...
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Guanosine Dianions Hydrated by One to Four Water Molecules
PublikacjaIntermolecular interactions such as those present in molecule···water complexes may profoundly influence the physicochemical properties of molecules. Here, we carried out an experimental–computational study on doubly deprotonated guanosine monophosphate···water clusters, [dGMP – 2H]2–·nH2O (n = 1–4), using a combination of negative anion photoelectron spectroscopy (NIPES) with molecular dynamics (MD) and quantum chemical (QM) calculations....
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Practical Approach to Large-Scale Electronic Structure Calculations in Electrolyte Solutions via Continuum-Embedded Linear-Scaling Density Functional Theory
PublikacjaWe present the implementation of a hybrid continuum-atomistic model for including the effects of a surrounding electrolyte in large-scale density functional theory (DFT) calculations within the Order-N Electronic Total Energy Package (ONETEP) linear-scaling DFT code, which allows the simulation of large complex systems such as electrochemical interfaces. The model represents the electrolyte ions as a scalar field and the solvent...
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Enhanced Charge Storage Mechanism And Long-Term Cycling Stability In Diamondized Titania Nanocomposite Supercapacitors Operating In Aqueous Electrolytes
PublikacjaThe long cycle life stability jointly with high energy density are limiting broader feasible applications of supercapacitors. The novel diamondized titania nanocomposite supercapacitors deliver high power and energy densities along with high capacitance retention rates. Supercapacitor electrodes were fabricated utilizing a combination of Ti anodization followed by chemical vapor deposition resulting in simultaneous growth of complex...
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Charge Transport in High-Entropy Oxides
PublikacjaThis work presents the results of research on the transport properties of the high-entropy BaZr1/8Hf1/8Sn1/8Ti1/8Y1/8In1/8Sm1/8Yb1/8O3–x perovskite oxide with special focus on proton transport. The presented study is part of broader work in which we focus on multiple different chemical compositions with the cation number varying from 5 up to 12 (in B-sublattice). The presence of proton defects is analyzed with thermogravimetry,...
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Water uptake and energetics of the formation of barium zirconate based multicomponent oxides
PublikacjaA group of multi-component oxides based on BaZrO3 have been prepared using a solid-state reaction method and examined in terms of their water uptake and thermodynamics of formation. Depending on the type and amount of acceptor substitution, the synthesized compounds exhibit various proton defect concentrations, reaching up to 0.2 mol/mol for a compound containing 10 different elements in the B-sublattice, where 50% of them are...
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Superconductivity in Bismuth Pyrochlore Lattice Compounds RbBi2 and CsBi2: The Role of Relativistic Effects
PublikacjaSuperconducting properties of two bismuthide intermetallic compounds, RbBi2 and CsBi2, were studied by means of experimental measurements and ab initio calculations. We show that in both compounds, the superconductivity emerges from the pyrochlore Bi lattice and its formation is heavily influenced by relativistic effects. Based on our analysis of the effect of spin–orbit coupling on the electron–phonon coupling, we suggest a possible...
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Band Gap Engineering toward Semimetallic Character of Quinone-Rich Polydopamine
PublikacjaSemiconductor|melanin interfaces have received increasingly more attention in the fields of photocatalysis and applied electrochemistry because of their facile synthesis, unique electrical properties, and strong capability toward photosensitization. In this work, we describe the electropolymerization of quinone-rich polydopamine (PDA) on the surface of hydrogenated TiO2 nanotubes with enhanced photoactivity in the visible spectrum....
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Proton conductivity in multi-component ABO4-type oxides
PublikacjaThis work investigates how configurational entropy in oxides could affect proton conductivity. For this purpose, three samples of different elemental compositions are synthesized. Five, six and seven elements were introduced into the A-site of ANbO4, forming La1/5 Nd1/5 Sm1/5Gd1/5 Eu1/5NbO4, La1/6Nd1/6Sm1/6Gd1/6Eu1/6Ho1/6NbO4 and La1/7Nd1/7Sm1/7Gd1/7Eu1/7Ho1/7Er1/7NbO4, respectively. The high configuration disorder changes the...
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Dissociative Electron Attachment to 5-Iodo-4-thio-2′-deoxyuridine: A Potential Radiosensitizer of Hypoxic Cells
PublikacjaIn the search for effective radiosensitizers for tumor cells, halogenated uracils have attracted more attention due to their large cross section for dissociation upon the attachment of low-energy electrons. In this study, we investigated dissociative electron attachment (DEA) to 5-iodo-4-thio-2'-deoxyuridine, a potential radiosensitizer using a crossed electron-molecule beam experiment coupled with quadrupole mass spectrometry....
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Tuning the work function of graphite nanoparticles via edge termination
PublikacjaGraphite nanoparticles are important in energy materials applications such as lithium-ion batteries (LIBs), supercapacitors and as catalyst supports. Tuning the work function of the nanoparticles allows local control of lithiation behaviour in LIBs, and the potential of zero charge of electrocatalysts and supercapacitors. Using large scale density functional theory (DFT) calculations, we find that the surface termination of multilayer...
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Surprising Radiolytic Stability of 8‑Thiomethyladenine in an Aqueous Solution
Publikacja8-Thiomethyladenine (ASCH3), a potentially radiosensitizing modified nucleobase, has been synthesized in a reaction between 8-thioadenine and methyl iodide. Despite favorable dissociative electron attachment (DEA) characteristics, the radiolysis of an aqueous solution of ASCH3 with a dose of X-ray amounting to as much as 300 Gy leads to no effects. Nevertheless, crossed electron-molecule beam experiments in the gas phase on ASCH3...
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Why Are Left-Handed G-Quadruplexes Scarce?
PublikacjaG-quadruplexes (G4s) are nucleic acid structures crucial for the regulation of gene expression and genome maintenance. While they hold promise as nanodevice components, achieving desired G4 folds requires understanding the interplay between stability and structural properties, like helicity. Although right-handed G4 structures dominate the experimental data, the molecular basis for this preference over left-handed helicity is unclear....
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Few-Layer Black Phosphorus/Chitosan Nanocomposite Electrodes via Controlled Electrodeposition for Enhanced Electrochemical Kinetic Performance
PublikacjaThis study presents the preparation and characterization of few-layer black phosphorus (FLBP) chitosan electrodes by controlled electrochemical deposition of chitosan nanoparticles on FLBP-modified glassy carbon electrodes. FLBP was prepared by solvent-assisted exfoliation of bulk BP and was further modified with chitosan forming together a nanocomposite, including easy cross-linking with nanomaterials and film-forming properties....
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Graph Neural Networks and Structural Information on Ionic Liquids: A Cheminformatics Study on Molecular Physicochemical Property Prediction
PublikacjaIonic liquids (ILs) provide a promising solution in many industrial applications, such as solvents, absorbents, electrolytes, catalysts, lubricants, and many others. However, due to the enormous variety of their structures, uncovering or designing those with optimal attributes requires expensive and exhaustive simulations and experiments. For these reasons, searching for an efficient theoretical tool for finding the relationship...
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Two-body dissociation of isoxazole following double photoionization – an experimental PEPIPICO and theoretical DFT and MP2 study
PublikacjaThe dissociative double photoionization of isoxazole molecules has been investigated experimentally and theoretically. The experiment has been carried out in the 27.5–36 eV photon energy range using vacuum ultraviolet (VUV) synchrotron radiation excitation combined with ion time-of-flight (TOF) spectrometry and photoelectron–photoion–photoion coincidence (PEPIPICO) technique. Five wellresolved two-body dissociation channels have...
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Core–shell excitation of isoxazole at the C, N, and O K-edges – an experimental NEXAFS and theoretical TD-DFT study
PublikacjaThe near-edge X-ray absorption fine structure (NEXAFS) spectra of the gas-phase isoxazole molecule have been measured by collecting total ion yields at the C, N, and O K-edges. The spectral structures have been interpreted using time-dependent density functional theory (TD-DFT) with the short-range corrected SRC2-BLYP exchange–correlation functional. Experimental and calculated energies of core excitations are generally in good...
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Early Stages of RNA-Mediated Conversion of Human Prions
PublikacjaPrion diseases are characterized by the conversion of prion proteins from a PrPC fold into a disease-causing PrPSC form that is self-replicating. A possible agent to trigger this conversion is polyadenosine RNA, but both mechanism and pathways of the conversion are poorly understood. Using coarse-grained molecular dynamic simulations we study the time evolution of PrPC over 600 μs. We find that both the D178N mutation and interacting...
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Properties of Oxygen Vacancy and Hydrogen Interstitial Defects in Strontium Titanate: DFT + Ud,p Calculations
PublikacjaThis work presents extensive theoretical studies focused on the mixed ion-electron transport in cubic strontium titanate (STO). A new approach to the description of this difficult system was developed within the framework of linear-scaling Kohn–Sham density functional theory, as realized in the ONETEP program. The description we present is free of any empirical parameters and relies on the Hubbard U and Hund’s J corrections applied...
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Linear and Nonlinear Optical Properties of Azobenzene Derivatives Modified with an (Amino)naphthalene Moiety
PublikacjaThe design of two-photon absorbing azobenzene (AB) derivatives has received much attention; however, the two-photon absorption (2PA) properties of bis-conjugated azobenzene systems are relatively less explored. Here, we present the synthesis of six azobenzene derivatives and three bisazobenzenes substituted (or not) at para position(s) with one or two amino group(s). Their linear and nonlinear absorption properties are studied...
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Atomic-Scale Finite-Element Modeling of Elastic Mechanical Anisotropy in Finite-Sized Strained Phosphorene Nanoribbons
PublikacjaNanoribbons are crucial nanostructures due to their superior mechanical and electrical properties. This paper is devoted to hybrid studies of the elastic mechanical anisotropy of phosphorene nanoribbons whose edges connect the terminals of devices such as bridges. Fundamental mechanical properties, including Young’s modulus, Poisson’s ratio, and density, were estimated from first-principles calculations for 1-layer, 3-layer, and...
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Integrated Experimental and Theoretical Approach for Efficient Design and Synthesis of Gold-Based Double Halide Perovskites
PublikacjaApplied cutting-edge electronic structure and phonon simulations provide a reliable knowledge about the stability of perovskite structures and their electronic properties, which are crucial for design of effective nanomaterials. Gold is one of the exceptional elements, which can exist both as a monovalent and a trivalent ion in the B site of a double perovskite such as A2BI BIIIX6. However, until now, electronic properties of Cs2AuI AuIIIX6...
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Non-ergodic fragmentation upon collision-induced activation of cysteine–water cluster cations
PublikacjaCysteine–water cluster cations Cys(H2O)3,6 + and Cys(H2O)3,6H+ are assembled in He droplets and probed by tandem mass spectrometry with collision-induced activation. Benchmark experimental data for this biologically important system are complemented with theory to elucidate the details of the collisioninduced activation process. Experimental energy thresholds for successive release of water are compared to water dissociation energies...
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The importance of the shape of the protein-water interface of a kinesin motor domain for dynamics of the surface atoms of the protein
PublikacjaSingle kinesin motor domain immersed in water has been investigated using molecular dynamics. It has been found that local properties of water in solvation shell change along with the nature of neighboring protein surface. However, a detailed analysis leads to the conclusion that the geometrical features of hydrogen bonds and overall structure of kinesin hydration water is not very different from bulk water. The local values of...
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Why the solvation water around proteins is more dense than bulk water
PublikacjaThe main aim of this work is to propose a rational explanation of commonly observed phenomenon of increasing water density within solvation shell of proteins. We have observed that geometry of the water-water hydrogen bond network within solvation layer differs from the one in bulk water and it is the effect of interactions of water molecules with protein surface. Altered geometry of the network reflects changes in the structure...
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Concentration-Dependent Fluorescence Properties of Rhodamine 6G in Titanium Dioxide and Silicon Dioxide Nanolayers
PublikacjaWytworzono cienkie warstwy zawierające rodaminę 6G w dwutlenku tytanu (R6G/TiO2) i w dwutlenku krzemu (R6G/SiO2) stosując metodę zol-żel. Badane były dwa rodzaje matryc, w których domieszkowano barwnik rodamina 6G (R6G) o różnych koncentracjach. Został stwierdzony istotny wpływ koncentracji barwnika na widma absorpcji i emisji oraz na czasowo rozdzielone widma fluorescencji. W szczególności stwierdzono znacznie mniejszą zdolność...
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Local Ordering Changes in Pt-Co Nanocatalyst Induced by Fuel Cell Working Conditions
PublikacjaPraca poświęcona jest szczegółowej analizie zmian w lokalnej strukturze atomowej i elektronowej nanocząstek Pt-Co pracujących jako katalizatory w polimerowych ogniwach paliwowych wywołanych cyklicznie zmieniającymi się warunkami pracy ogniwa. Do analizy wykorzystano badania XAS realizowane ex-situ i in-situ, XRD i TEM. Analizując widma XAFS wzięto pod uwagę możliwy wpływ nieporządku chemicznego oraz redukcję liczb koordynacyjnych...
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Limonene: electronic state spectroscopy by high-resolution vacuum ultraviolet photoabsorption, electron scattering, He(I) photoelectron spectroscopy and ab initio calculations
PublikacjaZbadano limonen metodami spektroskopii absorpcyjnej, elektronowej, fotojonizacyjnej. Wyniki porównano z obliczeniami ab initio. Otrzymano strukturę wibracyjną molekuły.
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A Novel Ru(II) Polypyridine Black Dye Investigated by Resonance Raman Spectroscopy and TDDFT Calculations
PublikacjaThe optical properties of a new(bipyridine)2Ru(4H-imidazole) complex presenting a remarkablebroad absorption in the visible range are investigated. Thestrong overlap of the absorption with the solar radiationspectrum renders the studied complex promising as a blackabsorber and hence as a starting structure for applications inthe field of dye-sensitized solar cells. The correlations betweenstructural and electronic features for...
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Theoretical Design of the Molecular Structure of Bent-Core Mesogens with Large Second-Order Nonlinear Optical Properties
PublikacjaABSTRACT: The first hyperpolarizability of two series of moleculeswith bent-shaped structures has been calculated at the ab initio level.The two series consist of carboxyl derivatives for which somemolecules are known to exhibit banana phases and of their sulfinatehomologues that have not been synthesized yet. The final purpose isto reveal the relevance or not in synthesizing these latter molecules.The strategy is based on reporting...
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Structural Control of Photoinduced Dynamics in 4H-Imidazole- Ruthenium Dyes
PublikacjaThe photoinduced dynamics of a series ofterpyridine 4H-imidazole-ruthenium complexes, which constitutea new family of panchromatic dyes, is investigated. Thedynamics involves two excited states localized within the 4Himidazolesphere. Upon MLCT excitation, an excited state ispopulated, which is localized on the central part of the 4Himidazoleligand caused by its nonplanar conformation. Thepopulation of the second excited state is...
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Influence of temperature and interactions with ligands on dissociation of dsDNA and ligand-dsDNA complexes of various types of binding : an electrochemical study.
PublikacjaSeveral medicinally important compounds that bind to dsDNA strands via intercalation (C-1311, C-1305, EtBr), major groove binding (Hoechst 33258) and covalent binding (cis-Pt) were examined. The obtained results suggest that both the transfer of conformation B to C and the denaturation process, for the ligand-dsDNA complexes, except for covalently bound cis-Pt, took place at higher temperatures compared to the unbound helix. Furthermore,...
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Modification of Titanium (IV) Dioxide with Small Silver Nanoparticles: Application in Photocatalysis
PublikacjaThe surface of commercial TiO2 compounds (P25 and ST01) has been modified with Ag nanoparticles induced by radiolysis. On P25, the Ag nanoclusters are very small (1−2 nm) and homogeneous in size while on ST01, two populations of nanoparticles are obtained, small nanoparticles (1−2 nm) and larger ones (mean diameter 7 to 12 nm depending on the silver loading). The photocatalytic properties of Ag-modified TiO2 have been studied for...
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A general approach to study molecular fragmentation and energy redistribution after an ionizing event
PublikacjaWe propose to combine quantum chemical calculations, statistical mechanical methods, and photoionization and particle collision experiments to unravel the redistribution of internal energy of the furan cation and its dissociation pathways. This approach successfully reproduces the relative intensity of the different fragments as a function of the internal energy of the system in photoelectron–photoion coincidence experiments and...
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Revealing the Frank–Evans “Iceberg” Structures within the Solvation Layer around Hydrophobic Solutes
PublikacjaUsing computer simulations, the structural properties of solvation water of three model hydrophobic molecules, methane and two fullerenes (C60 and C80), were studied. Systems were simulated at temperatures in the range of 250−298 K. By analyzing both the local ordering of the molecules of water in the solvation layers and the structure of hydrogen bond network, it is shown that in the solvation layer of hydrophobic molecules, ordered...
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Systematic Water Uptake Energetics of Yttrium-Doped Barium Zirconate—A High Resolution Thermochemical Study
PublikacjaA combination of surface area analyzer and microcalorimetry was employed to investigate the in situ water uptake energetics and the mechanism of proton incorporation in yttrium-doped barium zirconate in the temperature range 200–400 °C. The BaZr1–xYxO3 solid solutions are made with variable yttrium content (x = 10, 20, and 30 mol %) by a controlled oxidant-peroxo synthesis method. The water uptake increases as the partial pressure...