Related papers: Charge-transfer steps in Density Functional Theory…
The accurate description of open-shell molecules, in particular of transition metal complexes and clusters, is still an important challenge for quantum chemistry. While density-functional theory (DFT) is widely applied in this area, the…
Two electrons at the threshold of ionization represent a severe test case for electronic structure theory. A pseudospectral method yields a very accurate density of the two-electron ion with nuclear charge close to the critical value.…
A single-term density functional model for nondynamic and strong correlation is presented, based on single-determinant Kohn-Sham density functional theory. It is derived from modeling the adiabatic connection and contains only two nonlinear…
This paper derives and demonstrates a new, purely density-based ab initio approach for calculation of the energies and properties of many-electron systems. It is based upon the discovery of relationships that govern the "mechanics" of the…
The reconstruction of the exchange-correlation potential from accurate ab initio electron densities can provide insights into the limitations of the currently available approximate functionals and provide guidance for devising improved…
The derivative discontinuity in the exact exchange-correlation potential of ensemble Density Functional Theory (DFT) is investigated at the specific integer number that corresponds to the maximum number of bound electrons, $J_{max}$. A…
Quantum-mechanically-driven charge polarization and charge transfer are ubiquitous in biomolecular systems, controlling reaction rates, allosteric interactions, ligand-protein binding, membrane transport, and dynamically-driven structural…
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…
As a first step to meet the challenge to calculate the electronic structure and total energy of charged states of atoms and molecules adsorbed on ultrathin-insulating films supported by a metallic substrate using density functional theory…
Spherical density functional theory (DFT) is a reformulation of the classic theorems of DFT, in which the role of the total density of a many-electron system is replaced by a set of sphericalized densities, constructed by…
Electron-phonon coupling (EPC) is key for understanding many properties of materials such as superconductivity and electric resistivity. Although first principles density-functional-theory (DFT) based EPC calculations are used widely, their…
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…
The study of electronic transitions within a molecule connected to the absorption or emission of light is a common task in the process of the design of new materials. The transitions are complex quantum mechanical processes and a detailed…
Quantum-chemical processes in liquid environments impact broad areas of science, from molecular biology to geology to electrochemistry. While density-functional theory (DFT) has enabled efficient quantum-mechanical calculations which…
The exact form of the kinetic energy functional has remained elusive in orbital-free models of density functional theory (DFT). This has been the main stumbling block for the development of a general-purpose framework on this basis. Here,…
Recent experimental advances in strongly coupled light-matter systems has sparked the development of general ab-initio methods capable of describing interacting light-matter systems from first principles. One of these methods,…
The theoretical and computational description of materials properties is a task of utmost scientific and technological importance. A first-principles description of electron-electron interactions poses an immense challenge that is usually…
In order to assess the accuracy of commonly used approximate exchange-correlation density functionals, we present a comparison of accurate exchange and correlation potentials, exchange energy densities and energy components with the…
We present a first-principles framework to extract deformation potentials in Silicon based on density-functional theory (DFT) and density-functional perturbation theory (DFPT). We compute the electronic band structures, phonon dispersion…
The Ziman formulation of electrical conductivity is tested in warm and hot dense matter using the pseudo-atom molecular dynamics method. Several implementation options that have been widely used in the literature are systematically tested…