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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

The sensitivity of computed DFT (Density Functional Theory) molecular properties (including energetics, geometries, vibrational frequencies, and infrared intensities) to the radial and angular numerical integration grid meshes, as well as…

Chemical Physics · Physics 2012-08-27 Jan M. L. Martin , Charles W. Bauschlicher, , Alessandra Ricca

Linear-response time-dependent (TD) density-functional theory (DFT) has been implemented in the pseudopotential wavelet-based electronic structure program BigDFT and results are compared against those obtained with the all-electron…

Density functional calculations can fail for want of an accurate exchange-correlation approximation. The energy can instead be extracted from a sequence of density functional calculations of conditional probabilities (CP-DFT). Simple CP…

High-entropy alloys (HEAs) exhibit exceptional catalytic performance due to their complex surface structures. However, the vast number of active binding sites in HEAs, as opposed to conventional alloys, presents a significant computational…

Materials Science · Physics 2024-08-22 Mohamed Hendy , Okan K. Orhan , Homin Shin , Ali Malek , Mauricio Ponga

Accurate modeling in the warm dense matter regime is a persistent challenge with the most detailed models such as quantum molecular dynamics and path integral Monte Carlo being immensely computationally expensive. Density functional theory…

Materials Science · Physics 2024-09-04 Sameen Yunus , David A. Strubbe

Self-interaction is a fundamental flaw of practical Kohn-Sham Density Functional Theory (KS DFT) approximations responsible for numerous qualitative and even catastrophic shortcomings. Whereas self-interaction is easy to characterize in…

Chemical Physics · Physics 2024-07-16 Samuel A. Slattery , Edward F. Valeev

The implementation of an efficient self-consistent field (SCF) method including both scalar relativistic effects and spin-orbit interaction in density functional theory (DFT) is presented. We make use of Gaussian-type orbitals (GTOs) and…

Chemical Physics · Physics 2024-05-03 Yannick J. Franzke , Werner M. Schosser , Fabian Pauly

Multi-configurational wave functions are known to describe electronic structure across a Born-Oppenheimer surface qualitatively correct. However, for quantitative reaction energies, dynamical correlation originating from the many…

Chemical Physics · Physics 2020-04-16 Christopher J. Stein , Markus Reiher

We present a differentiation framework for plane-wave density-functional theory (DFT) that combines the strengths of forward-mode algorithmic differentiation (AD) and density-functional perturbation theory (DFPT). In the resulting AD-DFPT…

Materials Science · Physics 2025-12-23 Niklas Frederik Schmitz , Bruno Ploumhans , Michael F. Herbst

A hybrid Kohn-Sham Density Functional Theory (KS-DFT) and 1-electron Reduced Density Matrix Functional Theory (1-RDMFT) has recently been developed to describe strongly correlated systems at mean-field computational cost. This approach…

Computational Physics · Physics 2025-04-14 Daniel Gibney , Jan-Niklas Boyn

We construct a reference benchmark set for atomic and molecular random-phase-approximation (RPA) correlation energies in a density functional theory (DFT) framework at the complete basis set limit. This set is used to evaluate the accuracy…

Chemical Physics · Physics 2013-02-22 E. Fabiano , F. Della Sala

Standard approximations for the exchange-correlation (XC) functional in Kohn-Sham density functional theory (KS-DFT) typically lead to unacceptably large errors when applied to strongly-correlated electronic systems. Partition-DFT (PDFT) is…

Chemical Physics · Physics 2023-09-12 Yi Shi , Yuming Shi , Adam Wasserman

An approach is proposed for evaluating dipolar and multipolar inter-site interactions in strongly correlated materials. This approach is based on the single-site dynamical mean-field theory (DMFT) in conjunction with the atomic…

Strongly Correlated Electrons · Physics 2016-09-13 L. V. Pourovskii

We discuss various ways to handle self-interaction corrections (SIC) to Density Functional Theory (DFT) calculations. To that end, we use a simple model of few particles in a finite number of states together with a simple zero-range…

Other Condensed Matter · Physics 2009-11-13 P. M. Dinh , J. Messud , P. -G. Reinhard , E. Suraud

The strong-coupling perturbation theory (SCPT) for correlated electron systems is extended to the case of full Coulomb interaction. The Coulomb mechanism of the orbital polarization is discussed and attention is paid to the importance of…

Strongly Correlated Electrons · Physics 2007-05-23 I. Sandalov , U. Lundin , O. Eriksson

The knowledge of effective masses is a key ingredient to analyze numerous properties of semiconductors, like carrier mobilities, (magneto-)transport properties, or band extrema characteristics yielding carrier densities and density of…

A new and thorough derivation of linear-response subsystem time-dependent density functional theory (TD-DFT) is presented and analyzed in detail. Two equivalent derivations are presented and naturally yield self-consistent subsystem TD-DFT…

Chemical Physics · Physics 2013-06-12 Michele Pavanello

The treatment of degenerate states within Kohn-Sham density functional theory (KS-DFT) is a problem of longstanding interest. We propose a solution to this mapping from the interacting degenerate system to that of the noninteracting fermion…

Materials Science · Physics 2009-11-07 Viraht Sahni , Xiao-Yin Pan

A spin-current density-functional theory (SCDFT) is introduced, which takes into account currents of the spin-density and thus currents of the magnetization in addition to the electron density, the non-collinear spin-density, and the…

Materials Science · Physics 2009-11-11 Stefan Rohra , Andreas Goerling
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