Search results for "DFT"
showing 10 items of 361 documents
Synthesis of C2-Symmetrical Bis-(β-Enamino-Pyran-2,4-dione) Derivative Linked via 1,6-Hexylene Spacer: X-ray Crystal Structures, Hishfeld Studies and…
2021
The synthesis of C2-symmetrical bis(β-enamino-pyran-2,4-dione) derivative 3 connected via 1,6-hexylene linker was reported for the first time. X-ray structures and Hirshfeld studies of the new bis- β-enamino-pyran-2,4-dione derivative 3 along with two structurally related pyran-2,4-dione derivatives 2a,b were discussed. A comparative analysis of the different intermolecular contacts affecting the crystal stability was presented. Generally, the H…H, O…H, and H…C interactions are common in all compounds and are considered the most abundant contacts. In addition, DFT calculations were used to compute the electronic properties as well as the 1H and 13C NMR spectra of the studied systems. All co…
Universal correction for the Becke-Johnson exchange potential
2010
The Becke-Johnson exchange potential [A. D. Becke and E. R. Johnson, J. Chem. Phys. 124, 221101 (2006)] has been successfully used in electronic structure calculations within density-functional theory. However, in its original form, the potential may dramatically fail in systems with non-Coulombic external potentials, or in the presence of external magnetic or electric fields. Here, we provide a system-independent correction to the Becke-Johnson approximation by (i) enforcing its gauge-invariance and (ii) making it exact for any single-electron system. The resulting approximation is then better designed to deal with current-carrying states and recovers the correct asymptotic behavior for sy…
A first-principles time-dependent density functional theory framework for spin and time-resolved angular-resolved photoelectron spectroscopy in perio…
2017
We present a novel theoretical approach to simulate spin, time, and angular-resolved photoelectron spectroscopy (ARPES) from first-principles that is applicable to surfaces, thin films, few layer systems, and low-dimensional nanostructures. The method is based on a general formulation in the framework of time-dependent density functional theory (TDDFT) to describe the real time-evolution of electrons escaping from a surface under the effect of any external (arbitrary) laser field. By extending the so-called t-SURFF method to periodic systems one can calculate the final photoelectron spectrum by collecting the flux of the ionization current trough an analyzing surface. The resulting approach…
Spinorial formulation of the GW-BSE equations and spin properties of excitons in two-dimensional transition metal dichalcogenides
2021
In many paradigmatic materials, such as transition metal dichalcogenides, the role played by the spin degrees of freedom is as important as the one played by the electron-electron interaction. Thus an accurate treatment of the two effects and of their interaction is necessary for an accurate and predictive study of the optical and electronic properties of these materials. Despite the fact that the GW-BSE approach correctly accounts for electronic correlations, the spin-orbit coupling effect is often neglected or treated perturbatively. Recently, spinorial formulations of GW-BSE have become available in different flavors in material-science codes. However, an accurate validation and comparis…
Nuclear density functional theory with a semi-contact 3-body interaction
2015
International audience; Theories combining nuclear density functional approach (DFT) and effects beyond the independent particle/quasi-particle limit have attracted much attention recently. In particular, such theories, generically referred as “beyond mean-field” (BMF) seem unavoidable to account for both single-particle effects and complex quantum internal phenomena in nuclear finite many-body nuclear systems. It has been realized recently that BMF theories might lead to specific difficulties when applied within the nuclear DFT context. An example is the appearance of divergences in configuration mixing approaches. A short summary of the difficulties is given here. One source of problem is…
Mapováni spinů povrchových a bulkových Rashba stavů v tenkých vrstvách feroelektrického α-GeTe(111)
2015
Rozbíjení inverzní symetrie ve fereeleRashba efekt; Fotoemisse; DFTktrickém polovodiči způsobuje děleni stavů, tzv Rashba efekt. V tomto článku ukazujeme kompletně mapování spinové polarizace těchto Rashba stavů za pomoci spinovo rozlišené fotoemisse. The breaking of bulk inversion symmetry in ferroelectric semiconductors causes a Rashba-type spin splitting of electronic bulk bands. This is shown by a comprehensive mapping of the spin polarization of the electronic bands in ferroelectric α- GeTe(111) films using a time-of-flight momentum microscope equipped with an imaging spin filter that enables a simultaneous measurement of more than 10 000 data points. The experiment reveals an opposite…
Novel meso-substituted porphyrins: Synthesis, characterization and photocatalytic activity of their TiO2-based composites
2009
Abstract Two series of novel meso-substituted porphyrins, namely 5,10,15,20-tetra[4-(3-phenoxy)-propoxy]phenyl porphyrin, the structural analogue 5,10,15,20-tetra[2-(3-phenoxy)-propoxy]phenyl porphyrin and their Co(II) Cu(II) and Zn(II) complexes were synthesized. The compounds were characterized using various spectroscopic techniques and their molecular structure was proposed based on density functional theory calculations. The diverse properties of the porphyrin derivatives result from the different stereochemistry of the particular substituents at the meso site on the macrocycle and are controlled also by the coordinated metal. The 1H NMR spectrum of the free-base porphyrin showed a comp…
Computational investigation of isoeugenol transformations on a platinum cluster – I: Direct deoxygenation to propylcyclohexane
2022
The growing demand for renewable and sustainable fuels, protagonists of an increasingly important research area due to the exhaustion of fossil resources, has oriented our investigation towards the computational mechanistic analysis of the catalytic hydrodeoxygenation (HDO) reaction of isoeugenol. Having the most com mon functional groups, the isoeugenol molecule is actually considered as an experimental and computational model for typical species of biomass origin. The reported computational investigation outlines the energy bar riers and the intermediates along the path for the conversion of isoeugenol to propylcyclohexane through a direct deoxygenation mechanims, catalyzed by a subnano…
Density functional theory (DFT) prediction of structural and spectroscopic parameters of cytosine using harmonic and anharmonic approximations
2015
The applicability of popular and efficient B3LYP hybrid density functional and medium-size Pople-type basis set in combination with computationally expensive anharmonic model to obtain more accurate theoretical structure, vibrational frequencies and GIAO NMR parameters of cytosine was tested. We report on prediction of cytosine equilibrium (R e ) and rovibrationally averaged (R v ) structures and vibrational frequencies in the gas phase and DMSO solution using density functional theory combined with 6-311++G** basis set. The harmonic and anharmonic vibrational frequencies (using second-order vibrational perturbation theory, VPT2) were critically discussed. In comparison with initial harmoni…
Unravelling the GLY-PRO-GLU tripeptide induced reconstruction of the Au(110) surface at the molecular scale
2018
International audience; The adsorption of GLY-PRO-GLU tripeptide on Au(110) is investigated within the frame of all atom classical mechanics simulations and Density Functional Theory, focusing on the surface reconstruction. It is shown that the tripeptide adsorption reorganizes and restructures the Au(110) surface. A mechanism for the surface restructuration is proposed for both the neutral and zwitterionic form of the peptide at room temperature in Ultra High Vacuum. Diverse residues may be involved in the Au atoms displacement, and in particular glutamic acid, triggering a double proton transfer and the formation of a zwitter ionic state, is found to be responsible for the triggering of t…