Related papers: Understanding the core limitations of second-order…

In this perspective, the various measures of electron correlation used in wavefunction theory, density functional theory and quantum information theory are briefly reviewed. We then focus on a more traditional metric based on dominant…

Density Functional Theory (DFT) underpins much of modern computational chemistry and materials science. Yet, the reliability of DFT-derived predictions of experimentally measurable properties remains fundamentally limited by the need to…

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…

Modern extensions of density functional theory such as the density functional theory plus U and the density functional theory plus dynamical mean-field theory require choices, including selection of variable (charge vs spin density) for the…

Solving the Euler equation which corresponds to the energy minimum of a density functional expressed in orbital-free form involves related but distinct computational challenges. One is the choice between all-electron and pseudo-potential…

To address the impact of electron correlations in the linear and non-linear response regimes of interacting many-electron systems exposed to time-dependent external fields, we study one-dimensional (1D) systems where the interacting problem…

An explicitly orbital-dependent correlation energy functional is proposed, which is to be used in combination with the orbital-dependent exchange energy functional in energy-band calculations. It bears a close resemblance to the…

Using a linear combination of atomic orbitals approach, we report a systematic comparison of various Density Functional Theory (DFT) and hybrid exchange-correlation functionals for the prediction of the electronic and structural properties…

We present an approach based on density-functional theory for the calculation of fundamental gaps of both finite and periodic two-dimensional (2D) electronic systems. The computational cost of our approach is comparable to that of total…

The electronic and magnetic properties of many strongly-correlated systems are controlled by a limited number of states, located near the Fermi level and well isolated from the rest of the spectrum. This opens a formal way for combining the…

This review explains the relationship between density functional theory and strongly correlated models using the simplest possible example, the two-site Hubbard model. The relationship to traditional quantum chemistry is included. Even in…

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…

We present a new paradigm for the design of exchange-correlation functionals in density-functional theory. Electron pairs are correlated explicitly by means of the recently developed second order Bethe-Goldstone equation (BGE2) approach.…

We present a density difference based analysis for a range of orbital--dependent Kohn--Sham functionals. Results for atoms, some members of the neon isoelectronic series and small molecules are reported and compared with ab initio…

Finding accurate exchange-correlation (XC) functionals remains the defining challenge in density functional theory (DFT). Despite 40 years of active development, the desired chemical accuracy is still elusive with existing functionals. We…

Hydrogen bonding is an important non-covalent interaction that plays a major role in molecular self-organization and supramolecular structures. It can be described accurately with ab initio quantum chemical wave function methods, which…

Lack of memory (locality in time) is a major limitation of almost all present time-dependent density functional approximations. By using semiclassical dynamics to compute correlation effects within a density-matrix functional approach, we…

A geometry-based density functional theory is presented for mixtures of hard spheres, hard needles and hard platelets; both the needles and the platelets are taken to be of vanishing thickness. Geometrical weight functions that are…

Unlike covalent two-dimensional (2D) materials like graphene, 2D metals have non-layered structures due to their non-directional, metallic bonding. While experiments on 2D metals are still scarce and challenging, density-functional theory…

We reexamine the recently introduced basis-set correction theory based on density-functional theory consisting in correcting the basis-set incompleteness error of wave-function methods using a density functional. We use a one-dimensional…