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

While quantum computers have shown significant promise for electronic structure calculations, their potential to accelerate density functional theory (DFT) calculations remains unclear. In this work, we present a qubit-efficient encoding…

Orbital-free density functional theory (OF-DFT) constitutes a computationally highly effective tool for modeling electronic structures of systems ranging from room-temperature materials to warm dense matter. Its accuracy critically depends…

Presented here are calculations of the distortion of the density of an electron gas due to the electrostatic field of a proton. Several models based upon the local density approximation (LDA) of density functional theory [linear response…

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…

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…

Natural orbitals, defined in electronic structure and quantum chemistry as the (molecular) orbitals diagonalizing the one-particle reduced density matrix of the ground state, have been conjectured for decades to be the perfect reference…

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…

We explore the simplification of widely used meta-generalized-gradient approximation (mGGA) exchange-correlation functionals to the Laplacian level of refinement by use of approximate kinetic energy density functionals (KEDFs). Such…

We validate the application of our recent orbital-free density functional theory (DFT) approach, [Phys. Rev. Lett. 113, 155006 (2014)], for the calculation of ionic and electronic transport properties of dense plasmas. To this end, we…

Attempts to go beyond the local density approximation (LDA) of Density Functional Theory (DFT) have been increasingly based on the incorporation of more realistic Coulomb interactions. In their earliest implementations, methods like…

In this paper, we investigate the energy minimization model of the ensemble Kohn-Sham density functional theory for metallic systems, in which a pseudo-eigenvalue matrix and a general smearing approach are involved. We study the invariance…

In this review we provide a rigorous and self-contained presentation of one-body reduced density-matrix (1RDM) functional theory. We do so for the case of a finite basis set, where density-functional theory (DFT) implicitly becomes a 1RDM…

A widely used approximation to the exchange-correlation functional in density functional theory is the local density approximation (LDA), typically derived from the properties of the homogeneous electron gas (HEG). We previously introduced…

Adopting an accurate kinetic energy density functional (KEDF) to characterize the noninteracting kinetic energy within the framework of orbital-free density functional theory (OFDFT) is challenging. We propose a new form of the non-local…

Most realistic calculations of moderately correlated materials begin with a ground-state density functional theory (DFT) calculation. While Kohn-Sham DFT is used in about 40,000 scientific papers each year, the fundamental underpinnings are…

We propose hybrid schemes incorporating exact exchange into thermally-assisted-occupation density functional theory (TAO-DFT) [J.-D. Chai, J. Chem. Phys. 136, 154104 (2012)] for an improved description of nonlocal exchange effects. With a…

We present an accurate local density-functional for electronic-structure calculations within the density functional theory (DFT). The functional is derived by analyzing the structure of the standard perturbative expansion of the correlation…

A method is presented, which employs the density matrix renormalization group technique in order to construct exact ground state exchange correlation functionals for models of correlated electron systems coupled to external reservoirs. The…

We review the role of self-consistency in density functional theory. We apply a recent analysis to both Kohn-Sham and orbital-free DFT, as well as to Partition-DFT, which generalizes all aspects of standard DFT. In each case, the analysis…

Kohn-Sham Density Functional Theory (KS-DFT) has been traditionally solved by the Self-Consistent Field (SCF) method. Behind the SCF loop is the physics intuition of solving a system of non-interactive single-electron wave functions under…