相关论文: Occupation numbers in density-functional calculati…

Density functional theory is the workhorse of modern electronic structure calculations, with wide-ranging applications in chemistry, physics, materials science, and machine learning. At its heart lies the exchange-correlation functional, a…

I review arguments demonstrating how the concept of "particle" numbers arises in the form of equidistant energy eigenvalues of coupled harmonic oscillators representing free fields. Their quantum numbers (numbers of nodes of the wave…

A theory is developed for magnetically confined Fermi gas at low temperature based on the density functional theory. The theory is illustrated by numerical calculation of density distributions of Fermi atoms $^{40}$K with parameters…

We show that the spectrum and eigenstates of open-shell multicharged atomic ions near the ionization threshold are chaotic, as a result of extremely high level densities of multiply excited electron states ($10^3 eV^{-1}$ in Au^{24+}) and…

We adopt the so--called \emph{occupation number representation}, originally used in quantum mechanics and recently adopted in the description of several classical systems, in the analysis of the dynamics of some models of closed ecosystems.…

The analytic energy gradients in the atomic orbital representation have recently been published (J. Chem. Phys. 146, 014102, 2017) within the framework of the natural orbital functional theory (NOFT). We provide here an alternative…

We present the theory of orbital ordering in orbital-degenerate itinerant electron systems. After proposing the criterion of instability for orbital ordering or orbital density wave ordering, we find that the orbital and the spin-orbital…

We point out an error in the argument [PRL 105, 013002 (2010)] that the time independence of the occupation numbers in the adiabatic approximation follows from the invariance of the ground-state interaction energy functional with respect to…

Quantitatively accurate electronic structure calculations rely on the proper description of electron correlation. A judicious choice of the approximate quantum chemistry method depends upon the importance of dynamic and nondynamic…

In this work, a new functional is introduced to treat pairing correlations in finite many-body systems. Guided by the projected BCS framework, the energy is written as a functional of occupation numbers. It is shown to generalize the BCS…

Local density approximation (LDA) to the density functional theory (DFT) has continuous derivative of total energy as a number of electrons function and continuous exchange-correlation potential, while in exact DFT both should be…

The breaking of orbital degeneracy on a transition metal cation and the resulting unequal electronic occupations of these orbitals provide a powerful lever over electron density and spin ordering in metal oxides. Here, we show how to…

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 role of the generalized Pauli constraints (GPCs) in higher spatial dimensions and by incorporating spin degrees of freedom is systematically explored for a system of interacting fermions confined by a harmonic trap. Physical relevance…

We investigate the suitability of natural orbitals as a basis for describing many-body excitations. We analyze to which extend the natural orbitals describe both bound as well as ionized excited states and show that depending on the…

Oxygen vacancies at the SnO2(110) and (101) surface and subsurface sites have been studied in the framework of density functional theory by using both all-electron Gaussian and pseudopotential plane-wave methods. The all-electron…

We present a real-space formulation and higher-order finite-difference implementation of periodic Orbital-free Density Functional Theory (OF-DFT). Specifically, utilizing a local reformulation of the electrostatic and kernel terms, we…

A two-parameter extension of the density-scaled double hybrid approach of Sharkas et al. [J. Chem. Phys. 134, 064113 (2011)] is presented. It is based on the explicit treatment of a fraction of multideterminantal exact exchange. The…

Density functional theory (DFT) offers a desirable balance between quantitative accuracy and computational efficiency in practical many-electron calculations. Its central component, the exchange-correlation energy functional, has been…

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,…