Search results for "Hybrid functional"
showing 10 items of 45 documents
Insights into Intrinsic Defects and the Incorporation of Na and K in the Cu2ZnSnSe4 Thin-Film Solar Cell Material from Hybrid-Functional Calculations
2016
We have performed density functional theory calculations using the HSE06 hybrid functional to investigate the energetics, atomic, and electronic structure of intrinsic defects as well as Na and K impurities in the kesterite structure of the Cu2ZnSnSe4 (CZTSe) solar cell material. We found that both Na and K atoms prefer to be incorporated into this material as substitutional defects in the Cu sublattice. At this site highly stable (Na–Na), (K–K), and (Na–K) dumbbells can form. While Na interstitial defects are stable in CZTSe, the formation of K interstitial defects is unlikely. In general, the calculated formation energies for Na-related defects are always lower compared to their K-related…
Calculation of electronic g-tensors using coupled cluster theory.
2009
A scheme for the calculation of the electronic g-tensor at the coupled cluster (CC) level is presented. The reported implementation employs an effective one-electron spin-orbit operator, allows the inclusion of arbitrary excitations in the cluster operator, and offers various options concerning the treatment of orbital relaxation and choice of reference determinants. In addition, the use of gauge-including atomic orbitals (GIAOs) is possible to overcome the gauge origin problem. Benchmark calculations for the NH ((3)Sigma(-)) radical reveal the importance of electron correlation effects for the accurate prediction of the g-shift as well as the slow basis set convergence of such calculations…
DFT Study on the Interaction of Tris(benzene-1,2-dithiolato)molybdenum Complex with Water. A Hydrolysis Mechanism Involving a Feasible Seven-Coordina…
2016
In the present work, the reactivity of the tris(benzene-1,2-dithiolato)molybdenum complex ([Mo(bdt)3]) toward water is studied by means of the density functional theory (DFT). DFT calculations were performed using the M06, B3P86, and B3PW91 hybrid functionals for comparison purposes. The M06 method was employed to elucidate the reaction pathway, relative stability of the intermediate products, nature of the Mo–S bond cleavage, and electronic structure of the involved molybdenum species. This functional was also used to study the transference of electrons from the molybdenum center toward the ligands. The reaction pathway confirms that [Mo(bdt)3] undergoes hydrolysis, yielding dihydroxo-bis(…
Incorporation of Li dopant into Cu2ZnSnSe4 photovoltaic absorber: hybrid-functional calculations
2015
We have studied the formation of Li extrinsic defects in CuZnSnSe by first-principles hybrid functional calculations. Li atoms in the Cu site (Li) and Li atoms in the Se site (Li) are the most and the least stable point defect, respectively. The formation energies of two Li interstitial defects with different numbers of nearest neighbors are the same. These interstitial point defects act as a donor but do not create gap states. Formation of the acceptor point defects (Li and Li) is less likely in p-type CuZnSnSe compared with n-type CuZnSnSe. In contrast to Li which does not create gap states, the formation of Li creates two charge transition levels in the middle of the bandgap which might …
Ab Initio Study of BiFeO3: Thermodynamic Stability Conditions
2015
BiFeO3 is investigated intensively, mainly as a multiferroic material. In this paper, the state-of-the-art ab initio hybrid functional approach with atomic basis sets was employed for a study of the stability range of BiFeO3 with respect to its decomposition into binary oxides and elementary metals, as a function of temperature and oxygen partial pressure. The calculated atomic and electronic structure of BiFeO3 was compared with previous LDA+U calculations using plane-wave basis sets. Based on performed calculations, the phase diagram was constructed, which allows us to predict the stability region of stoichiometric BiFeO3.
DFT calculation of 1J(119Sn,13C) and 2J(119Sn,1H) coupling constants in di- and trimethyltin(IV) compounds
2008
We have tested several computational protocols, at the nonrelativistic DFT level of theory, for the calculation of 1J(119Sn, 13C) and 2J(119Sn, 1H) spin-spin coupling constants in di- and trimethyltin(IV) derivatives with various ligands. Quite a good agreement with experimental data has been found with several hybrid functionals and a double-zeta basis set for a set of molecules comprising tetra-, penta-, and hexa-coordinated tin(IV). Then, some of the protocols have been applied to the calculation of the 2J(119Sn, 1H) of the aquodimethyltin(IV) ion and dimethyltin(IV) complex with D-ribonic acid and to the calculation of 1J(119Sn, 13C) and 2J(119Sn, 1H) of the dimethyltin(IV)-glycylglycin…
Thermodynamic stability of stoichiometric LaFeO 3 and BiFeO 3 : a hybrid DFT study
2017
BiFeO3 perovskite attracts great attention due to its multiferroic properties and potential use as a parent material for Bi1−xSrxFeO3−δ and Bi1−xSrxFe1−yCoyO3−δ solid solutions in intermediate temperature cathodes of oxide fuel cells. Another iron-based LaFeO3 perovskite is the end member for well-known solid solutions (La1−xSrxFe1−yCoyO3−δ) used for oxide fuel cells and other electrochemical devices. In this study an ab initio hybrid functional approach was used for the study of the thermodynamic stability of both LaFeO3 and BiFeO3 with respect to decompositions to binary oxides and to elements, as a function of temperature and oxygen pressure. The localized (LCAO) basis sets describing th…
DFT study of polarizabilities and dipole moments of water clusters
2005
Density functional theory (DFT) calculations with different exchange- correlation functionals, Becke's three-parameter exchange functional and the gradient- corrected functional of Lee, Yang, and Paar (B3LYP) and Becke's three-parameter functional with Perdew-Wang correlational functional (B3PW91), are performed to study the dielectric properties of small and medium-sized water clusters. For these H- bonded systems, we optimize the geometries and compute the dipole moments and polarizabilities using a supermolecule approach. The corresponding properties of the individual water molecules in the clusters are extracted from the molecular properties using the Hirshfeld expansion of the electron…
Linear scaling exchange gradients for Hartree–Fock and hybrid density functional theory
2000
Abstract A new method is introduced which allows to form the exchange part of self-consistent field energy gradients in a way which scales linearly with molecular size for molecules with a non-vanishing HOMO–LUMO gap. This is not only important for Hartree–Fock but as well for the popular hybrid density functional theory methods. The method preserves the optimized integral-driven structure of conventional direct methods. Efficiency and scaling behavior of the new method are illustrated for DNA fragments.
Deciphering the Role of Dipolar Interactions in Magnetic Layered Double Hydroxides
2018
Layered double hydroxides (LDHs) exhibit unparalleled anion exchange properties and the ability to be exfoliated into 2D nanosheets, which can be used as a building block to fabricate a wide variety of hybrid functional nanostructured materials. Still, if one wants to use LDHs as a magnetic building blocks in the design of complex architectures, the role played by the dipolar magnetic interactions in these layered materials needs to be understood. In this work, we synthesized and characterized a five-membered CoAl-LDH series with basal spacing ranging from 7.5 to 34 Å. A detailed experimental characterization allows us to conclude that the main factor governing the dipolar interactions betw…