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A framework for developing new approximate electronic structure methods is presented, in which the correlation energy of a many-electron system in the ground state is computed as in the single-reference second-order many-body perturbation…

Chemical Physics · Physics 2011-06-15 Dimitri Laikov

Approximate functionals used in practical density functional theory (DFT) deviate from the piecewise linear behavior of the exact functional for fractional charges. This deviation causes excess charge delocalization, which leads to…

Chemical Physics · Physics 2018-10-23 Diptarka Hait , Martin Head-Gordon

A fundamental weakness of density functional theory (DFT) is the difficulty in making systematic improvements to approximations for the exchange and correlation functionals. In this paper, we follow a wave-function-based approach [N.I.…

Chemical Physics · Physics 2018-10-05 Timothy J. Callow , Nikitas I. Gidopoulos

We evaluate, by means of variational calculations, the bound state energy E_B of a pair of charges located on the surface of a cylinder, interacting via Coulomb potential - e^2 / r . The trial wave function involves three variational…

Condensed Matter · Physics 2009-11-07 M. K. Kostov , M. W. Cole , G. D. Mahan

Nuclear density functional theory (DFT) is the only microscopic, global approach to the structure of atomic nuclei. It is used in numerous applications, from determining the limits of stability to gaining a deep understanding of the…

Nuclear Theory · Physics 2015-02-06 Nicolas Schunck , Jordan D. McDonnell , Jason Sarich , Stefan M. Wild , Dave Higdon

Electron dispersion forces play a crucial role in determining the structure and properties of biomolecules, molecular crystals and many other systems. However, an accurate description of dispersion is highly challenging, with the most…

Materials Science · Physics 2013-01-30 Jiří Klimeš , Angelos Michaelides

We decompose the energy error of any variational DFT calculation into a contribution due to the approximate functional and that due to the approximate density. Typically, the functional error dominates, but in many interesting situations,…

Chemical Physics · Physics 2015-06-12 Min-Cheol Kim , Eunji Sim , Kieron Burke

An extension of the Variational Quantum Eigensolver (VQE) method is presented where a quantum computer generates an accurate exchange-correlation potential for a Density Functional Theory (DFT) simulation on classical hardware. The method…

Quantum Physics · Physics 2019-03-14 Ryan Hatcher , Jorge A. Kittl , Christopher Bowen

Diamond defects are among the most promising qubits. Modelling their properties through accurate quantum mechanical simulations can further their development into robust units of information. We use the recently developed capped density…

Quantum Physics · Physics 2026-03-23 John Mark P. Martirez

The piecewise linearity condition on the total energy with respect to the total magnetization of finite quantum systems is derived, using the infinite-separation-limit technique. This generalizes the well-known constancy condition, related…

Strongly Correlated Electrons · Physics 2024-07-22 Andrew C. Burgess , Edward Linscott , David D. O'Regan

DFT calculations have become widespread in both chemistry and materials, because they usually provide useful accuracy at much lower computational cost than wavefunction-based methods. All practical DFT calculations require an approximation…

Chemical Physics · Physics 2022-03-15 Eunji Sim , Suhwan Song , Stefan Vuckovic , Kieron Burke

Based on a functional-integral formalism, a generalization of the self-energy-functional theory (SFT) is proposed which is applicable to systems of interacting electrons with disorder. Similar to the pure case without disorder, a…

Strongly Correlated Electrons · Physics 2013-05-29 Michael Potthoff , Matthias Balzer

Orbital-optimized density functional theory (DFT) has emerged as an alternative to time-dependent (TD) DFT capable of describing difficult excited states with significant electron density redistribution, such as charge-transfer, Rydberg,…

Chemical Physics · Physics 2025-01-22 Hanh D. M. Pham , Rustam Z. Khaliullin

The theorems of density functional theory (DFT) and reduced density matrix functional theory (RDMFT) establish a bijective map between the external potential of a many-body system and its electron density or one-particle reduced density…

Chemical Physics · Physics 2023-02-22 Xuecheng Shao , Lukas Paetow , Mark E. Tuckerman , Michele Pavanello

Embedded density functional theory (e-DFT) is used to describe the electronic structure of strongly interacting molecular subsystems. We present a general implementation of the Exact Embedding (EE) method [J. Chem. Phys. 133, 084103 (2010)]…

Other Condensed Matter · Physics 2011-07-27 Jason D. Goodpaster , Taylor A. Barnes , Thomas F. Miller

A Hamiltonian based approach using spatially localized projection operators is introduced to give precise meaning to the chemically intuitive idea of the electronic energy on a quantum subsystem. This definition facilitates the study of…

Quantum Physics · Physics 2015-06-11 Yaser R. Khan , Paul Brumer

A variational method is studied based on the minimum of energy variance. The method is tested on exactly soluble problems in quantum mechanics, and is shown to be a useful tool whenever the properties of states are more relevant than the…

High Energy Physics - Phenomenology · Physics 2009-01-07 Luca Marotta , Fabio Siringo

The efficiency of the variational perturbation theory [Phys. Rev. C {\bf 62}, 045503 (2000)] formulated recently for many-particle systems is examined by calculating the ground state correlation energy of the 3D electron gas with the…

Strongly Correlated Electrons · Physics 2009-11-07 Sang Koo You , Noboru Fukushima

Van der Waals interactions between two neutral but polarizable systems at a separation $R$ much larger than the typical size of the systems are at the core of a broad sweep of contemporary problems in settings ranging from atomic, molecular…

High Energy Physics - Phenomenology · Physics 2017-06-14 Nora Brambilla , Vladyslav Shtabovenko , Jaume Tarrús Castellà , Antonio Vairo

Methods for correcting residual energy errors of configuration interaction (CI) calculations of molecules and other electronic systems are discussed based on the assumption that the energy defect can be mapped onto atomic regions. The…

Chemical Physics · Physics 2022-10-05 Jerry L. Whitten
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