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The average energy curvature as a function of the particle number is a molecule-specific quantity, which measures the deviation of a given functional from the exact conditions of density functional theory (DFT). Related to the lack of…

Chemical Physics · Physics 2020-11-11 Alberto Fabrizio , Benjamin Meyer , Clemence Corminboeuf

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…

Strongly Correlated Electrons · Physics 2015-03-20 Tim Baldsiefen , F. G. Eich , E. K. U. Gross

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…

Strongly Correlated Electrons · Physics 2015-02-26 Stefano Di Sabatino , Jan A. Berger , Lucia Reining , Pina Romaniello

The Kohn-Sham equations underlie many important applications such as the discovery of new catalysts. Recent machine learning work on catalyst modeling has focused on prediction of the energy, but has so far not yet demonstrated significant…

Machine Learning · Computer Science 2023-10-31 Phillip Pope , David Jacobs

We use the exact strong-interaction limit of the Hohenberg-Kohn energy density functional to approximate the exchange-correlation energy of the restricted Kohn-Sham scheme. Our approximation corresponds to a highly non-local density…

Strongly Correlated Electrons · Physics 2012-12-12 Francesc Malet , Paola Gori-Giorgi

A sufficiently damped iteration of the Kohn-Sham equations with the exact functional is proven to always converge to the true ground-state density, regardless of the initial density or the strength of electron correlation, for finite…

Materials Science · Physics 2013-08-30 Lucas O. Wagner , E. M. Stoudenmire , Kieron Burke , Steven R. White

In the distributed nucleus approximation we represent the singular nucleus as smeared over a smallportion of a Cartesian grid. Delocalizing the nucleus allows us to solve the Poisson equation for theoverall electrostatic potential using a…

chem-ph · Physics 2009-10-28 Karthik A. Iyer , Michael P. Merrick , Thomas L. Beck

All-electron calculations play an important role in density functional theory, in which improving computational efficiency is one of the most needed and challenging tasks. In the model formulations, both nonlinear eigenvalue problem and…

Computational Physics · Physics 2020-07-29 Bin Gao , Guanghui Hu , Yang Kuang , Xin Liu

We propose a systematic procedure for the approximation of density functionals in density functional theory that consists of two parts. First, for the efficient approximation of a general density functional, we introduce an efficient ansatz…

Strongly Correlated Electrons · Physics 2016-08-29 Michael Lubasch , Johanna I. Fuks , Heiko Appel , Angel Rubio , J. Ignacio Cirac , Mari-Carmen Bañuls

We propose a lattice density-functional theory for {\it ab initio} quantum chemistry or physics as a route to an efficient approach that approximates the full configuration interaction energy and orbital occupations for molecules with…

Strongly Correlated Electrons · Physics 2019-04-19 J. P. Coe

We describe a numerical algorithm for approximating the equilibrium-reduced density matrix and the effective (mean force) Hamiltonian for a set of system spins coupled strongly to a set of bath spins when the total system (system+bath) is…

Quantum Physics · Physics 2023-01-25 Tyler Chen , Yu-Chen Cheng

One of the goals in the development of large scale electronic structure methods is to perform calculations explicitly for a localised region of a system, while still taking into account the rest of the system outside of this region. An…

Materials Science · Physics 2009-10-01 J. R. Trail , D. M. Bird

We compare Kohn-Sham results (density, cohesive energy, size and effect of charging) of the Spherical Averaged Pseudopotential Model with the Stabilized Jellium Model for clusters of sodium and aluminum with less than 20 atoms. We find that…

Condensed Matter · Physics 2009-10-30 Armando Vieira , M. Begona Torres , Carlos Fiolhais , L. Carlos Balbas

Frozen Density Embedding (FDE) represents a versatile embedding scheme to describe the environmental effect on the electron dynamics in molecular systems. The extension of the general theory of FDE to the real-time time-dependent Kohn-Sham…

We present, within Kohn-Sham Density Functional Theory calculations, a quantitative method to identify and assess the partitioning of a large quantum mechanical system into fragments. We then show how within this framework simple…

Chemical Physics · Physics 2017-09-28 Stephan Mohr , Michel Masella , Laura E. Ratcliff , Luigi Genovese

This article generalizes the notion of the local density of a many-body system to introduce collective coordinates as explicit degrees of freedom. It is shown that the energy of the system can be expressed as a functional of this object.…

Nuclear Theory · Physics 2014-04-23 Thomas Lesinski

Self-consistent theory of electron localization in disordered systems is generalized for the case of interacting electrons. We propose and critically compare a number of possible self-consistency schemes which take into account the lowest…

Condensed Matter · Physics 2008-02-03 E. Z. Kuchinskii , M. V. Sadovskii , V. G. Suvorov

We show an $\textit{ab initio}$ construction of the energy density functional (EDF) for electron systems using the functional renormalization group. The correlation energies of the homogeneous electron gas given in our framework reproduce…

Strongly Correlated Electrons · Physics 2021-08-03 Takeru Yokota , Tomoya Naito

The quantum mechanical ground state of electrons is described by Density Functional Theory, which leads to large minimization problems. An efficient minimization method uses a selfconsistent field (SCF) solution of large eigenvalue…

Materials Science · Physics 2007-05-23 Claus Bendtsen , Ole H. Nielsen , Lars B. Hansen

We show that the energetics and lifetimes of resonances of finite systems under an external electric field can be captured by Kohn--Sham density functional theory (DFT) within the formalism of uniform complex scaling. Properties of…

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