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Embedded density functional theory (e-DFT) is used to describe the electronic structure of strongly interacting molecular subsystems. We present a general implementation of the Exact Embedding (EE) method [J. Chem. Phys. 133, 084103 (2010)]…

Other Condensed Matter · Physics 2011-07-27 Jason D. Goodpaster , Taylor A. Barnes , Thomas F. Miller

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

Density functional theory (DFT), the most widely adopted method in modern computational chemistry, fails to describe accurately the electronic structure of strongly correlated systems. Here we show that DFT can be formally and practically…

Chemical Physics · Physics 2022-04-18 Daniel Gibney , Jan-Niklas Boyn , David A. Mazziotti

Effective field theory (EFT) methods are applied to density functional theory (DFT) as part of a program to systematically go beyond mean-field approaches to medium and heavy nuclei. A system of fermions with short-range, natural…

Nuclear Theory · Physics 2007-05-23 S. J. Puglia , A. Bhattacharyya , R. J. Furnstahl

Quantum-electrodynamical density-functional theory (QEDFT) provides a promising avenue for exploring complex light-matter interactions in optical cavities for real materials. Similar to conventional density-functional theory, the Kohn-Sham…

Computational Physics · Physics 2024-02-16 I-Te Lu , Michael Ruggenthaler , Nicolas Tancogne-Dejean , Simone Latini , Markus Penz , Angel Rubio

The optimized effective potential (OEP) method is a promising technique for calculating the ground state properties of a system within the density functional theory. However, it is not widely used as its computational cost is rather high…

Materials Science · Physics 2016-12-15 Taro Fukazawa , Hisazumi Akai

The interaction between excited states of a closed-shell chromophore and a nearby free radical species gives rise to spin-coupled doublet states, namely singdoublet and tripdoublet, as well as a quartet state. This coupling facilitates…

Chemical Physics · Physics 2025-03-25 Chenyu Liu , Yang Xu , Peng Bao , Yangyi Lu , Jiali Gao

Due to efficient scaling with electron number N, density functional theory (DFT) is widely used for studies of large molecules and solids. Restriction of an exact mean-field theory to local potential functions has recently been questioned.…

Other Condensed Matter · Physics 2015-06-24 Robert K. Nesbet

A description of non-collinear magnetism in the framework of spin-density functional theory is presented for the exact exchange energy functional which depends explicitly on two-component spinor orbitals. The equations for the effective…

We introduce 'single-particle-exact density functional theory' (1pEx-DFT), a novel density functional approach that represents all single-particle contributions to the energy with exact functionals. Here, we parameterize interaction energy…

Using the optimized effective potential method in conjunction with the semi-analytical approximation due to Krieger, Li and Iafrate, we have performed fully self-consistent exact exchange-only density-functional calculations for diatomic…

chem-ph · Physics 2008-02-03 T. Grabo , E. K. U. Gross

The performance of correlated optimized effective potential (OEP) functionals based on the spin-resolved second-order correlation energy is analyzed. The relative importance of singly- and doubly- excited contributions as well as the effect…

Chemical Physics · Physics 2014-07-31 I. Grabowski , E. Fabiano , A. Teale , S. Śmiga , A. Buksztel , F. Della Sala

We present a Gaussian-basis implementation of orbital-free density-functional theory (OF-DFT) in which the trust-region image method (TRIM) is used for optimization. This second-order optimization scheme has been constructed to provide…

Chemical Physics · Physics 2021-09-15 Matthew S. Ryley , Michael Withnall , Tom J. P. Irons , Trygve Helgaker , Andrew M. Teale

According to the Hohenberg-Kohn theorem of density-functional theory (DFT), all observable quantities of systems of interacting electrons can be expressed as functionals of the ground-state density. This includes, in principle, the spin…

Strongly Correlated Electrons · Physics 2019-09-04 Carsten A. Ullrich

Most approximate exchange-correlation functionals used within density functional theory are constructed as the sum of two distinct contributions for exchange and correlation. Separating the exchange component from the entire functional is…

Condensed Matter · Physics 2009-10-28 Claudia Filippi , C. J. Umrigar , Xavier Gonze

The energy density functional (EDF) method is currently the only microscopic theoretical approach able to tackle the entire nuclear chart. Nevertheless, it suffers from limitations resulting from its empirical character and deteriorating…

Nuclear Theory · Physics 2024-04-04 Kilian Fraboulet , Jean-Paul Ebran

For exchange-correlation functionals that depend explicitly on the Kohn-Sham orbitals, the potential $V_{\mathrm{xc}\sigma}(\re)$ must be obtained as the solution of the optimized effective potential (OEP) integral equation. This is very…

Materials Science · Physics 2009-11-07 Stephan Kümmel , John P. Perdew

Kohn-Sham Density Functional Theory (KS-DFT) has been traditionally solved by the Self-Consistent Field (SCF) method. Behind the SCF loop is the physics intuition of solving a system of non-interactive single-electron wave functions under…

We propose hybrid schemes incorporating exact exchange into thermally-assisted-occupation density functional theory (TAO-DFT) [J.-D. Chai, J. Chem. Phys. 136, 154104 (2012)] for an improved description of nonlocal exchange effects. With a…

Chemical Physics · Physics 2017-01-24 Jeng-Da Chai

Quantum mechanical methods based on the density functional theory (DFT) offer a realistic possibility of first-principles design of organic donor-acceptor systems and engineered band-gap materials. This promise is contingent upon the…

Chemical Physics · Physics 2013-12-03 Marcin Modrzejewski , Grzegorz Chałasiński , Małgorzata M. Szczęśniak