Related papers: Open shells in reduced-density-matrix-functional t…
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…
We employ reduced density-matrix functional theory in the calculation of the fundamental gap of open-shell systems. The formula for the calculation of the fundamental gap is derived with special attention to the spin of the neutral and the…
Using the newly introduced theory of finite-temperature reduced density matrix functional theory, we apply the first-order approximation to the homogeneous electron gas. We consider both collinear spin states as well as symmetry broken…
By introducing the self-energy density functionals for the dissipative interactions between the reduced system and its environment, we develop a time-dependent density-functional theory formalism based on an equation of motion for the…
We apply reduced density-matrix functional theory to the parabolically confined quantum Hall droplet in the spin-frozen strong magnetic field regime. One-body reduced density matrix functional method performs remarkably well in obtaining…
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…
Based on our derivation of finite temperature reduced density matrix functional theory and the discussion of the performance of its first-order functional this work presents several different correlation-energy functionals and applies them…
In the recent work of S. Sharma \emph{et al.}, (arxiv.org: arxiv:0912.1118), a single-electron spectrum associated with the natural orbitals was defined as the derivative of the total energy with respect to the occupation numbers at half…
We prove that the electron density function of a real physical system can be uniquely determined by its values on any finite subsystem. This establishes the existence of a rigorous density-functional theory for any open electronic system.…
We consider density functionals for exchange and correlation energies in two-dimensional systems. The functionals are constructed by making use of exact constraints for the angular averages of the corresponding exchange and correlation…
We introduce an energy functional for ground-state electronic structure calculations. Its variables are the natural spin-orbitals of singlet many-body wave functions and their joint occupation probabilities deriving from controlled…
In this work we explore the performance of approximations to electron correlation in reduced density-matrix functional theory (RDMFT) and of approximations to the observables calculated within this theory. Our analysis focuses on the…
The problem of degenerate ground states of open-shell atoms is investigated in spin-restricted and unrestricted density functional theory using the exact exchange energy functional. For the spin-unrestricted case, spurious energy splittings…
A fermion ground state energy functional is set up in terms of particle density, relative pair density, and kinetic energy tensor density. It satisfies a minimum principle if constrained by a complete set of compatibility conditions. A…
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…
Density functional theory (DFT) embedding provides a formally exact framework for interfacing correlated wave-function theory (WFT) methods with lower-level descriptions of electronic structure. Here, we report techniques to improve the…
The quest for an approximate yet accurate kinetic energy density functional is central to the development of orbital-free density functional theory. While a recipe for closed-shell systems has been proposed earlier, we have shown that it…
Reduced density matrix functional theory for the case of solids is presented and a new exchange correlation functional based on a fractional power of the density matrix is introduced. We show that compared to other functionals, this…
Electrons in zero external magnetic field can be studied with density functional theory (DFT) or with spin-DFT (SDFT). The latter is normally used for open shell systems because its approximations appear to model better the exchange and…
We introduce a novel energy functional for ground-state electronic-structure calculations. Its fundamental variables are the natural spin-orbitals of the implied singlet many-body wave function and their joint occupation probabilities. The…