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A relativistic density-functional theory based on a Fock-space effective quantum-electrodynamics (QED) Hamiltonian using the Coulomb or Coulomb-Breit two-particle interaction is developed. This effective QED theory properly includes the…

Chemical Physics · Physics 2021-05-03 Julien Toulouse

New local "hybrid" functionals proposed by V. V. Karasiev in [J. Chem. Phys. {\bf 118}, 8567 (2003)] are benchmarked against nonlocal hybrid functionals. Their performance is tested on the total and high occupied orbital energies, as well…

Chemical Physics · Physics 2012-10-26 Ivan A. Mikhailov , Olga A. Shukruto , Artem E. Masunov , Valentin V. Karasiev

Hydrogen bonding is an important non-covalent interaction that plays a major role in molecular self-organization and supramolecular structures. It can be described accurately with ab initio quantum chemical wave function methods, which…

Chemical Physics · Physics 2025-05-16 Usman Ahmed , Mikael P. Johansson , Susi Lehtola , Dage Sundholm

Empirical fitting of parameters in approximate density functionals is common. Such fits conflate errors in the self-consistent density with errors in the energy functional, but density-corrected DFT (DC-DFT) separates these two. We…

Chemical Physics · Physics 2020-12-02 Suhwan Song , Stefan Vuckovic , Eunji Sim , Kieron Burke

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

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

Following earlier work [Mehta, N.; Martin, J. M. L.; J. Chem. Theory Comput. 2022, 18, acs.jctc.2c00426] that showed how the slow basis set convergence of double hybrid density functional theory can be obviated by the use of F12 explicit…

Chemical Physics · Physics 2022-10-04 Nisha Mehta , Jan M. L. Martin

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

The positive definite Kohn-Sham kinetic energy(KS-KE) density plays crucial role in designing semilocal meta generalized gradient approximations(meta-GGAs) for low dimensional quantum systems. It has been rigorously shown that near nucleus…

Materials Science · Physics 2017-03-17 Subrata Jana , Prasanjit Samal

Coupled cluster theory with a Kohn-Sham reference (KS-CC) can dramatically outperform its Hartree-Fock counterpart for strongly correlated systems, but the origin of these improvements has remained unclear. Here we demonstrate that these…

A fundamental weakness of density functional theory (DFT) is the difficulty in making systematic improvements to approximations for the exchange and correlation functionals. In this paper, we follow a wave-function-based approach [N.I.…

Chemical Physics · Physics 2018-10-05 Timothy J. Callow , Nikitas I. Gidopoulos

We use coupled-cluster quantum chemical methods to calculate the energetics of molecular clusters cut out of periodic molecular hydrogen structures that model observed phases of solid hydrogen. The hydrogen structures are obtained from…

Materials Science · Physics 2017-03-15 J. R. Trail , P. López Ríos , R. J. Needs

Multi-center transition metal complexes (MCTMs) with magnetically interacting ions have been proposed as components for information processing devices and storage units. For any practical application of MCTMs as magnetic units, it is…

Chemical Physics · Physics 2023-04-03 Henry C. Fitzhugh , James W. Furness , Mark R. Pederson , Juan E. Peralta , Jianwei Sun

A van der Waals (vdW) density functional was implemented in the mixed basis approach previously developed for studying two dimensional systems, in which the vdW interaction plays an important role. The basis functions here are taken to be…

Computational Physics · Physics 2017-12-27 Chung-Yuan Ren , Yia-Chung Chang , Chen-Shiung Hsue

Following Hollins et al. [J. Phys.: Condens. Matter 29, 04LT01 (2017)], we invert the electronic ground state densities for various semiconducting and insulating solids calculated using several density functional approximations within the…

Chemical Physics · Physics 2025-11-05 Visagan Ravindran , Nikitas I. Gidopoulos , Stewart J. Clark

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

Density functional theory (DFT) offers an exceptional balance between accuracy and efficiency, but practical density functional approximations face an unavoidable trade-off among simplicity, accuracy, and transferability. A systematic…

Chemical Physics · Physics 2026-03-25 Jiashu Liang , Martin Head-Gordon

Kohn-Sham (KS) formalism of Density Functional Theory is modified to include the systems with strong non-dynamic electron correlation. Unlike in extended KS and broken symmetry unrestricted KS formalisms, cases of both singlet-triplet and…

Chemical Physics · Physics 2007-05-23 Artem Masunov

We formulate a set of equations that facilitate an exact numerical solution of the Kohn-Sham potential for a finite Hubbard chain with nearest neighbour hopping and arbitrary site potentials. The approach relies on a mapping of the…

Strongly Correlated Electrons · Physics 2018-10-25 Kossi Amouzouvi , Daniel Joubert

The ability of several density-functional theory (DFT) exchange-correlation functionals to describe hydrogen bonds in small water clusters (dimer to pentamer) in their global minimum energy structures is evaluated with reference to second…

Materials Science · Physics 2009-07-20 Biswajit Santra , Angelos Michaelides , Matthias Scheffler