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showing 10 items of 13546 documents

Density-Functional Theory on Graphs

2021

The principles of density-functional theory are studied for finite lattice systems represented by graphs. Surprisingly, the fundamental Hohenberg–Kohn theorem is found void, in general, while many insights into the topological structure of the density-potential mapping can be won. We give precise conditions for a ground state to be uniquely v-representable and are able to prove that this property holds for almost all densities. A set of examples illustrates the theory and demonstrates the non-convexity of the pure-state constrained-search functional. peerReviewed

Chemical Physics (physics.chem-ph)Quantum PhysicstiheysfunktionaaliteoriaGeneral Physics and AstronomyFOS: Physical sciences02 engineering and technologyMathematical Physics (math-ph)021001 nanoscience & nanotechnology01 natural sciencesPhysics - Chemical Physics0103 physical scienceskvanttimekaniikkaPhysical and Theoretical Chemistry010306 general physics0210 nano-technologyQuantum Physics (quant-ph)Mathematical Physics
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A Molecular Electron Density Theory Study of the Reactivity of Azomethine Imine in [3+2] Cycloaddition Reactions

2017

The electronic structure and the participation of the simplest azomethine imine (AI) in [3+2] cycloaddition (32CA) reactions have been analysed within the Molecular Electron Density Theory (MEDT) using DFT calculations at the MPWB1K/6-311G(d) level. Electron localisation function (ELF) topological analysis reveals that AI has a pseudoradical structure, while the conceptual DFT reactivity indices characterise this TAC as a moderate electrophile and a good nucleophile. The non-polar 32CA reaction of AI with ethylene takes place through a one-step mechanism with low activation energy, 5.3 kcal/mol-1. A bonding evolution theory (BET) study indicates that this reaction takes place through a non-…

Models MolecularThiosemicarbazones[3+2] cycloaddition reactionsImineMolecular Conformationmolecular mechanismsazomethine iminePharmaceutical ScienceElectronsElectronic structureActivation energy010402 general chemistry01 natural sciencesArticlebonding evolution theoryAnalytical Chemistrychemistry.chemical_compoundNucleophileComputational chemistryDrug Discoveryconceptual density functional theoryMoleculeReactivity (chemistry)organic_chemistryelectron densityPhysical and Theoretical Chemistryazomethine imine; [3+2] cycloaddition reactions; molecular electron density theory; conceptual density functional theory; electron localisation function; bonding evolution theory; electron density; molecular mechanisms; chemical reactivityCycloaddition ReactionMolecular Structure010405 organic chemistrymolecular electron density theoryOrganic ChemistryCycloaddition0104 chemical scienceschemistryChemistry (miscellaneous)ElectrophileQuantum TheoryThermodynamicsMolecular MedicineDensity functional theoryImineselectron localisation functionAzo Compoundschemical reactivityMolecules; Volume 22; Issue 5; Pages: 750
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Towards an accurate molecular orbital theory for excited states : Ethene, butadiene, and hexatriene

1993

A newly proposed quantum chemical approach for ab initio calculations of electronic spectra of molecular systems is applied to the molecules ethene, trans‐1,3‐butadiene, and trans‐trans‐1,3,5‐hexatriene. The method has the aim of being accurate to better than 0.5 eV for excitation energies and is expected to provide structural and physical data for the excited states with good reliability. The approach is based on the complete active space (CAS) SCF method, which gives a proper description of the major features in the electronic structure of the excited state, independent of its complexity, accounts for all near degeneracy effects, and includes full orbital relaxation. Remaining dynamic ele…

ErrorsGeneral Physics and AstronomyPolyenesElectronic structuresymbols.namesakeRydberg StatesAb initio quantum chemistry methodsComputational chemistrySinglet statePhysical and Theoretical ChemistryTriplet state:FÍSICA::Química física [UNESCO]AccuracyExcitationCalculation MethodsButadieneTripletsChemistryMolecular orbital theoryScf CalculationsExcited StatesCalculation Methods ; Quantum Chemistry ; Ab Initio Calculations ; Electron Spectra ; Butadiene ; Accuracy ; Scf Calculations ; Triplets ; Rydberg States ; Excitation ; Errors ; Polyenes ; Excited StatesQuantum ChemistryUNESCO::FÍSICA::Química físicaElectron SpectraExcited stateRydberg formulasymbolsRydberg stateAtomic physicsAb Initio Calculations
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Nature of Interactions at the Interface of Two Water-Saturated Commercial TiO2 Polymorphs

2013

Two commercial TiO2 samples, a 100% anatase and a 100% rutile, were used for the fast field cycling NMR experiments. The results showed a different behavior between the different samples. In particular, water molecules were unbonded to the solid surface for the rutile sample, whereas they appeared to chemically interact with the surface through H-bond formation with the anatase sample. The above findings accord with the generally lower activity of rutile with respect to anatase reported in literature for photocatalytic oxidation reactions in water. The difficulty of water to interact with rutile surface, indeed, could hinder the formation of OH radicals, which are the most important oxidant…

AnataseMaterials scienceField cyclingInterface (Java)relaxometrySettore AGR/13 - Chimica AgrariaMineralogySurfaces Coatings and FilmsElectronic Optical and Magnetic MaterialsGeneral EnergyChemical engineeringRutileSettore CHIM/07 - Fondamenti Chimici Delle TecnologiePhysical and Theoretical ChemistryThe Journal of Physical Chemistry C
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Two-view “cylindrical decomposition” of binary images

2001

This paper describes the discrete cylindrical algebraic decomposition (DCAD) construction along two orthogonal views of binary images. The combination of two information is used to avoid ambiguities for image recognition purposes. This algorithm associates an object connectivity graph to each connected component, allowing a complete description of the structuring information. Moreover, an easy and compact representation of the scene is achieved by using strings in a five letter alphabet. Examples on complex digital images are also provided. © 2001 Elsevier Science Inc.

Connected componentNumerical AnalysisAlgebra and Number TheoryTheoretical computer scienceSettore INF/01 - InformaticaBinary imageObject (computer science)StructuringCylindrical algebraic decompositionString representationDigital imageImage decompositionComputer Science::Computer Vision and Pattern RecognitionDecomposition (computer science)Discrete Mathematics and CombinatoricsGeometry and TopologyRepresentation (mathematics)AlgorithmShape descriptionMathematicsLinear Algebra and its Applications
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Approximate treatment of higher excitations in coupled-cluster theory.

2005

The possibilities for the approximate treatment of higher excitations in coupled-cluster (CC) theory are discussed. Potential routes for the generalization of corresponding approximations to lower-level CC methods are analyzed for higher excitations. A general string-based algorithm is presented for the evaluation of the special contractions appearing in the equations specific to those approximate CC models. It is demonstrated that several iterative and noniterative approximations to higher excitations can be efficiently implemented with the aid of our algorithm and that the coding effort is mostly reduced to the generation of the corresponding formulas. The performance of the proposed and …

PhysicsCoupled clusterGeneralizationExcited stateBenchmark (computing)General Physics and AstronomyStatistical physicsPhysical and Theoretical ChemistryMolecular systemsAtomic physicsString (physics)The Journal of chemical physics
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Calix[4]arene-functionalized naphthalene and perylene imide dyes.

2002

[reaction: see text] Calix[4]arenes bearing one, two, or four 1,8-naphthyl imide groups at the wide rim and bis-calix[4]arenes connected via perylene-bisimide dye spacers have been synthesized. The low-temperature NMR spectrum of the tetranaphthylimide suggests, in agreement with a crystal structure, a C2-symmetrical pinched cone conformation stabilized via face-to-face pi-pi interactions between opposite naphthylimide groups. UV-vis and fluorescence studies have been carried out for the perylene bis-calix[4]arene dyes.

Molecular StructureChemistryOrganic ChemistryCrystal structureNuclear magnetic resonance spectroscopyNaphthalenesPhotochemistryImidesBiochemistryFluorescencechemistry.chemical_compoundPhenolsPolymer chemistryCalixareneMoleculePhysical and Theoretical ChemistryCalixarenesImideColoring AgentsPerylenePeryleneNaphthaleneFluorescent DyesOrganic letters
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Diffusive equilibrium properties of O2 in amorphous SiO2 nanoparticles probed via dependence of concentration on size and pressure

2014

An experimental study on the diffusive equilibrium value of interstitial O2 in silica nanoparticles was carried out on samples with average particles diameter 40, 14, and 7 nm. The investigation was performed by measuring the concentration of interstitial O2 by Raman and photoluminescence techniques. The dependence of diffusive equilibrium concentration on pressure and temperature was investigated in the pressure range from 0.2 to 76 bar and in the temperature range from 98 to 244 °C. The equilibrium concentration of interstitial O2 follows Henry’s law at pressures below 13 bar whereas a departure from this model is observed at higher pressures. In particular, O2 concentration saturates abo…

PhotoluminescenceChemistrySettore FIS/01 - Fisica SperimentaleAnalytical chemistryThermodynamicsNANOSILICA DIFFUSIONAtmospheric temperature rangeSurfaces Coatings and FilmsElectronic Optical and Magnetic MaterialsAmorphous solidSilica nanoparticlesPressure rangesymbols.namesakeGeneral EnergySio2 nanoparticlessymbolsPhysical and Theoretical ChemistryRaman spectroscopyBar (unit)
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C-H Bond Arylation of Pyrazoles at the β-Position: General Conditions and Computational Elucidation for a High Regioselectivity

2021

International audience; Direct arylation of most five-membered ring heterocycles are generally easily accessible and strongly favored at the α-position using classical palladium-catalysis. Conversely, regioselective functionalization of such heterocycles at the concurrent β-position remains currently very challenging. Herein, we report general conditions for regioselective direct arylation at the β-position of pyrazoles, while C-H α-position is free. By using aryl bromides as the aryl source and a judicious choice of solvent, the arylation reaction of variously N-substituted pyrazoles simply proceeds via β-C-H bond functionalization. The β-regioselectivity is promoted by a ligand-free palla…

chemistry.chemical_element010402 general chemistryRing (chemistry)01 natural sciencesCatalysischemistry.chemical_compoundbeta-C−H arylationsolvent effectcatalysis010405 organic chemistry[CHIM.ORGA]Chemical Sciences/Organic chemistryArylOrganic ChemistryRegioselectivityGeneral Chemistry[CHIM.CATA]Chemical Sciences/CatalysispalladiumCombinatorial chemistry0104 chemical sciences[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistrychemistryIntramolecular forceSolvent effectsProtic solventPalladiumheterocycle
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Bortezomib potentiates the antitumor effect of tributyltin(IV) ferulate in colon cancer cells exacerbating ER stress and promoting apoptosis

2022

Organotin(IV) complexes represent promising drugs in medicinal chemistry for their potential use in cancer therapy. We recently reported synthesis and characterization of a new organotin(IV) complex of ferulic acid (FA), tributyltin(IV) ferulate (TBT-F), showing its antitumor action in colon cancer cells. Here we provide evidence that the efficacy of this compound is strongly potentiated by the proteasome inhibitor bortezomib (BTZ). While low concentrations of tributyltin(IV) ferulate alone promoted autophagy without reducing cell viability, combination of the two compounds markedly affected colon cancer cell viability, cell morphology and exasperated endoplasmic reticulum (ER) stress, as r…

Inorganic ChemistryMaterials ChemistryApoptosisProteasome inhibitorFerulic acidPhysical and Theoretical ChemistryER stressOrganotin(IV) complexes
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