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The accurate calculation of electronic potential energy surfaces for ground and excited states is crucial for understanding photochemical processes, particularly near conical intersections. While classical methods are limited by scaling and…

Quantum Physics · Physics 2025-09-18 Tomáš Bezděk

We present a new first-principles formalism for calculating forces for optically excited electronic states using the interacting Green's function approach with the GW-Bethe Salpeter Equation method. This advance allows for efficient…

Materials Science · Physics 2013-05-29 Sohrab Ismail-Beigi Steven G. Louie

A detailed exploration of the $f$-atomic orbital occupancy space for UO$_2$ is performed using a first principles approach based on density functional theory (DFT), employing a full hybrid functional within a systematic basis set.…

Strongly Correlated Electrons · Physics 2022-01-05 Laura E. Ratcliff , Luigi Genovese , Hyowon Park , Peter B. Littlewood , Alejandro Lopez-Bezanilla

We present an alternative to the Kohn-Sham formulation of density functional theory for the ground-state properties of strongly interacting electronic systems. The idea is to start from the limit of zero kinetic energy and systematically…

Strongly Correlated Electrons · Physics 2015-05-13 Paola Gori-Giorgi , Michael Seidl , G. Vignale

Given a set of Kohn-Sham orbitals from an insulating system, we present a simple, robust, efficient and highly parallelizable method to construct a set of, optionally orthogonal, localized basis functions for the associated subspace. Our…

Computational Physics · Physics 2014-11-05 Anil Damle , Lin Lin , Lexing Ying

We resolve a fundamental issue associated with the conventional Kohn-Sham formulation of real-time time-dependent density functional theory. We show that unphysical multielectron excitations, generated during time propagation of the…

Computational Physics · Physics 2020-01-16 Xiaoning Zang , Udo Schwingenschlogl , Mark T. Lusk

We present an efficient post-processing method for calculating the electronic structure of nanosystems based on the divide-and-conquer approach to density functional theory (DC-DFT), in which a system is divided into subsystems whose…

Materials Science · Physics 2017-01-06 Shunsuke Yamada , Fuyuki Shimojo , Ryosuke Akashi , Shinji Tsuneyuki

The exact formulation of multi-configuration density-functional theory (DFT) is discussed in this work. As an alternative to range-separated methods, where electron correlation effects are split in the coordinate space, the combination of…

Chemical Physics · Physics 2015-02-26 Emmanuel Fromager

A model is developed, based on the density functional perturbation theory and the inverse Kohn-Sham method, that can be used to improve relativistic nuclear energy density functionals towards an exact but unknown Kohn-Sham…

Nuclear Theory · Physics 2021-04-28 Giacomo Accorto , Tomoya Naito , Haozhao Liang , Tamara Niksic , Dario Vretenar

We report on a methodology for the treatment of the Coulomb energy and potential in Kohn-Sham density functional theory that is free from self-interaction effects. Specifically, we determine the Coulomb potential given as the functional…

Materials Science · Physics 2016-06-29 M. Däne , A. Gonis , D. M. Nicholson , G. M. Stocks

Orbital-free density functional theory promises to deliver linear-scaling electronic structure calculations. This requires the knowledge of the non-interacting kinetic-energy density functional (KEDF), which should be accurate and must…

Materials Science · Physics 2024-12-12 Michael A. J. Mitchell , Teresa Del Aguila Ferrandis , Stefano Sanvito

A recently developed density functional method, within Hohenberg-Kohn-Sham framework, is used for faithful description of atoms, molecules in Cartesian coordinate grid, by using an LCAO-MO ansatz. Classical Coulomb potential is obtained by…

Chemical Physics · Physics 2013-07-16 Amlan K. Roy

A recent work [arXiv:2401.04685] has merged $N$-centered ensembles of neutral and charged electronic ground states with ensembles of neutral ground and excited states, thus providing a general and in-principle exact (so-called extended…

Strongly Correlated Electrons · Physics 2024-05-14 Filip Cernatic , Emmanuel Fromager

Charge-transfer excited states are highly relevant for applications in molecular electronics. However, the accurate calculation of these states in large systems is challenging since wave function methods are prohibitively expensive,…

Chemical Physics · Physics 2025-05-20 Nicola Bogo , Zeyi Zhang , Martin Head-Gordon , Christopher J. Stein

We combine recent advances in excited state variational principles, fast multi-Slater Jastrow methods, and selective configuration interaction to create multi-Slater Jastrow wave function approximations that are optimized for individual…

Strongly Correlated Electrons · Physics 2019-06-19 Sergio D. Pineda Flores , Eric Neuscamman

The simulation of molecular electronic structure is an important application of quantum devices. Recently, it has been shown that quantum devices can be effectively combined with classical supercomputing centers in the context of the…

Quantum Physics · Physics 2025-02-28 Stefano Barison , Javier Robledo Moreno , Mario Motta

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

An axiomatic approach is herein used to determine the physically acceptable forms for general $D$-dimensional kinetic energy density functionals (KEDF). The resulted expansion captures most of the known forms of one-point KEDFs. By…

Chemical Physics · Physics 2017-06-08 Sabre Kais , Fahhad H Alharbi

The self consistent version of the density functional theory is presented, which allows to calculate the ground state and dynamic properties of finite multi-electron systems. An exact functional equation for the effective interaction, from…

Materials Science · Physics 2017-08-23 M. Ya. Amusia , A. Z. Msezane , V. R. Shaginyan

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