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Rigorous formulation of two-parameter double-hybrid density-functionals  [PDF]
Emmanuel Fromager
Physics , 2011, DOI: 10.1063/1.3671384
Abstract: A two-parameter extension of the density-scaled double hybrid approach of Sharkas et al. [J. Chem. Phys. 134, 064113 (2011)] is presented. It is based on the explicit treatment of a fraction of multideterminantal exact exchange. The connection with conventional double hybrids is made when neglecting density scaling in the correlation functional as well as second-order corrections to the density. In this context, the fraction ac of second-order M{\o}ller-Plesset (MP2) correlation energy is not necessarily equal to the square of the fraction ax of Hartree-Fock exchange. More specifically, it is shown that ac \leq ax2, a condition that conventional semi-empirical double hybrids actually fulfill. In addition, a new procedure for calculating the orbitals, which has a better justification than the one routinely used, is proposed. Referred to as {\lambda}1 variant, the corresponding double hybrid approximation has been tested on a small set consisting of H2, N2, Be2, Mg2, and Ar2. Three conventional double hybrids (B2-PLYP, B2GP-PLYP, and PBE0-DH) have been considered. Potential curves obtained with {\lambda}1- and regular double hybrids can, in some cases, differ significantly. In particular, for the weakly bound dimers, the {\lambda}1 variants bind systematically more than the regular ones, which is an improvement in many but not all cases. Including density scaling in the correlation functionals may of course change the results significantly. Moreover, optimized effective potentials based on a partially-interacting system could also be used to generate proper orbitals. Work is currently in progress in those directions.
Density-based mixing parameter for hybrid functionals  [PDF]
Miguel A. L. Marques,Julien Vidal,Micael J. T. Oliveira,Lucia Reining,Silvana Botti
Physics , 2010, DOI: 10.1103/PhysRevB.83.035119
Abstract: A very popular ab-initio scheme to calculate electronic properties in solids is the use of hybrid functionals in density functional theory (DFT) that mixes a portion of Fock exchange with DFT functionals. In spite of their success, a major problem still remains, related to the use of one single mixing parameter for all materials. Guided by physical arguments that connect the mixing parameter to the dielectric properties of the solid, and ultimately to its band gap, we propose a method to calculate this parameter from the electronic density alone. This method is able to cut significantly the error of traditional hybrid functionals for large and small gap materials, while retaining a good description of structural properties. Moreover, its implementation is simple and leads to a negligible increase of the computational time.
Analysis of double hybrid density-functionals along the adiabatic connection  [PDF]
Yann Cornaton,Odile Franck,Andrew M. Teale,Emmanuel Fromager
Physics , 2013, DOI: 10.1080/00268976.2013.783640
Abstract: We present a graphical analysis of the adiabatic connections underlying double-hybrid density-functional methods that employ second-order perturbation theory. Approximate adiabatic connection formulae relevant to the construction of these functionals are derived and compared directly with those calculated using accurate ab initio methods. The discontinuous nature of the approximate adiabatic integrands is emphasized, the discontinuities occurring at interaction strengths which mark the transitions between regions that are: (i) described predominantly by second- order perturbation theory (ii) described by a mixture of density-functional and second-order perturbation theory contributions and (iii) described purely by density-functional theory. Numerical examples are presented for a selection of small molecular systems and van der Waals dimers. The impacts of commonly used approximations in each of the three sections of the adiabatic connection are discussed along with possible routes for the development of improved double-hybrid methodologies.
Hybrid functionals for solids with an optimized Hartree-Fock mixing parameter  [PDF]
David Koller,Peter Blaha,Fabien Tran
Physics , 2013, DOI: 10.1088/0953-8984/25/43/435503
Abstract: (Screened) hybrid functionals are being used more and more for solid-state calculations. Usually the fraction alpha of Hartree-Fock exchange is kept fixed during the calculation, however there is no single (universal) value for alpha which systematically leads to satisfying accuracy. Instead, one could use a property of the system under consideration to determine alpha and in this way the functional would be more flexible and potentially more accurate. Recently, it was proposed to use the static dielectric constant epsilon for the calculation of alpha [Shimazaki and Asai, Chem. Phys. Lett. 466, 91 (2008) and Marques et al., Phys. Rev. B 83, 035119 (2011)]. We explore this idea further and propose a scheme where the connection between epsilon and alpha is optimized based on experimental band gaps. epsilon, and thus alpha, is recalculated at each iteration of the self-consistent procedure. We present results for the band gap and lattice constant of various semiconductors and insulators with this procedure. In addition, we show that this approach can also be combined with a non-self-consistent hybrid approximation to speed up the calculations considerably, while retaining an excellent accuracy in most cases.
Double-hybrid density-functional theory applied to molecular crystals  [PDF]
Kamal Sharkas,Julien Toulouse,Lorenzo Maschio,Bartolomeo Civalleri
Physics , 2014, DOI: 10.1063/1.4890439
Abstract: We test the performance of a number of two- and one-parameter double-hybrid approximations, combining semilocal exchange-correlation density functionals with periodic local second-order M{\o}ller-Plesset (LMP2) perturbation theory, for calculating lattice energies of a set of molecular crystals: urea, formamide, ammonia, and carbon dioxide. All double-hybrid methods perform better on average than the corresponding Kohn-Sham calculations with the same functionals, but generally not better than standard LMP2. The one-parameter double-hybrid approximations based on the PBEsol density functional gives lattice energies per molecule with an accuracy of about 6 kJ/mol, which is similar to the accuracy of LMP2. This conclusion is further verified on molecular dimers and on the hydrogen cyanide crystal.
Seeking for reliable double-hybrid density functionals without fitting parameters: The PBE0-2 functional  [PDF]
Jeng-Da Chai,Shan-Ping Mao
Physics , 2012, DOI: 10.1016/j.cplett.2012.04.045
Abstract: Without the use of any empirical fitting to experimental or high-level ab initio data, we present a double-hybrid density functional approximation for the exchange-correlation energy, combining the exact Hartree-Fock exchange and second-order Moller-Plesset (MP2) correlation with the Perdew-Burke-Ernzerhof (PBE) functional. This functional, denoted as PBE0-2, is shown to be accurate for a wide range of applications, when compared with other functionals and the ab initio MP2 method. The qualitative failures of conventional density functional approximations, such as self-interaction error and noncovalent interaction error, are significantly reduced by PBE0-2.
Double-hybrid density-functional theory with meta-generalized-gradient approximations  [PDF]
Sidi Ould Souvi,Kamal Sharkas,Julien Toulouse
Physics , 2013, DOI: 10.1063/1.4865963
Abstract: We extend the previously proposed one-parameter double-hybrid density-functional theory [K. Sharkas, J. Toulouse, and A. Savin, J. Chem. Phys. 134, 064113 (2011)] to meta-generalized-gradient-approximation (meta-GGA) exchange-correlation density functionals. We construct several variants of one-parameter double-hybrid approximations using the Tao-Perdew-Staroverov-Scuseria (TPSS) meta-GGA functional and test them on test sets of atomization energies and reaction barrier heights. The most accurate variant uses the uniform coordinate scaling of the density and of the kinetic energy density in the correlation functional, and improves over both standard Kohn-Sham TPSS and second-order Moller-Plesset calculations.
Color centers in NaCl by hybrid functionals  [PDF]
Wei Chen,Christoph Tegenkamp,Herbert Pfnür,Thomas Bredow
Physics , 2010, DOI: 10.1103/PhysRevB.82.104106
Abstract: We present in this work the electronic structure and transition energies (both thermodynamic and optical) of Cl vacancies in NaCl by hybrid density functionals. The underestimated transition energies by the semi-local functional inherited from the band gap problem are recovered by the PBE0 hybrid functional through the non-local exact exchange, whose amount is adjusted to reproduce the experimental band gap. The hybrid functional also gives a better account of the lattice relaxation for the defect systems arising from the reduced self-interaction. On the other hand, the quantitative agreement with experimental vertical transition energy cannot be achieved with hybrid functionals due to the inaccurate descriptions of the ionization energies of the localized defect and the positions of the band edges.
A General MSSM Parameter Scan  [PDF]
Andre Sopczak
Physics , 2000, DOI: 10.1142/S0217751X01008187
Abstract: The excluded tan(beta) range and Higgs boson mass regions in the framework of the Minimal Supersymmetric extension of the Standard Model (MSSM) depend on several parameters. The Higgs boson masses, cross-sections and branching fractions have been determined including two-loop diagrammatic calculations. The limits obtained with a more general scan over the parameter space of the MSSM are compared with those in the so-called benchmark scenario. The combination of the searches for Higgs particles in the 1999 data collected by the DELPHI collaboration at center-of-mass energies between 191.6 and 201.7 GeV allows stringent limits to be set in combination with previous DELPHI results. In addition, an interpretation in the framework of the general MSSM scan of the 2000 LEP data at the hightest energies between 201.7 and 209.0 GeV is given. We show that the current data for the HZ and hA production can be comfortably accommodated in the MSSM.
Hybrid inverse problems and internal functionals  [PDF]
Guillaume Bal
Mathematics , 2011,
Abstract: This paper reviews recent results on hybrid inverse problems, which are also called coupled-physics inverse problems of multi-wave inverse problems. Inverse problems tend to be most useful in, e.g., medical and geophysical imaging, when they combine high contrast with high resolution. In some settings, a single modality displays either high contrast or high resolution but not both. In favorable situations, physical effects couple one modality with high contrast with another modality with high resolution. The mathematical analysis of such couplings forms the class of hybrid inverse problems. Hybrid inverse problems typically involve two steps. In a first step, a well-posed problem involving the high-resolution low-contrast modality is solved from knowledge of boundary measurements. In a second step, a quantitative reconstruction of the parameters of interest is performed from knowledge of the point-wise, internal, functionals of the parameters reconstructed during the first step. This paper reviews mathematical techniques that have been developed in recent years to address the second step. Mathematically, many hybrid inverse problems find interpretations in terms of linear and nonlinear (systems of) equations. In the analysis of such equations, one often needs to verify that qualitative properties of solutions to elliptic linear equations are satisfied, for instance the absence of any critical points. This paper reviews several methods to prove that such qualitative properties hold, including the method based on the construction of complex geometric optics solutions.
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