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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

Density-functional theory (DFT) has revolutionized computer simulations in chemistry and material science. A faithful implementation of the theory requires self-consistent calculations. However, this effort involves repeatedly diagonalizing…

Quantum Physics · Physics 2023-07-17 Taehee Ko , Xiantao Li , Chunhao Wang

Density functional theory (DFT) has emerged as one of the most versatile and lucrative approaches in electronic structure calculations of many-electron systems in past four decades. Here we give an account of the development of a…

Chemical Physics · Physics 2019-04-19 Abhisek Ghosal , Amlan K. Roy

Density Functional Theory (DFT) has become the quasi-standard for ab-initio simulations for a wide range of applications. While the intrinsic cubic scaling of DFT was for a long time limiting the accessible system size to some hundred…

Materials Science · Physics 2018-02-23 Stephan Mohr , Marc Eixarch , Maximilian Amsler , Mervi J. Mantsinen , Luigi Genovese

We propose a local real-space formulation for orbital-free DFT with density dependent kinetic energy functionals and a unified variational framework for computing the configurational forces associated with geometry optimization of both…

Materials Science · Physics 2015-06-15 Sambit Das , Mrinal Iyer , Vikram Gavini

Local density approximation (LDA) to the density functional theory (DFT) has continuous derivative of total energy as a number of electrons function and continuous exchange-correlation potential, while in exact DFT both should be…

Strongly Correlated Electrons · Physics 2010-06-28 V. I. Anisimov , A. V. Kozhevnikov , M. A. Korotin , A. V. Lukoyanov , D. A. Khafizullin

Density functional theory (DFT), the most widely adopted method in modern computational chemistry, fails to describe accurately the electronic structure of strongly correlated systems. Here we show that DFT can be formally and practically…

Chemical Physics · Physics 2022-04-18 Daniel Gibney , Jan-Niklas Boyn , David A. Mazziotti

We showcase the advantages of orbital-free density-potential functional theory (DPFT), a more flexible variant of Hohenberg-Kohn density functional theory. DPFT resolves the usual trouble with the gradient-expanded kinetic energy functional…

Quantum Gases · Physics 2021-06-16 Martin-Isbjörn Trappe , Jun Hao Hue , Berthold-Georg Englert

Density functional theory (DFT) is routinely employed in material science and in quantum chemistry to simulate weakly correlated electronic systems. Recently, deep learning (DL) techniques have been adopted to develop promising functionals…

Strongly Correlated Electrons · Physics 2023-10-02 Emanuele Costa , Rosario Fazio , Sebastiano Pilati

We introduce a practical hybrid approach that combines orbital-free density functional theory (DFT) with Kohn-Sham DFT for speeding up first-principles molecular dynamics simulations. Equilibrated ionic configurations are generated using…

It is believed that the density functional theory (DFT) describes most elements with s, p and d orbitals very well, except some materials that having strongly localized and correlated valence electrons. In this work, we find that the widely…

Materials Science · Physics 2020-03-17 Y. X. Wang , Hua Y. Geng , Q. Wu , Xiang R. Chen

Orbital-free density functional theory (OF-DFT) runs at low computational cost that scales linearly with the number of simulated atoms, making it suitable for large-scale material simulations. It is generally considered that OF-DFT strictly…

Materials Science · Physics 2022-04-05 Qiang Xu , Cheng Ma , Wenhui Mi , Yanchao Wang , Yanming Ma

Standard density functional approximations often give questionable results for odd-electron radical complexes, with the error typically attributed to self-interaction. In density corrected density functional theory (DC-DFT), certain classes…

Chemical Physics · Physics 2015-06-19 Min-Cheol Kim , Eunji Sim , Kieron Burke

Linear-scaling implementations of density functional theory (DFT) reach their intended efficiency regime only when applied to systems having a physical size larger than the range of their Kohn-Sham density matrix (DM). This causes a problem…

Chemical Physics · Physics 2022-03-25 Marcel David Fabian , Ben Shpiro , Eran Rabani , Daniel Neuhauser , Roi Baer

Recently, an approximate theoretical framework was introduced, called local reduced density matrix functional theory (local-RDMFT), where functionals of the one-body reduced density matrix (1-RDM) are minimized under the additional…

First-principles density functional theory (DFT) codes which employ a localized basis offer advantages over those which use plane-wave bases, such as better scaling with system size and better suitability to low-dimensional systems. The…

Materials Science · Physics 2024-11-25 Daniel Bennett , Michele Pizzochero , Javier Junquera , Efthimios Kaxiras

Kohn-Sham density functional theory (DFT) has long struggled with the accurate description of strongly correlated and open shell systems and improvements have been minor even in the newest hybrid functionals. In this Letter we treat the…

Chemical Physics · Physics 2021-04-01 Danny Gibney , Jan-Niklas Boyn , David A. Mazziotti

We develop a method in which the electronic densities of small fragments determined by Kohn-Sham density functional theory (DFT) are embedded using stochastic DFT to form the exact density of the full system. The new method preserves the…

Chemical Physics · Physics 2015-06-19 Daniel Neuhauser , Roi Baer , Eran Rabani

The design of better exchange-correlation functionals for Density Functional Theory (DFT) is a central challenge of modern electronic structure theory. However, current developments are limited by the mathematical form of the functional,…

Chemical Physics · Physics 2024-08-19 Kyle Bystrom , Boris Kozinsky

Recently, we introduced (e-print arXiv:1407.7128) {\em local reduced density matrix functional theory} (local RDMFT), a theoretical scheme capable of incorporating static correlation effects in Kohn-Sham equations. Here, we apply local…

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