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Linear scaling methods for density-functional theory (DFT) simulations are formulated in terms of localised orbitals in real-space, rather than the delocalised eigenstates of conventional approaches. In local-orbital methods, relative to…

Materials Science · Physics 2011-05-30 N. D. M. Hine , M. Robinson , P. D. Haynes , C. -K. Skylaris , M. C. Payne , A. A. Mostofi

Due to efficient scaling with electron number N, density functional theory (DFT) is widely used for studies of large molecules and solids. Restriction of an exact mean-field theory to local potential functions has recently been questioned.…

Other Condensed Matter · Physics 2015-06-24 Robert K. Nesbet

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…

Linear scaling density functional theory approaches to electronic structure are often based on the tendency of electrons to localize even in large atomic and molecular systems. However, in many cases of actual interest, for example in…

Chemical Physics · Physics 2022-03-25 Marcel David Fabian , Ben Shpiro , Roi Baer

Localized basis sets in the projector augmented wave formalism allow for computationally efficient calculations within density functional theory (DFT). However, achieving high numerical accuracy requires an extensive basis set, which also…

Materials Science · Physics 2020-11-18 G. Gandus , A. Valli , D. Passerone , R. Stadler

Over many years, computational simulations based on Density Functional Theory (DFT) have been used extensively to study many different materials at the atomic scale. However, its application is restricted by system size, leaving a number of…

Mesoscale and Nanoscale Physics · Physics 2018-12-05 Carlos Romero-Muñiz , Ayako Nakata , Pablo Pou , David R. Bowler , Tsuyoshi Miyazaki , Rubén Pérez

We present an approach to the DFT+U method (Density Functional Theory + Hubbard model) within which the computational effort for calculation of ground state energies and forces scales linearly with system size. We employ a formulation of…

Strongly Correlated Electrons · Physics 2012-02-14 David D. O'Regan , Nicholas D. M. Hine , Mike C. Payne , Arash A. Mostofi

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…

Chemical Physics · Physics 2015-06-03 Jeng-Da Chai

We show that a lattice formulation of density-functional theory (DFT), guided by renormalization-group concepts, can be used to obtain numerical predictions of energy gaps, spin-density profiles, critical exponents, sound velocities,…

Strongly Correlated Electrons · Physics 2009-11-13 Francisco C. Alcaraz , Klaus Capelle

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…

Chemical Physics · Physics 2015-06-12 Jason D. Goodpaster , Taylor A. Barnes , Frederick R. Manby , Thomas F. Miller

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

We propose a novel scheme to bring reduced density matrix functional theory (RDMFT) into the realm of density functional theory (DFT) that preserves the accurate density functional description at equilibrium, while incorporating accurately…

Chemical Physics · Physics 2014-11-07 Nektarios N. Lathiotakis , Nicole Helbig , Angel Rubio , Nikitas I. Gidopoulos

This chapter presents controlled approximations of Kohn-Sham density functional theory (DFT) that enable very large scale simulations. The work is motivated by the study of defects in crystalline solids, though the ideas can be used in…

Materials Science · Physics 2021-12-14 Kaushik Bhattacharya , Vikram Gavini , Michael Ortiz , Mauricio Ponga , Phanish Suryanarayana

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…

Computational Physics · Physics 2015-12-23 Swarnava Ghosh , Phanish Suryanarayana

Density functional theory (DFT) is the most promising method for calculating quantum properties of molecules and materials at moderate and large scales. However, commonly used density functional approximations (DFAs) have systematic…

Chemical Physics · Physics 2026-03-24 Yichen Fan , Jacob Z. Williams , Weitao Yang

Density functional theory is a successful branch of numerical simulations of quantum systems. While the foundations are rigorously defined, the universal functional must be approximated resulting in a `semi'-ab initio approach. The search…

Quantum Physics · Physics 2017-11-22 James Daniel Whitfield , Norbert Schuch , Frank Verstraete

Density-potential functional theory (DPFT) is an alternative formulation of orbital-free density functional theory that may be suitable for modeling the electronic structure of large systems. To date, DPFT has been applied mainly to quantum…

Materials Science · Physics 2023-04-21 Martin-Isbjörn Trappe , William C. Witt , Sergei Manzhos

The practical utility of M{\o}ller-Plesset (MP) perturbation theory is severely constrained by the use of Hartree-Fock (HF) orbitals. It has recently been shown that use of regularized orbital-optimized MP2 orbitals and scaling of MP3…

Chemical Physics · Physics 2021-01-06 Adam Rettig , Diptarka Hait , Luke W. Bertels , Martin Head-Gordon

Constrained density functional theory (cDFT) is a versatile electronic structure method that enables ground-state calculations to be performed subject to physical constraints. It thereby broadens their applicability and utility. Automated…

Other Condensed Matter · Physics 2016-08-03 David D. O'Regan , Gilberto Teobaldi

Density-corrected density functional theory (DC-DFT) is enjoying substantial success in improving semilocal DFT calculations in a wide variety of chemical problems. This paper provides the formal theoretical framework and assumptions for…

Chemical Physics · Physics 2019-08-19 Stefan Vuckovic , Suhwan Song , John Kozlowski , Eunji Sim , Kieron Burke
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