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We show that as an electron transfers between closed-shell molecular fragments at large separation, the exact correlation potential of time-dependent density functional theory gradually develops a step and peak structure in the bonding…

Chemical Physics · Physics 2014-02-11 Johanna I. Fuks , Peter Elliott , Angel Rubio , Neepa T. Maitra

We present and test a new approximation for the exchange-correlation (xc) energy of Kohn-Sham density functional theory. It combines exact exchange with a compatible non-local correlation functional. The functional is by construction free…

Chemical Physics · Physics 2014-05-23 Tobias Schmidt , Eli Kraisler , Adi Makmal , Leeor Kronik , Stephan Kümmel

It was recently shown [Y. Suzuki, L. Lacombe, K. Watanabe, and N. T. Maitra, Phys. Rev. Lett. 119, 263401 (2017)] that peak and valley structures in the exact exchange-correlation potential of time-dependent density functional theory are…

Chemical Physics · Physics 2018-07-04 Lionel Lacombe , Yasumitsu Suzuki , Kazuyuki Watanabe , Neepa T. Maitra

Thermal density functional theory calculations often use the Mermin-Kohn-Sham scheme, but employ ground-state approximations to the exchange-correlation (XC) free energy. In the simplest solvable nontrivial model, an asymmetric Hubbard…

Strongly Correlated Electrons · Physics 2016-06-29 Justin C Smith , Aurora Pribram-Jones , Kieron Burke

Physically valid and numerically efficient approximations for the exchange and correlation energy are critical for reduced density-matrix functional theory to become a widely used method in electronic structure calculations. Here we examine…

Strongly Correlated Electrons · Physics 2016-03-23 A. Putaja , F. G. Eich , T. Baldsiefen , E. Rasanen

In approximate Kohn-Sham density-functional theory, self-interaction manifests itself as the dependence of the energy of an orbital on its fractional occupation. This unphysical behavior translates into qualitative and quantitative errors…

Materials Science · Physics 2010-09-28 Ismaila Dabo , Andrea Ferretti , Nicolas Poilvert , Yanli Li , Nicola Marzari , Matteo Cococcioni

We construct a nonlocal density functional approximation with full exact exchange, while preserving the constraint-satisfaction approach and justified error cancellations of simpler semilocal functionals. This is achieved by interpolating…

Chemical Physics · Physics 2009-11-13 John P. Perdew , Viktor N. Staroverov , Jianmin Tao , Gustavo E. Scuseria

Exact-exchange energy density and energy density of a semilocal density functional approximation are two key ingredients for modeling the static correlation, a strongly nonlocal functional of the density, through a local hybrid functional.…

Materials Science · Physics 2009-11-13 Jianmin Tao , Viktor N. Staroverov , Gustavo E. Scuseria , John P. Perdew

We analyze possible nonlinear exciton-exciton correlation effects in the optical response of semiconductors by using a time-dependent density-functional theory (TDDFT) approach. For this purpose, we derive the nonlinear (third-order) TDDFT…

Materials Science · Physics 2015-06-16 Volodymyr Turkowski , Michael N. Leuenberger

We first exploit the physical condition satisfying the symmetry relation of the ``exact'' spin-resolved exchange correlation kernel based on the ``mixed scheme'' in soft magnetic layered systems. The conditions are derived and examined by…

Strongly Correlated Electrons · Physics 2007-05-23 Ina Yeo , Kyung-Soo Yi

A complete understanding of a material requires both knowledge of the excited states as well as of the ground state. In particular, the low energy excitations are of utmost importance while studying the electronic, magnetic, dynamical, and…

Materials Science · Physics 2019-01-30 N. Singh , P. Elliott , T. Nautiyal , J. K. Dewhurst , S. Sharma

Certain excitations, especially ones of long-range charge transfer character, are poorly described by time-dependent density functional theory (TDDFT) when typical (semi-)local functionals are used. A proper description of these excitations…

Chemical Physics · Physics 2018-08-01 J. Garhammer , F. Hofmann , R. Armiento , S. Kümmel

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 exchanging the energy functionals in ground-state DFT with physically equivalent exact force expressions as a new promising route towards approximations to the exchange-correlation potential and energy. In analogy to the usual…

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

A new class of orbital-dependent exchange-correlation (xc) potentials for applications in noncollinear spin-density-functional theory is developed. Starting from the optimized effective potential (OEP) formalism for the exact exchange…

Mesoscale and Nanoscale Physics · Physics 2018-08-01 Carsten A. Ullrich

A decomposition of the exact exchange-correlation potential of time-dependent density functional theory into an interaction component and a kinetic component offers a new starting point for non- adiabatic approximations. The components are…

Chemical Physics · Physics 2018-11-14 Johanna I. Fuks , Lionel Lacombe , Soeren E. B. Nielsen , Neepa T. Maitra

The exchange-correlation hole and potential of the homogeneous electron gas have been investigated within the random-phase approximation, employing the plasmon-pole approximation for the linear density response function. The angular…

Strongly Correlated Electrons · Physics 2023-04-12 K. Karlsson , F. Aryasetiawan

We present an alternative to the Kohn-Sham formulation of density functional theory for the ground-state properties of strongly interacting electronic systems. The idea is to start from the limit of zero kinetic energy and systematically…

Strongly Correlated Electrons · Physics 2015-05-13 Paola Gori-Giorgi , Michael Seidl , G. Vignale

A method for calculating the Kohn--Sham exchange-correlation potential, $v_\text{XC}(\mathbf{r})$, from a given electronic wavefunction is devised and implemented. It requires on input one- and two-electron density matrices and involves…

Chemical Physics · Physics 2015-08-19 Ilya G. Ryabinkin , Sviataslau V. Kohut , Viktor N. Staroverov