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We construct a nonlocal density functional approximation with full exact exchange, while preserving the constraint-satisfaction approach and justified error cancellations of simpler semilocal functionals. This is achieved by interpolating…

Chemical Physics · Physics 2009-11-13 John P. Perdew , Viktor N. Staroverov , Jianmin Tao , Gustavo E. Scuseria

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

Nonlocal kinetic energy density functionals (KEDFs) with density-dependent kernels are currently the most accurate functionals available for orbital-free density functional theory (OF-DFT) calculations. However, despite advances in…

Materials Science · Physics 2024-12-05 Yongshuo Chen , Cheng Ma , Boning Cui , Tian Cui , Wenhui Mi , Qiang Xu , Yanchao Wang , Yanming Ma

Electron transfer with changing occupation in the 4f subshell poses a considerable challenge for quantitative predictions in quantum chemistry. Using the example of cerium oxide, we identify the main deficiencies of common…

Chemical Physics · Physics 2021-12-07 Tobias Schäfer , Nathan Daelman , Núria López

We investigate the behavior of oxygen vacancies in three different metal-oxide semiconductors (rutile and anatase TiO2, monoclinic WO3, and tetragonal ZrO2) using a recently proposed hybrid density-functional method in which the fraction of…

High-throughput computational screening has emerged as a critical component of materials discovery. Direct density functional theory (DFT) simulation of inorganic materials and molecular transition metal complexes is often used to describe…

Materials Science · Physics 2017-05-18 Jon Paul Janet , Heather J. Kulik

Performing high accuracy hybrid functional calculations for condensed matter systems containing a large number of atoms is at present computationally very demanding - when not out of reach - if high quality basis sets are used. We present a…

Materials Science · Physics 2017-12-22 Laura E. Ratcliff , A. Degomme , José A. Flores-Livas , Stefan Goedecker , Luigi Genovese

This work presents a new class of hybrid density functional theory (DFT) approximations, incorporating nonlocal exact exchange in predefined states such as core atomic orbitals (AOs). These projected hybrid density functionals are a…

Chemical Physics · Physics 2023-05-16 Benjamin G. Janesko

Orbital-free density functional theory (OF-DFT) holds the promise to compute ground state molecular properties at minimal cost. However, it has been held back by our inability to compute the kinetic energy as a functional of the electron…

Chemical Physics · Physics 2023-10-25 Roman Remme , Tobias Kaczun , Maximilian Scheurer , Andreas Dreuw , Fred A. Hamprecht

The accurate prediction of electronic and optical properties in chalcopyrite semiconductors has been a persistent challenge for density functional theory (DFT) based approaches. Addressing this issue, we demonstrate that very accurate…

Materials Science · Physics 2024-01-31 Arghya Ghosh , Subrata Jana , Dimple Rani , Manoar Hossain , Manish K Niranjan , Prasanjit Samal

We propose a new molecular simulation framework that combines the transferability, robustness and chemical flexibility of an ab initio method with the accuracy and efficiency of a machine learned force field. The key to achieve this mix is…

Computational Physics · Physics 2020-01-08 Sebastian Dick , Marivi Fernandez-Serra

By including a fraction of exact exchange (EXX), hybrid functionals reduce the self-interaction error in semi-local density functional theory (DFT), and thereby furnish a more accurate and reliable description of the electronic structure in…

Computational Physics · Physics 2021-05-10 Hsin-Yu Ko , Junteng Jia , Biswajit Santra , Xifan Wu , Roberto Car , Robert A. DiStasio

We present a density functional theory (DFT) for lattice models with local electron-electron (e-e) and electron-phonon (e-ph) interactions. Exchange-correlation potentials are derived via dynamical mean field theory for the…

Strongly Correlated Electrons · Physics 2019-09-04 E. Viñas Boström , P. Helmer , P. Werner , C. Verdozzi

We present a critical analysis of the popular fragment-orbital density-functional theory (FO-DFT) scheme for the calculation of electronic coupling values. We discuss the characteristics of different possible formulations or 'flavors' of…

Materials Science · Physics 2016-02-17 Christoph Schober , Karsten Reuter , Harald Oberhofer

Machine learning (ML) has recently gained attention as a means to develop more accurate exchange-correlation (XC) functionals for density functional theory, but functionals developed thus far need to be improved on several metrics,…

Chemical Physics · Physics 2022-03-14 Kyle Bystrom , Boris Kozinsky

For the theoretical understanding of the reactivity of complex chemical systems accurate relative energies between intermediates and transition states are required. Despite its popularity, density functional theory (DFT) often fails to…

Chemical Physics · Physics 2016-06-23 Gregor N. Simm , Markus Reiher

Recent advances in X-ray free-electron laser diagnostics have enabled direct probing of the electronic structure under extreme pressures and temperatures, such as those encountered in stellar interiors and inertial confinement fusion…

Time-dependent orbital-free density functional theory (TD-OFDFT) is an efficient ab-initio method for calculating the electronic dynamics of large systems. In comparison to standard TD-DFT, it computes only a single electronic state…

Chemical Physics · Physics 2021-12-15 Kaili Jiang , Xuecheng Shao , Michele Pavanello

The derivative discontinuity in the exact exchange-correlation potential of ensemble Density Functional Theory (DFT) is investigated at the specific integer number that corresponds to the maximum number of bound electrons, $J_{max}$. A…

Quantum Physics · Physics 2011-11-09 Daniel L. Whitenack , Yu Zhang , Adam Wasserman

Improving the accuracy and thus broadening the applicability of electronic density functional theory (DFT) is crucial to many research areas, from material science, to theoretical chemistry, biophysics and biochemistry. In the last three…

Strongly Correlated Electrons · Physics 2019-03-27 Paola Gori-Giorgi , Michael Seidl
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