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Electronic states with fractional spins arise in systems with large static correlation (strongly correlated systems). Such fractional-spin states are shown to be ensembles of degenerate ground states with normal spins. It is proven here…

Other Condensed Matter · Physics 2009-11-13 Aron J. Cohen , Paula Mori-Sánchez , Weitao Yang

Standard approximations for the exchange-correlation functional are known to deviate from linear dependence of the energy on the electron and spin numbers (in -space). Violation of this flat-plane condition underlies the failure of all…

Classical Physics · Physics 2013-10-28 Ali M. Malek , Robert Balawender

The derivative discontinuity is a key concept in electronic structure theory in general and density functional theory in particular. The electronic energy of a quantum system exhibits derivative discontinuities with respect to different…

Chemical Physics · Physics 2017-09-13 Paula Mori-Sánchez , Aron J. Cohen

The fundamental gap is a central quantity in the electronic structure of matter. Unfortunately, the fundamental gap is not generally equal to the Kohn-Sham gap of density functional theory (DFT), even in principle. The two gaps differ…

Materials Science · Physics 2015-09-01 Eli Kraisler , Leeor Kronik

The derivative discontinuity in the exact exchange-correlation potential of ensemble Density Functional Theory (DFT) is investigated at the specific integer number that corresponds to the maximum number of bound electrons, $J_{max}$. A…

Quantum Physics · Physics 2011-11-09 Daniel L. Whitenack , Yu Zhang , Adam Wasserman

The design of better exchange-correlation functionals for Density Functional Theory (DFT) is a central challenge of modern electronic structure theory. However, current developments are limited by the mathematical form of the functional,…

Chemical Physics · Physics 2024-08-19 Kyle Bystrom , Boris Kozinsky

Approximate functionals used in practical density functional theory (DFT) deviate from the piecewise linear behavior of the exact functional for fractional charges. This deviation causes excess charge delocalization, which leads to…

Chemical Physics · Physics 2018-10-23 Diptarka Hait , Martin Head-Gordon

Perdew et al. [Phys. Rev. Lett 49, 1691 (1982)] discovered and proved two different properties of exact Kohn-Sham density functional theory (DFT): (i) The exact total energy versus particle number is a series of linear segments between…

Other Condensed Matter · Physics 2015-03-13 Tamar Stein , Jochen Autschbach , Niranjan Govind , Leeor Kronik , Roi Baer

The prominence of density functional theory (DFT) in the field of electronic structure computation stems from its ability to usefully balance accuracy and computational effort. At the base of this ability is a functional of the electron…

The calculation of the band-gap by density-functional theory (DFT) methods is examined by considering the behavior of the energy as a function of number of electrons. It is found that the incorrect band-gap prediction with most approximate…

Materials Science · Physics 2009-11-13 Aron J. Cohen , Paula Mori-Sánchez , Weitao Yang

The derivative discontinuity of the exchange-correlation functional of density-functional theory is cast as the difference of two types of electron affinities. We show that standard Kohn-Sham calculations can be used to calculate both…

Chemical Physics · Physics 2007-12-13 F. P. Rosselli , A. B. F. da Silva , K. Capelle

Charge transfer plays a crucial role in many processes of interest in physics, chemistry, and bio-chemistry. In many applications the size of the systems involved calls for time-dependent density functional theory (TDDFT) to be used in…

Chemical Physics · Physics 2017-10-11 Neepa T. Maitra

It is shown that the DFT exchange and correlation functionals satisfy an expression that couples exchange and correlation functionals and functional derivatives evaluated at three different densities and for two particle numbers. This…

Materials Science · Physics 2015-05-30 Daniel P. Joubert

The exact universal functional of integer charge leads to an extension to fractional charge asymptotically when it is applied to a system made of asymptotically separated densities. The extended functional is asymptotically local and is…

Chemical Physics · Physics 2024-12-17 Jing Kong

We propose a new approach to approximate the exchange and correlation (XC) functional in density functional theory. The XC potential is considered as an electrostatic potential, generated by a fictitious XC density, which is in turn a…

Chemical Physics · Physics 2013-05-29 Xavier Andrade , Alán Aspuru-Guzik

Spin is a fundamental property of any many-electron system. The ability of density functional theory to accurately predict the physical properties of a system, while varying its spin, is crucial for describing magnetic materials and…

Chemical Physics · Physics 2024-11-05 Alon Hayman , Eli Kraisler , Tamar Stein

Exchange interactions are a manifestation of the quantum mechanical nature of the electrons and play a key role in predicting the properties of materials from first principles. In density functional theory (DFT), a widely used approximation…

Materials Science · Physics 2020-03-27 Marco Bernardi

Density functional approximations to the exchange-correlation energy of Kohn-Sham theory, such as the local density approximation and generalized gradient approximations, lack the well-known integer discontinuity, a feature that is critical…

Chemical Physics · Physics 2015-06-18 Martin A. Mosquera , Adam Wasserman

The random phase approximation (RPA) to the correlation energy is extended to fractional occupations and its performance examined for exact conditions on fractional charges and fractional spins. RPA satisfies the constancy condition for…

Other Condensed Matter · Physics 2009-03-26 Paula Mori-Sánchez , Aron J. Cohen , Weitao Yang

We consider density functionals for exchange and correlation energies in two-dimensional systems. The functionals are constructed by making use of exact constraints for the angular averages of the corresponding exchange and correlation…

Strongly Correlated Electrons · Physics 2010-02-25 E. Rasanen , S. Pittalis
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