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The systematic underestimation of band gaps is one of the most fundamental challenges in semilocal density functional theory (DFT). In addition to hindering the application of DFT to predicting electronic properties, the band gap problem is…

Chemical Physics · Physics 2024-08-27 Kyle Bystrom , Stefano Falletta , Boris Kozinsky

Density-functional theory (DFT) has revolutionized computational prediction of atomic-scale properties from first principles in physics, chemistry and materials science. Continuing development of new methods is necessary for accurate…

State-of-the-art methods for calculating neutral excitation energies are typically demanding and limited to single electron-hole pairs and their composite plasmons. Here we introduce excitonic density-functional theory (XDFT) a…

Chemical Physics · Physics 2023-01-09 Subhayan Roychoudhury , Stefano Sanvito , David D. O'Regan

The exact ground-state exchange-correlation functional of Kohn-Sham density functional theory yields the exact transmission through an Anderson junction at zero bias and temperature. The exact impurity charge susceptibility is used to…

Mesoscale and Nanoscale Physics · Physics 2015-06-03 Zhenfei Liu , Justin P. Bergfield , Kieron Burke , Charles A. Stafford

Density functional theory (DFT) is an exact alternative formulation of quantum mechanics, in which it is possible to calculate the total energy, the spin and the charge density of many-electron systems in the ground state. In practice, it…

Atomic Physics · Physics 2014-03-25 Uri Argaman , Guy Makov , Eli Kraisler

We report a local, weight-dependent correlation density-functional approximation that incorporates information about both ground and excited states in the context of density-functional theory for ensembles (eDFT). This density-functional…

Chemical Physics · Physics 2020-06-05 Pierre-François Loos , Emmanuel Fromager

Density functional theory (DFT) provides a theoretical framework for efficient and fairly accurate calculations of the electronic structure of molecules and crystals. The main features of density functional theory are described and DFT…

Chemical Physics · Physics 2012-06-12 Hauke Paulsen , Alfred Xaver Trautwein

We present libvdwxc, a general library for evaluating the energy and potential for the family of vdW-DF exchange--correlation functionals. libvdwxc provides an efficient implementation of the vdW-DF method and can be interfaced with various…

Materials Science · Physics 2021-01-14 Ask Hjorth Larsen , Mikael Kuisma , Joakim Löfgren , Yann Pouillon , Paul Erhart , Per Hyldgaard

We consider electronic exchange and correlation effects in density-functional calculations of two-dimensional systems. Starting from wave function calculations of total energies and electron densities of inhomogeneous model systems, we…

Mesoscale and Nanoscale Physics · Physics 2012-05-30 Ilja Makkonen , Mikko M. Ervasti , Ville Kauppila , Ari Harju

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

An overview of the Conquest linear scaling density functional theory (DFT) code is given, focussing particularly on the scaling behaviour on modern high- performance computing (HPC) platforms. We demonstrate that essentially perfect linear…

Materials Science · Physics 2010-02-03 D. R. Bowler , T. Miyazaki

We show that the exact exchange-correlation potential of time-dependent density-functional theory displays dynamical step structures that have a spatially non-local and time non-local dependence on the density. Using one-dimensional…

Chemical Physics · Physics 2015-06-12 Peter Elliott , Johanna I. Fuks , Angel Rubio , Neepa T. Maitra

The predominance of Kohn-Sham density functional theory (KS-DFT) for the theoretical treatment of large experimentally relevant systems in molecular chemistry and materials science relies primarily on the existence of efficient software…

Computational Physics · Physics 2020-07-08 David B. Williams-Young , Wibe A. de Jong , Hubertus J. J. van Dam , Chao Yang

Electron transfer with changing occupation in the 4f subshell poses a considerable challenge for quantitative predictions in quantum chemistry. Using the example of cerium oxide, we identify the main deficiencies of common…

Chemical Physics · Physics 2021-12-07 Tobias Schäfer , Nathan Daelman , Núria López

Machine learning (ML) has recently gained attention as a means to develop more accurate exchange-correlation (XC) functionals for density functional theory, but functionals developed thus far need to be improved on several metrics,…

Chemical Physics · Physics 2022-03-14 Kyle Bystrom , Boris Kozinsky

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

We establish the theoretical foundations for embedding a correlated wave function in an environment formed by Kohn-Sham orbitals. We show that introducing an approximation which equates two, in principle distinct, kinetic-energy functionals…

Chemical Physics · Physics 2026-03-06 Enzo Monino , Daria Drwal , Michał Hapka , Libor Veis , Katarzyna Pernal

Density functional theory (DFT) is the most promising method for calculating quantum properties of molecules and materials at moderate and large scales. However, commonly used density functional approximations (DFAs) have systematic…

Chemical Physics · Physics 2026-03-24 Yichen Fan , Jacob Z. Williams , Weitao Yang

Rare-earth oxides (REOs) are an important class of materials owing to their unique properties, including high ionic conductivities, large dielectric constants, and elevated melting temperatures, making them relevant to several technological…

We argue that any general mathematical measure of density error, no matter how reasonable, is too arbitrary to be of universal use. However the energy functional itself provides a universal relevant measure of density errors. For the…

Computational Physics · Physics 2018-11-13 Eunji Sim , Suhwan Song , Kieron Burke