Search results for "DENSITY FUNCTIONAL THEORY"
showing 10 items of 981 documents
Magnetic anisotropy in Fe/U and Ni/U bilayers
2021
Magnetometry measurements of Fe/U and Ni/U bilayer systems reveal a non-monotonic dependence of the magnetic anisotropy for U thicknesses in the range 0 nm - 8 nm, with the Fe/U bilayers showing a more prominent effect as compared to Ni/U. The stronger response for Fe/U is ascribed to the stronger 3d-5f hybridization of Fe and U. This non-monotonic behaviour is thought to arise from quantum well states in the uranium overlayers. Estimating an oscillation period from the non-monotonic data, and comparing it to Density Functional Theory calculations, we find that wavevector matches to the experimental data can be made to regions of high spectral density in (010) and (100) cuts of the electron…
Quantum Well States in Two-Dimensional Gold Clusters on MgO Thin Films
2008
The electronic structure of ultra-small Au clusters on thin MgO/Ag(001) films has been analyzed by scanning tunneling spectroscopy and density functional theory. The clusters exhibit two-dimensional (2D) quantum well states, whose shapes resemble the eigen-states of a 2D electron gas confined in a parabolic potential. From the symmetries of the HOMO and LUMO of a particular cluster, its electron filling and charge state is determined. In accordance to a DFT Bader-charge analysis, aggregates containing up to twenty atoms accumulate one to four extra electrons due to a charge transfer from the MgO/Ag interface. The HOMO - LUMO gap is found to close for clusters containing between 70 and 100 a…
Ab initio DFT+U study of He atom incorporation into UO(2) crystals.
2009
We present and discuss results of a density functional theory (DFT) study of a perfect UO2 crystals and He atoms in octahedral interstitial positions. We have calculated basic bulk crystal properties and He incorporation energies into the low temperature anti-ferromagnetic UO2 phase using several exchange-correlation functionals within the spin-polarized local density (LDA) and generalized gradient (GGA) approximations. In all these DFT calculations we included the on-site correlation corrections using the Hubbard model (DFT+U approach). We analysed a potential crystalline symmetry reduction and confirmed the presence of the Jahn-Teller effect in a perfect UO2. We discuss also the problem o…
Nonmagnetic and magnetic thiolate-protected Au25superatoms on Cu(111), Ag(111), and Au(111) surfaces
2012
Geometry, electronic structure, and magnetic properties of methylthiolate-stabilized Au$_{25}$L$_{18}$ and MnAu$_{24}$L$_{18}$ (L = SCH$_3$) clusters adsorbed on noble-metal (111) surfaces have been investigated by using spin-polarized density functional theory computations. The interaction between the cluster and the surface is found to be mediated by charge transfer mainly from or into the ligand monolayer. The electronic properties of the 13-atom metal core remain in all cases rather undisturbed as compared to the isolated clusters in gas phase. The Au$_{25}$L$_{18}$ cluster retains a clear HOMO - LUMO energy gap in the range of 0.7 eV to 1.0 eV depending on the surface. The ligand layer…
Existence, uniqueness, and construction of the density-potential mapping in time-dependent density-functional theory
2014
In this work we review the mapping from densities to potentials in quantum mechanics, which is the basic building block of time-dependent density-functional theory and the Kohn-Sham construction. We first present detailed conditions such that a mapping from potentials to densities is defined by solving the time-dependent Schr\"odinger equation. We specifically discuss intricacies connected with the unboundedness of the Hamiltonian and derive the local-force equation. This equation is then used to set up an iterative sequence that determines a potential that generates a specified density via time propagation of an initial state. This fixed-point procedure needs the invertibility of a certain…
Quantum Mechanical Modelling of Pure and Defective KNbO3 Perovskites
2000
Ab initio electronic structure calculations using the density-functional theory (DFT) are performed for KNbO3 with and without defects. Ferroelectric distortive transitions involve very small changes in energies and are therefore sensitive to DFT-approximations. This is discussed by comparing results obtained with the local density approximation (LDA) to those where generalized gradient approximations (GGA) are used. The results of ab initio calculations for F-type centers and bound hole polarons are compared to those obtained by a semiempirical method of the Intermediate Neglect of the Differential Overlap (INDO), based on the HartreeFock formalism. Supercells with 40 and 320 atoms were us…
<title>Computer modeling of point defects, polarons, excitons, and surfaces in perovskite ferroelectrics</title>
2003
We review results of our recent large-scale computer simulations of point defects, excitons and polarons in ABO3 perovskite crystals, focusing mostly on KNbO3 and KTaO3 as representative examples. We have calculated the atomic and electronic structure of defects, their optical absorption and defect-induced electron density redistribution. The majority of results are obtained using the quantum chemical method of the intermediate neglect of differential overlap (INDO) based on the Hartree-Frock formalism. The main findings are compared with results of ab initio Density Functional Theory (FP-LMTO) first-principles calculations. The results of the electronic structure calculations for different…
Theoretical and Experimental Studies of Capillary Hysteresis in MCM-41
1996
Mesoporous materials of MCM-41 type are considered to be reference model adsorbents due to their regular pore structure. Nitrogen adsorption isotherms on MCM-41 are modeled using the Non-Local Density Functional Theory (NLDFT). The thermal dependence of the thermodynamic hysteresis predicted by the NLDFT is confirmed by experimental measurements. The nitrogen hysteresis on MCM-41 at temperatures below 77.4 K or in pores greater than 4 nm is associated with the metastability of the adsorption branch of the isotherm. In the hysteresis regime, the desorption branch is likely to be thermodynamically stable and is recommended for calculating pore size distributions.
First principles simulations of F centers in cubic SrTiO 3
2005
Atomic and electronic structure of regular and O-deficient SrTiO3 have been studied. Several types of first principles atomistic simulations: Hartree-Fock method, Density Functional Theory, and hybrid HF-DFT functionals, have been applied to periodic models that consider supercells of different sizes (ranging between 40 and 240 atoms). We confirm the ionic character of the Sr-O bonds and the high covalency of the Ti-O2 substructure. For the stoichiometric cubic crystal; the lattice constant and bulk modulus correctly reproduce the experimental data whereas the band gap is only properly obtained by the B3PW functional. The relaxed geometry around the F center shows a large expansion of the t…
Calculations of radiation-induced point defects, polarons and excitons in ferroelectric perovskites
2002
Abstract We review results of our recent large-scale computer simulations of radiation-induced point defects, excitons and polarons in ABO3 perovskite crystals, focusing mostly on KNbO3 and KTaO3 as representative examples. We have calculated the atomic and electronic structure of defects, their optical absorption, defect-induced electron density redistribution, and activation energies for defect migration. The majority of our results were obtained using the quantum-chemical method of the intermediate neglect of differential overlap (INDO) based on the Hartree–Fock formalism, as well as the shell model (SM). The main findings are compared with those obtained by means of ab initio density fu…