相关论文: Orbitals from local RDMFT: Are they Kohn-Sham or N…

In contrast to the original Kohn-Sham (KS) formalism, we propose a density functional theory (DFT) with fractional orbital occupations for the study of ground states of many-electron systems, wherein strong static correlation is shown to be…

We present fully empirical exchange-correlation functionals to be used within reduced density matrix functional theory (RDMFT). These are of the popular J-K form, where the function of the occupation numbers that multiplies the Fock orbital…

Orbital-free density functional theory (OF-DFT) runs at low computational cost that scales linearly with the number of simulated atoms, making it suitable for large-scale material simulations. It is generally considered that OF-DFT strictly…

A system of electrons in a local or nonlocal external potential can be studied with 1-matrix functional theory (1MFT), which is similar to density functional theory (DFT) but takes the one-particle reduced density matrix (1-matrix) instead…

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 general procedure underlying Hartree-Fock and Kohn-Sham density functional theory calculations consists in optimizing orbitals for a self-consistent solution of the Roothaan-Hall equations in an iterative process. It is often ignored…

The practical success of density functional theory (DFT) is largely credited to the Kohn-Sham approach, which enables the exact calculation of the non-interacting electron kinetic energy via an auxiliary noninteracting system. Yet, the…

Reduced density-matrix functional theory (RDMFT) is a promising alternative approach to the problem of electron correlation. Like standard density functional theory, it contains an unknown exchange-correlation functional, for which several…

We present a $\Delta$-machine learning model for obtaining Kohn-Sham accuracy from orbital-free density functional theory (DFT) calculations. In particular, we employ a machine learned force field (MLFF) scheme based on the kernel method to…

Density functional theory (DFT), the most widely adopted method in modern computational chemistry, fails to describe accurately the electronic structure of strongly correlated systems. Here we show that DFT can be formally and practically…

Currently, there is a growing interest in the development of a new hierarchy of methods based on the concept of seniority, which has been introduced quite recently in quantum chemistry. Despite the enormous potential of these methods, the…

Hubertus J. J. van Dam [Phys. Rev. A 93, 052512, 2016] claims that the one-particle reduced density matrix (1RDM) of an interacting system can be represented by means of a single-determinant wavefunction of fictitious non-interacting…

This chapter provides a comprehensive review of fundamental concepts related to approximate natural orbital functionals (NOFs), emphasizing their significance in quantum chemistry and physics. Focusing on fermions, the discussion excludes…

Favorably scaling numerical time-dependent many-electron techniques such as time-dependent density functional theory (TDDFT) with adiabatic exchange-correlation potentials typically fail in capturing highly correlated electron dynamics. We…

Reduced density-matrix functional theory (RDMFT) provides a variational route to electronic correlations beyond conventional density-functional approximations, but explicit evaluations of density-matrix functionals still scale exponentially…

In many of the approximate functionals in one-body reduced density matrix (1RDM) functional theory, the approximate two-body reduced density matrix (2RDM) in the natural orbital representation only depends on the natural occupation numbers.…

It is found that, in closed-$l$-shell atoms, the exact local exchange potential $v_{\text{x}}(\bf r)$ of the density functional theory (DFT) is very well represented, within the region of every atomic shell, by each of the suitably shifted…

Incorporating nuclear shell effects within the framework of orbital-free density functional theory (DFT) has remained a longstanding challenge in nuclear physics. While the Hohenberg-Kohn theorem formally guarantees the existence of an…

We introduce a practical hybrid approach that combines orbital-free density functional theory (DFT) with Kohn-Sham DFT for speeding up first-principles molecular dynamics simulations. Equilibrated ionic configurations are generated using…

In this paper, we study a few theoretical issues in the discretized Kohn-Sham (KS) density functional theory (DFT). The equivalence between either a local or global minimizer of the KS total energy minimization problem and the solution to…