Density Functionals for Correlation Energies of Atoms and Molecules

Stoll, Hermann; Savin, Andreas

doi:10.1007/978-1-4757-0818-9_7

Cited by 98 publications

(70 citation statements)

References 56 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Even the best approximations of its key ingredient, the exchange-correlation (XC) energy functional, cannot describe strong electron correlations, like those of the cuprates, and cannot exactly cancel the so-called self-interaction, a property which the exact functional should satisfy. On top of that, they fail to recover long-range van der Waals interactions, 4 are not completely safe for the description of the hydrogen bond, 5 and have intrinsic problems with situations of near degeneracy (when two sets of Kohn-Sham orbitals have very close energies); 6,7,8 more generally, the "chemical accuracy" has not yet been reached. To overcome the latter group of problems, there has been a growing interest in "mixed schemes" which combine the DFT with other approximate methods by splitting the coulombic electron-electron interaction 1/r = v ee (r) into a short-range (SR) and a long-range (LR) part (see e.g.…”

Section: Density Functional Theorymentioning

confidence: 99%

Local-spin-density functional for multideterminant density functional theory

Paziani¹,

et al. 2006

View full text Add to dashboard Cite

Based on exact limits and quantum Monte Carlo simulations, we obtain, at any density and spin polarization, an accurate estimate for the energy of a modified homogeneous electron gas where electrons repel each other only with a long-range coulombic tail. This allows us to construct an analytic local-spin-density exchange-correlation functional appropriate to new, multideterminantal versions of the density functional theory, where quantum chemistry and approximate exchange-correlation functionals are combined to optimally describe both long-and short-range electron correlations.

show abstract

Section: Density Functional Theorymentioning

confidence: 99%

Local-spin-density functional for multideterminant density functional theory

Paziani¹,

et al. 2006

View full text Add to dashboard Cite

show abstract

“…Another route to explore is the combination of the present periodic CIS method with TD-DFT (or its Tamm-Dancoff approximation) in the framework of a longrange-short-range separation of the electron-electron interaction operator. 78 …”

Section: Discussionmentioning

confidence: 99%

Local ab initio methods for calculating optical bandgaps in periodic systems. II. Periodic density fitted local configuration interaction singles method for solids

Lorenz

Maschio

Schütz

et al. 2012

The Journal of Chemical Physics

View full text Add to dashboard Cite

Local ab initio methods for calculating optical band gaps in periodic systems. I. Periodic density fitted local configuration interaction singles method for polymers J. Chem. Phys. 134, 094101 (2011) We present a density fitted local configuration interaction singles (CIS) method for calculating optical bandgaps in 3D-periodic systems. We employ an Ewald technique to carry out infinite lattice summations for the exciton-exciton interaction, and robust product-density specific local density fitting in direct space for the electron-hole interaction. Moreover, we propose an alternative to the usual cyclic model with Born-von Karman periodic boundary conditions, the so called Wigner-Seitz supercell truncated infinite model, which exhibits much improved convergence of the CIS excitation energy with respect to the size of the supercell. Test calculations on a series of prototypical systems demonstrate that the method at the present stage can be used to calculate the excitonic bandgaps of 3D periodic systems with up to a dozen atoms in the unit cell, ranging from wide-gap insulators to semiconductors.

show abstract

“…This suggests a range-separation of the electron-electron interaction and a treatment of the long-range component with methods that can describe static correlation [107][108][109][110][111]. Subsequently approximate RDMFT functionals have been used for the long-range part [112,113], thus establishing a hybrid DFT-RDMFT scheme.…”

Section: Hybrid Theoriesmentioning

confidence: 99%

Reduced density-matrix functionals from many-particle theory

Schade

Kamil

Blöchl

2017

Eur. Phys. J. Spec. Top.

View full text Add to dashboard Cite

Abstract. In materials with strong electron correlation the proper treatment of local atomic physics described by orbital occupations is crucial. Reduced density-matrix functional theory is a natural extension of density functional theory for systems that are dominated by orbital physics. We review the current state of reduced density-matrix functional theory (RDMFT). For atomic structure relaxations or abinitio molecular dynamics the combination of density functional theory (DFT) and dynamical mean-field theory (DMFT) possesses a number of disadvantages, like the cumbersome evaluation of forces. We therefore describe a method, DFT+RDMFT, that combines many-particle effects based on reduced density-matrix functional theory with a density functional-like framework. A recent development is the construction of density-matrix functionals directly from many-particle theory such as methods from quantum chemistry or many-particle Green's functions. We present the underlying exact theorems and describe current progress towards quantitative functionals.

show abstract

Density Functionals for Correlation Energies of Atoms and Molecules

Cited by 98 publications

References 56 publications

Local-spin-density functional for multideterminant density functional theory

Local-spin-density functional for multideterminant density functional theory

Local ab initio methods for calculating optical bandgaps in periodic systems. II. Periodic density fitted local configuration interaction singles method for solids

Reduced density-matrix functionals from many-particle theory

Contact Info

Product

Resources

About