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This chapter concerns with the recent development of a new DFT methodology for accurate, reliable prediction of many-electron systems. Background, need for such a scheme, major difficulties encountered, as well as their potential remedies…

Chemical Physics · Physics 2019-04-19 Amlan K. Roy

We consider a system of particles interacting via a purely repulsive, soft-core potential recently introduced to model effective pair interactions between dendrimers, which is expected to lead to the formation of crystals with multiple…

Soft Condensed Matter · Physics 2015-05-11 Davide Pini

We investigate fundamental properties of meta-generalized-gradient approximations (meta-GGAs) to the exchange-correlation energy functional, which have an implicit density dependence via the Kohn-Sham kinetic-energy density. To this…

Chemical Physics · Physics 2014-12-10 F. G. Eich , Maria Hellgren

Gross-Oliveira-Kohn density-functional theory (GOK-DFT) is an extension of DFT to excited states where the basic variable is the ensemble density, i.e. the weighted sum of ground- and excited-state densities. The ensemble energy (i.e. the…

Strongly Correlated Electrons · Physics 2018-07-17 Killian Deur , Laurent Mazouin , Bruno Senjean , Emmanuel Fromager

We argue that the success of DFT can be understood in terms of a semiclassical expansion around a very specific limit. This limit was identified long ago by Lieb and Simon for the total electronic energy of a system. This is a universal…

Chemical Physics · Physics 2021-05-18 Pavel Okun , Kieron Burke

We present an extension of reverse engineered Kohn-Sham potentials from a density matrix renormalization group calculation towards the construction of a density functional theory functional via deep learning. Instead of applying machine…

Disordered Systems and Neural Networks · Physics 2021-05-05 Peter Schmitteckert

Degenerate perturbation theory from quantum mechanics is inadequate in density functional theory (DFT) because of nonlinearity in the Kohn-Sham potential. Herein, we develop the fully general perturbation theory for open-shell, degenerate…

Materials Science · Physics 2017-07-19 Mark C. Palenik , Brett I. Dunlap

The stochastic density functional theory (DFT) [Phys. Rev. Lett. 111, 106402 (2013)] is a valuable linear scaling approach to Kohn-Sham DFT that does not rely on the sparsity of the density matrix. Linear (and often sub-linear) scaling is…

Chemical Physics · Physics 2019-02-20 Ming Chen , Roi Baer , Daniel Neuhauser , Eran Rabani

Density functional theory (DFT) has transformed our ability to investigate and understand electronic ground states. In its original formulation, however, DFT is not suited to addressing (e.g.) degenerate ground states, mixed states with…

Chemical Physics · Physics 2025-10-30 Tim Gould , Leeor Kronik , Stefano Pittalis

Gross--Oliveira--Kohn (GOK) ensemble density-functional theory (GOK-DFT) is a time-\textit{independent} extension of density-functional theory (DFT) which allows to compute excited-state energies via the derivatives of the ensemble energy…

Chemical Physics · Physics 2020-06-18 Clotilde Marut , Bruno Senjean , Emmanuel Fromager , Pierre-François Loos

Screened range-separated hybrid (SRSH) functionals within generalized Kohn-Sham density functional theory (GKS-DFT) have been shown to restore a general $1/(r\varepsilon)$ asymptotic decay of the electrostatic interaction in dielectric…

Computational Physics · Physics 2023-06-26 Tammo van der Heide , Bálint Aradi , Ben Hourahine , Thomas Frauenheim , Thomas A. Niehaus

A long-standing puzzle in density-functional theory is the issue of the long-range behavior of the Kohn-Sham exchange-correlation potential at metal surfaces. As an important step towards its solution, it is proved here, through a rigurouos…

Materials Science · Physics 2015-05-18 C. M. Horowitz , C. R. Proetto , J. M. Pitarke

DFT calculations have become widespread in both chemistry and materials, because they usually provide useful accuracy at much lower computational cost than wavefunction-based methods. All practical DFT calculations require an approximation…

Chemical Physics · Physics 2022-03-15 Eunji Sim , Suhwan Song , Stefan Vuckovic , Kieron Burke

We present a method to make highly accurate pseudopotentials for use with orbital-free density functional theory (OF-DFT) with given exchange-correlation and kinetic energy functionals, which avoids the compounding of errors of Kohn-Sham…

Materials Science · Physics 2015-02-04 Fleur Legrain , Sergei Manzhos

In the near future, material and drug design may be aided by quantum computer assisted simulations. These have the potential to target chemical systems intractable by the most powerful classical computers. However, the resources offered by…

Ensemble Density Functional Theory (EDFT) is a generalization of ground-state Density Functional Theory (GS DFT), which is based on an exact formal theory of finite collections of a system's ground and excited states. EDFT in various forms…

Materials Science · Physics 2024-08-27 Remi J. Leano , Aurora Pribram-Jones , David A. Strubbe

We study the accuracy of Kohn-Sham density functional theory (DFT) for warm- and hot-dense matter (WDM and HDM). Specifically, considering a wide range of systems, we perform accurate ab initio molecular dynamics simulations with…

Computational Physics · Physics 2024-11-21 Phanish Suryanarayana , Arpit Bhardwaj , Xin Jing , Shashikant Kumar , John E. Pask

We propose a local real-space formulation for orbital-free DFT with density dependent kinetic energy functionals and a unified variational framework for computing the configurational forces associated with geometry optimization of both…

Materials Science · Physics 2015-06-15 Sambit Das , Mrinal Iyer , Vikram Gavini

We review and expand on our work to impose constraints on the effective Kohn Sham (KS) potential of local and semi-local density functional approximations. In this work, we relax a previously imposed positivity constraint, which increased…

In this paper, we consider an approximation method, and a novel general analysis, for second-order elliptic differential equations with heterogeneous multiscale coefficients. We obtain convergence of the Generalized Multi-scale Finite…

Numerical Analysis · Mathematics 2024-12-20 Eduardo Abreu , Ciro Diaz , Juan Galvis