Search results for "ELECTRONIC STRUCTURE"
showing 10 items of 722 documents
Size-Dependent Structural Evolution and Chemical Reactivity of Gold Clusters
2006
Ground-state structures and other experimentally relevant isomers of Au(15) (-) to Au(24) (-) clusters are determined through joint first-principles density functional theory and photoelectron spectroscopy measurements. Subsequent calculations of molecular O(2) adsorption to the optimal cluster structures reveal a size-dependent reactivity pattern that agrees well with earlier experiments. A detailed analysis of the underlying electronic structure shows that the chemical reactivity of the gold cluster anions can be elucidated in terms of a partial-jellium picture, where delocalized electrons occupying electronic shells move over the ionic skeleton, whose geometric structure is strongly infl…
Cholesky decomposition-based definition of atomic subsystems in electronic structure calculations
2010
Decomposing the Hartree-Fock one-electron density matrix and a virtual pseudodensity matrix, we obtain an orthogonal set of normalized molecular orbitals with local character to be used in post-Hartree-Fock calculations. The applicability of the procedure is illustrated by calculating CCSD(T) energies and CCSD molecular properties in reduced active spaces. © 2010 American Institute of Physics.
Selected dissociation‐ and correlation‐consistent configuration interaction by a perturbative criterion
1990
We propose a perturbative criterion to select the most important dissociation‐ or correlation‐consistent type of contributions to perform generalized valence bond‐configuration interaction (GVB‐CI) calculations, dissociation‐consistent configuration interaction (DCCI) or correlation‐consistent configuration interaction (CCCI) approach, respectively. The procedure presented is computationally less demanding than the CCCI proposed by Goddard and co‐workers. To ensure the distance consistency of the MOs used, the nonvalence virtual orbitals are obtained by a projection technique. The results obtained for a few test calculations show the ability of the suggested approach to get close results to…
Fourier-transform spectroscopy, direct-potential-fit, and electronic structure calculations on the entirely perturbed (4)1Π state of RbCs
2018
We performed a high-resolution Fourier-transform spectroscopic study of the (4)1Π state of the RbCs molecule by applying two-step (4)1Π ← A1Σ+ ∼ b3Π ← X1Σ+ optical excitation followed by observation of the (4)1Π → X1Σ+ laser induced fluorescence (LIF) spectra. In many LIF progressions the collision-induced satellite rotational lines were observed thus increasing the amount of term values and allowing to estimate the Λ-doubling effect in the (4)1Π state. The Direct-Potential-Fit (DPF) of experimental term values of 777 rovibronic levels of both 85RbCs and 87RbCs isotopologues has been performed by means of the robust weighted non-linear least squares method. The PFanalysis based on adiabatic…
Electronic structure and transport properties of the Heusler compound Co2TiAl
2009
The properties of the Heusler compound Co2TiAl were investigated in detail by experimental techniques and theoretical methods. X-ray diffraction measurements indicate that as-cast samples of the compound exhibit the L21 structure with a small amount of B2-type disorder. This leads to a reduced saturation magnetization per formula unit of 0.747 μB. The Curie temperature is approximately 120 K. The transport properties are influenced by the change in the electronic structure at the Curie temperature, as revealed experimentally by conductivity, thermal transport and specific heat measurements. Different theoretical models based on ab initio calculations of the electronic structure are used to …
An experimental investigation on the poor hydrogen sorption properties of nano-structured LaNi5 prepared by ball-milling
2011
Abstract Nano-structured LaNi5 hydrogen storage materials prepared by ball-milling is analysed using differential scanning calorimetry (DSC) and x-ray photoelectron spectroscopy (XPS). DSC results indicate a partial elimination of defects at 500 °C in a more efficient way for the short-time ball-milled powders compared to the long-time ball-milled ones. XPS results show almost no change in the core-level electronic structure for La and Ni of LaNi5 in the bulk and the nano-structured forms, but gives an indication that the self-restoring mechanism of the active surface observed in the bulk sample (Siegmann et al. Phys. Rev. Lett. 40, 972) may not be occurring in the nano-powders. Results fro…
Effect of pressure on the structural properties and electronic band structure of GaSe
2007
The structural properties of GaSe have been investigated up to 38 GPa by monochromatic X-ray diffraction. The onset of the phase transition from the e-GaSe to a disordered NaCi-type structural motif is observed near 21 GPa. Using the experimentally determined lattice parameters of the layered e-phase as input, constrained ab-initio total energy calculations were performed in order to optimize the internal structural parameters at different pressures. The results obtained for the nearest-neighbor Ga-Se distance agree with those derived from recent EXAFS measurements. In addition, information is obtained on the changes of Ga-Ga and Se-Se bond lengths which were not accessible to a direct expe…
Computational chemistry meets experiments for explaining the geometry, electronic structure, and optical properties of Ca10V6O25
2018
In this paper, we present a combined experimental and theoretical study to disclose, for the first time, the structural, electronic, and optical properties of Ca10V6O25 crystals. The microwave-assisted hydrothermal (MAH) method has been employed to synthesize these crystals with different morphologies, within a short reaction time at 120 °C. First-principle quantum mechanical calculations have been performed at the density functional theory level to obtain the geometry and electronic properties of Ca10V6O25 crystal in the fundamental and excited electronic states (singlet and triplet). These results, combined with the measurements of X-ray diffraction (XRD) and Rietveld refinements, confirm…
Elektrónová a pásová štruktúra CuMnAs študovaná optickou a fotoemissinou spektroskopiou
2017
Tetragonal phase of CuMnAs progressively appears as one of the key materials for antiferromagnetic spintronics due to efficient current-induced spin-orbit torques whose existence can be directly inferred from crystal symmetry. Theoretical understanding of spintronic phenomena in this material, however, relies on the detailed knowledge of electronic structure (band structure and corresponding wave functions) which has so far been tested only to a limited extent. We show that AC permittivity (obtained from ellipsometry) and UV photoelectron spectra agree with density functional calculations. Together with the x-ray diffraction and precession electron diffraction tomography, our analysis confi…
Site-specific atomic order and band structure tailoring in the diluted magnetic semiconductor (In,Ga,Mn)As
2021
Physical review / B 103(7), 075107 (1-13) (2021). doi:10.1103/PhysRevB.103.075107