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A generalization of the Kohn--Sham approach is derived where the correlation-energy functional depends on the one-particle density matrix of noninteracting states and on the external potential from the interacting target-state. The…

Chemical Physics · Physics 2007-05-23 James P. Finley

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

In this study, we propose a quantum-classical hybrid scheme for performing orbital-free density functional theory (OFDFT) using probabilistic imaginary-time evolution (PITE), designed for the era of fault-tolerant quantum computers (FTQC),…

Quantum Physics · Physics 2024-07-24 Yusuke Nishiya , Hirofumi Nishi , Taichi Kosugi , Yu-ichiro Matsushita

Correlated systems at both zero and nonzero temperature are treated here from a novel angle using a functional method. This functional method is an extension of the usual effective potential method. Here, however the effective action is…

Condensed Matter · Physics 2007-05-23 A. Rebei , W. N. G. Hitchon

We present a new theory for partitioning simulations of periodic and solid-state systems into physically sound atomic contributions at the level of Kohn-Sham density functional theory. Our theory is based on spatially localized linear…

Chemical Physics · Physics 2024-10-01 Luna Zamok , Janus J. Eriksen

A direct orbital optimization method is presented for density functional calculations of excited electronic states using either a real space grid or a plane wave basis set. The method is variational, provides atomic forces in the excited…

Computational Physics · Physics 2022-11-09 Aleksei V. Ivanov , Gianluca Levi , Elvar Ö. Jónsson , Hannes Jónsson

We present a reformulation of QM/MM as a fully quantum mechanical theory of interacting subsystems, all treated at the level of density functional theory (DFT). For the MM subsystem, which lacks orbitals, we assign an ad hoc electron…

Ab initio molecular dynamics (AIMD) simulations employing density functional theory (DFT) and plane waves are routinely carried out using density functionals at the level of Generalized Gradient Approximation (GGA). AIMD simulations…

Chemical Physics · Physics 2020-03-04 Sagarmoy Mandal , Nisanth N. Nair

Recently, Tao and Mo (TM) derived a meta-generalized gradient approximation functional based on a model exchange-correlation hole. In this work, the performance of this functional is assessed on standard test sets, using the…

Chemical Physics · Physics 2017-01-04 Yuxiang Mo , Guocai Tian , Roberto Car , Viktor N. Staroverov , Gustavo E. Scuseria , Jianmin Tao

We introduce a non-equilibrium density-functional theory of local temperature and associated local energy density that is suited for the study of thermoelectric phenomena. The theory rests on a local temperature field coupled to the…

Strongly Correlated Electrons · Physics 2014-05-16 F. G. Eich , M. Di Ventra , G. Vignale

Kohn-Sham density functional theory (DFT) is nowadays widely used for electronic structure theory simulations, and the accuracy and efficiency of DFT rely on approximations of the exchange-correlation functional. By inclusion of the kinetic…

Materials Science · Physics 2023-06-01 Renxi Liu , Daye Zheng , Xinyuan Liang , Xinguo Ren , Mohan Chen , Wenfei Li

The formation and migration energies for various point defects, including vacancies and self-interstitials in aluminum are reinvestigated systematically using the supercell approximation in the framework of orbital-free density functional…

Materials Science · Physics 2020-01-14 Ruizhi Qiu , Haiyan Lu , Bingyun Ao , Li Huang , Tao Tang , Piheng Chen

Warm dense matter (WDM) has emerged as one of the frontiers of both experimental and theoretical physics and is challenging traditional concepts of plasma, atomic, and condensed-matter physics. While it has become common practice to model…

Plasma Physics · Physics 2021-10-01 Zhandos Moldabekov , Tobias Dornheim , Maximilian Böhme , Jan Vorberger , Attila Cangi

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

Molecular Density Functional Theory (MDFT) offers an efficient implicit- solvent method to estimate molecule solvation free-energies whereas conserving a fully molecular representation of the solvent. Even within a second order ap-…

Soft Condensed Matter · Physics 2014-06-12 Volodymyr P. Sergiievskyi , Guillaume Jeanmairet , Maximilien Levesque , Daniel Borgis

We introduce a class of interatomic potential models that can be automatically generated from data consisting of the energies and forces experienced by atoms, derived from quantum mechanical calculations. The resulting model does not have a…

Computational Physics · Physics 2015-05-14 Albert P. Bartók , Mike C. Payne , Risi Kondor , Gábor Csányi

We introduce an energy functional for ground-state electronic structure calculations. Its variables are the natural spin-orbitals of singlet many-body wave functions and their joint occupation probabilities deriving from controlled…

Chemical Physics · Physics 2016-12-04 Ralph Gebauer , Morrel H. Cohen , Roberto Car

Density functional calculations on atoms are often used for determining accurate initial guesses as well as generating various types of pseudopotential approximations and efficient atomic-orbital basis sets for polyatomic calculations. To…

Computational Physics · Physics 2023-10-30 Susi Lehtola

We analyze the methodology and the performance of subsystem density functional theory (DFT) with meta-generalized gradient approximation (meta-GGA) exchange-correlation functionals for non-bonded systems. Meta-GGA functionals depend on the…

Other Condensed Matter · Physics 2015-05-05 S. Śmiga , E. Fabiano , S. Laricchia , L. A. Constantin , F. Della Sala

Aspects of Density Functional Resonance Theory (DFRT) [Phys. Rev. Lett. \textbf{107}, 163002 (2011)], a recently developed complex-scaled version of ground-state Density Functional Theory (DFT), are studied in detail. The asymptotic…

Quantum Physics · Physics 2015-06-04 Daniel L. Whitenack , Adam Wasserman