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This work presents the formalism and implementation of excited state nuclear forces within density functional linear response theory (TDDFT) using a plane wave basis set. An implicit differentiation technique is developed for computing…

Other Condensed Matter · Physics 2009-11-11 Nikos L. Doltsinis , D. S. Kosov

We use projector operators to correct the Kohn-Sham Hamiltonian of density functional theory (KS-DFT) so that the resulting mean-field scheme yields, in finite systems, virtual orbitals and energy gaps in better agreement with those…

Other Condensed Matter · Physics 2008-06-26 Hector Mera

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

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

Exchange interactions are a manifestation of the quantum mechanical nature of the electrons and play a key role in predicting the properties of materials from first principles. In density functional theory (DFT), a widely used approximation…

Materials Science · Physics 2020-03-27 Marco Bernardi

Accurate treatment of amide resonance is important in electronic structure calculation of protein, for Resonance-Assisted Hydrogen Bonding in the hydrogen bonded chains of backbone amides of protein secondary structures such as beta sheets…

Chemical Physics · Physics 2016-10-03 John N. Sharley

Self-interaction is a fundamental flaw of practical Kohn-Sham Density Functional Theory (KS DFT) approximations responsible for numerous qualitative and even catastrophic shortcomings. Whereas self-interaction is easy to characterize in…

Chemical Physics · Physics 2024-07-16 Samuel A. Slattery , Edward F. Valeev

Orbital-free density functional theory (OF-DFT) constitutes a computationally highly effective tool for modeling electronic structures of systems ranging from room-temperature materials to warm dense matter. Its accuracy critically depends…

We derive an exact representation of the exchange-correlation energy within density functional theory (DFT) which spawns a class of approximations leading to correct long-range asymptotic behavior. In what amounts to be the simplest…

Materials Science · Physics 2009-11-10 Roi Baer , Daniel Neuhauser

The accurate resolution of the chemical properties of strongly correlated systems, such as biradicals, requires the use of electronic structure theories that account for both multi-reference as well as dynamic correlation effects. A variety…

Chemical Physics · Physics 2023-01-03 Jan-Niklas Boyn , David A. Mazziotti

State-specific orbital optimized approaches are more accurate at predicting core-level spectra than traditional linear-response protocols, but their utility had been restricted on account of the risk of `variational collapse' down to the…

This work presents an alternative, general, and in-principle exact extension of electronic Kohn-Sham density functional theory (KS-DFT) to the fully quantum-mechanical molecular problem. Unlike in existing multi-component or…

Chemical Physics · Physics 2024-05-14 Emmanuel Fromager , Benjamin Lasorne

Accurate charge densities are essential for reliable electronic structure calculations because they significantly impact predictions of various chemical properties and in particular, according to the Hellmann-Feynman theorem, atomic forces.…

Chemical Physics · Physics 2025-03-12 Moritz Gubler , Moritz R. Schäfer , Jörg Behler , Stefan Goedecker

We present an orbital-resolved extension of the Hubbard $U$ correction to density-functional theory (DFT). Compared to the conventional shell-averaged approach, the prediction of energetic, electronic and structural properties is strongly…

Materials Science · Physics 2024-09-18 Eric Macke , Iurii Timrov , Nicola Marzari , Lucio Colombi Ciacchi

We decompose the energy error of any variational DFT calculation into a contribution due to the approximate functional and that due to the approximate density. Typically, the functional error dominates, but in many interesting situations,…

Chemical Physics · Physics 2015-06-12 Min-Cheol Kim , Eunji Sim , Kieron Burke

Density functional theory (DFT) is the most promising method for calculating quantum properties of molecules and materials at moderate and large scales. However, commonly used density functional approximations (DFAs) have systematic…

Chemical Physics · Physics 2026-03-24 Yichen Fan , Jacob Z. Williams , Weitao Yang

We introduce surrogate functionals: machine-learned energy functionals for orbital-free density functional theory (OF-DFT) which are defined not by universal fidelity to a physical reference, but merely by the requirement that density…

Machine Learning · Computer Science 2026-04-23 Roman Remme , Fred A. Hamprecht

We have performed {\it ab initio} calculations for a series of energetic solids to explore their structural and electronic properties. To evaluate the ground state volume of these molecular solids, different dispersion correction methods…

Materials Science · Physics 2015-09-29 S. Appalakondaiah , G. Vaitheeswaran , S. Lebègue

A method is presented, which employs the density matrix renormalization group technique in order to construct exact ground state exchange correlation functionals for models of correlated electron systems coupled to external reservoirs. The…

Mesoscale and Nanoscale Physics · Physics 2009-11-13 Peter Schmitteckert , Ferdinand Evers

We investigate configuration-interaction (CI) calculations on a basis of molecular orbitals generated by preliminary density-functional theory (DFT) calculations. We use this CI/DFT framework to improve the modeling of core-excited states…

Chemical Physics · Physics 2025-09-11 Giorgio Visentin , Francois Mauger