Search results for "ab initio"
showing 10 items of 990 documents
Ab initiocalculations of BaTiO3(111) surfaces
2013
The article presents the results of calculations of polar (111) surface relaxations and energetics using the ab initio code CRYSTAL and a hybrid description of exchange and correlation. Using a hybrid B3LYP approach, the surface relaxation has been calculated for the two possible Ti and BaO3 BaTiO3 (111) surface terminations. For both Ti- and BaO3-terminated BaTiO3 (111) surfaces, the upper layer atoms relax inward. The second layer atoms, with the sole exception of Ti-terminated BaTiO3 (111) surface Ba atom, relax outward. The calculated surface relaxation energy for Ti-terminated BaTiO3 (111) surface is more than two times larger than the surface relaxation energy for BaO3-terminated BaTi…
Ab initio calculations for the polar (0 0 1) surfaces of YAlO3
2018
Abstract The results of ab initio calculations of polar YAlO3 (0 0 1) surfaces by means of a hybrid B3LYP exchange-correlation functional as it is implemented in the CRYSTAL computer code are presented. Both polar YO and AlO2-terminations of the cubic YAlO3 (0 0 1) surface were considered. We performed relaxation of atoms on the upper three layers of both YO and AlO2-terminated YAlO3 (0 0 1) surfaces using in our calculations slabs containing 22 and 23 atoms as well as 9 layers, respectively. We predict a significant increase of the Al-O chemical bond covalency on the AlO2-terminated YAlO3 (0 0 1) surface with respect to the YAlO3 bulk. Our calculated YO and AlO2-terminated YAlO3 polar (0 0…
Ab initio thermodynamic study of (Ba,Sr)(Co,Fe)O3 perovskite solid solutions for fuel cell applications
2013
(Ba,Sr)(Co,Fe)O3 (BSCF) perovskite solid solutions are promising materials for solid oxide fuel cell cathodes and oxygen permeation membranes. Cathode performance strongly depends on the morphology of these materials remaining as a single phase or two-phase mixture. Combining ab initio calculations of the atomic and electronic structure of different supercells with thermodynamics of solid solutions, we have constructed and discussed phase diagrams of several important BSCF chemical compositions. It is demonstrated that in BSC cobaltite solid solution the spinodal decomposition may occur already at relatively low temperatures, while ferrite (BSF and SCF) solid solutions decompose at relative…
Ab initio hybrid DFT calculations of BaTiO3, PbTiO3, SrZrO3 and PbZrO3 (111) surfaces
2015
Abstract The results of ab initio calculations for polar BaTiO 3 , PbTiO 3 , SrZrO 3 and PbZrO 3 (111) surfaces using the CRYSTAL code are presented. By means of the hybrid B3LYP approach, the surface relaxation has been calculated for two possible B (B = Ti or Zr) or AO 3 (A = Ba, Pb or Sr) BaTiO 3 , PbTiO 3 , SrZrO 3 and PbZrO 3 (111) surface terminations. According to performed B3LYP calculations, all atoms of the first surface layer, for both terminations, relax inwards. The only exception is a small outward relaxation of the PbO 3 -terminated PbTiO 3 (111) surface upper layer Pb atom. B3LYP calculated surface energies for BaO 3 , PbO 3 , SrO 3 and PbO 3 -terminated BaTiO 3 , PbTiO 3 , …
Dissociation mechanisms of cluster ions resolved using ab-initio molecular orbital calculations
2007
We have examined the cluster-size effect on fragments in the collision-induced dissociation (CID) of small boron clusters (B + n , n ≤ 8) by means of ab-initio molecular orbital (MO) calculation, for conditions representative of low-Z cationic clusters in plasma. Single cations B + (leaving B 0 n-1 ) are predominantly fragmented from small clusters B + n (n < 5) by low-energy collisions (<10 eV) with Xe atoms. With increasing the size n, beyond n = 5, B + n-1 (leaving B°) clusters are observed preferentially. This alternating trend in experiment has not been quantitatively explained by previous ab-initio MO calculations. We used a density functional method called B3LYP and basis functions 6…
Experimental Investigations and Ab Initio Studies of Tellurium(II) Dithiolates, Te(SR)2
1999
The reaction between Te(O(i)Pr)(4) and HSR offers a new and effective route to tellurium dithiolates, Te(SR)(2). Te(S(i)Pr)(2) (1) and Te(S(t)Bu)(2) (2) are stable compounds whereas Te(SPh)(2) (3) slowly decomposes at room temperature to give Te and Ph(2)S(2). IR spectra of 1-3 and ab initio calculations (HF/3-21G(d) and MP2 with double-zeta polarization effective core potential basis set) show nu(as)(Te-S) and nu(s)(Te-S) to be around 340 and 380 cm(-)(1), respectively. UV spectra exhibit similar lambda(max) (346-348 nm) for all three compounds, with the greater extinction coefficient of 3 accounting for its different and more intense color. Analysis of the molecular orbitals of the model …
Simulations of Glassforming Network Fluids: Classical Molecular Dynamics versus Car-Parrinello Molecular Dynamics
2010
Abstract Static and dynamic Properties of molten germanium dioxide are studied by two simulation methods, classical Molecular Dynamics (MD) using the Oeffner-Elliott (OE) potential, and “ab initio” Car-Parrinello Molecular Dynamics (CPMD). While CPMD provides a (presumably) more accurate description of the local structure and the forces, it severely suffers from finite size effects when the structure beyond the first neighbor shells is considered. For glassforming fluids, the demanding equilibrium needs are a further reason, why simply MD is still preferable, when a “good” effective potential is available.
Ab initio study on the photoisomers of a nitro-substituted spiropyran
2000
Structural and spectroscopic properties of the photoisomers of a nitro-substituted spiropyran have been investigated by performing ab initio molecular orbital (MO) calculations both in vacuo and in hexafluoro-2-propanol solution. Full geometry optimisation of the closed form and of the transoid conformations of the open form has been carried out. Dipole moments of both photoisomers have been determined, the ratio of which agrees with recent experimental results. Net atomic charges have also been determined according to three different approaches.
Gas-phase detection of HSOH: synthesis by flash vacuum pyrolysis of di-tert-butyl sulfoxide and rotational-torsional spectrum.
2003
Gas-phase oxadisulfane (HSOH), the missing link between the well-known molecules hydrogen peroxide (HOOH) and disulfane (HSSH), was synthesized by flash vacuum pyrolysis of di-tert-butyl sulfoxide. Using mass spectrometry, the pyrolysis conditions have been optimized towards formation of HSOH. Microwave spectroscopic investigation of the pyrolysis products allowed-assisted by high-level quantum-chemical calculations--the first measurement of the rotational-torsional spectrum of HSOH. In total, we have measured approximately 600 lines of the rotational-torsional spectrum in the frequency range from 64 GHz to 1.9 THz and assigned some 470 of these to the rotational-torsional spectrum of HSOH …
Ab initio Hartree-Fock calculations of LaMnO3 (110) surfaces
2003
We present the results of ab initio Hartree-Fock calculations of the LaMnO3 (110) surface. Using seven-plane slabs, periodic in 2D and containing three formula units, we compare the properties of a stoichiometric surface with oxygen vacancies, and non-stoichiometric, defect-free surfaces, analyze the dispersion of the effective charges near the surface, and calculate the surface energy before and after relaxation, for both ferromagnetric and antiferromagnetic spin orderings in a slab. q 2003 Elsevier Ltd. All rights reserved.