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Efficient hybrid DFT simulations of solid state materials would be extremely beneficial for computational chemistry and materials science, but is presently bottlenecked by difficulties in computing Hartree-Fock (HF) exchange with plane wave…

Chemical Physics · Physics 2024-10-30 Yuanheng Wang , Diptarka Hait , Pablo A. Unzueta , Juncheng Harry Zhang , Todd J. Martínez

In the near future, material and drug design may be aided by quantum computer assisted simulations. These have the potential to target chemical systems intractable by the most powerful classical computers. However, the resources offered by…

Delocalization errors, such as charge-transfer and some self-interaction errors, plague computationally-efficient and otherwise-accurate density functional approximations (DFAs). Evaluating a semi-local DFA non-self-consistently on the…

Chemical Physics · Physics 2023-01-02 Aaron D. Kaplan , Chandra Shahi , Pradeep Bhetwal , Raj K. Sah , John P. Perdew

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

The evaluation of exact (Hartree--Fock, HF) exchange operator is a crucial ingredient for the accurate description of electronic structure in periodic systems through ab initio and hybrid density functional approaches. An efficient…

Chemical Physics · Physics 2020-10-28 Xiao Wang , Cannada A. Lewis , Edward F. Valeev

We present an efficient and accurate implementation of hybrid exchange-correlation (XC) functionals in the SIESTA code, enabling large-scale simulations based on Hartree-Fock-type exact exchange combined with strictly localized numerical…

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

A new method for implementing the kinetic energy operator for real-space, grid-based electronic structure codes is developed. It is based on multi-order Adaptive Finite Differencing (AFD) and uses atomic pseudo orbitals produced by the…

Computational Physics · Physics 2023-05-23 E. L. Briggs , Wenchang Lu , J. Bernholc

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

We introduce the semiclassical limit to electronic systems by taking the limit $\hbar\rightarrow 0$ in the solution of Schr\"odinger equations. We show that this limit is closely related to one type of strong correlation that is…

Computational Physics · Physics 2025-01-07 Yunzhi Li , Chen Li

We present an accurate, efficient and massively parallel finite-element code, DFT-FE, for large-scale ab-initio calculations (reaching $\sim 100,000$ electrons) using Kohn-Sham density functional theory (DFT). DFT-FE is based on a local…

Computational Physics · Physics 2020-01-08 Phani Motamarri , Sambit Das , Shiva Rudraraju , Krishnendu Ghosh , Denis Davydov , Vikram Gavini

A new, very fast, implementation of the exact (Fock) exchange operator for electronic structure calculations within the plane-wave pseudopotential method is described in detail for both molecular and periodic systems, and carefully…

Materials Science · Physics 2018-12-12 Ivan Carnimeo , Stefano Baroni , Paolo Giannozzi

We propose a new molecular simulation framework that combines the transferability, robustness and chemical flexibility of an ab initio method with the accuracy and efficiency of a machine learned force field. The key to achieve this mix is…

Computational Physics · Physics 2020-01-08 Sebastian Dick , Marivi Fernandez-Serra

The real-space density-functional perturbation theory (DFPT) for the computations of the response properties with respect to the atomic displacement and homogeneous electric field perturbation has been recently developed and implemented…

Computational Physics · Physics 2020-10-28 Honghui Shang , Wanzhen Liang , Yunquan Zhang , Jinlong Yang

Recent advances in continuum embedding models have enabled the incorporation of solvent and electrolyte effects into density functional theory (DFT) simulations of material surfaces, significantly benefiting electrochemistry, catalysis, and…

Computational Physics · Physics 2025-10-10 Jakob Filser , Edan Bainglass , Karsten Reuter , Oliviero Andreussi

Computational studies of electrochemical interfaces based on density-functional theory (DFT) play an increasingly important role in present research on electrochemical processes for energy conversion and storage. The homogeneous background…

Materials Science · Physics 2022-04-26 Arthur Hagopian , Marie-Liesse Doublet , Jean-Sébastien Filhol , Tobias Binninger

We implement and benchmark the frozen core approximation, a technique commonly adopted in electronic structure theory to reduce the computational cost by means of mathematically fixing the chemically inactive core electron states. The…

Materials Science · Physics 2021-06-14 Victor Wen-zhe Yu , Jonathan Moussa , Volker Blum

A two-parameter extension of the density-scaled double hybrid approach of Sharkas et al. [J. Chem. Phys. 134, 064113 (2011)] is presented. It is based on the explicit treatment of a fraction of multideterminantal exact exchange. The…

Chemical Physics · Physics 2012-01-12 Emmanuel Fromager

(Screened) hybrid functionals are being used more and more for solid-state calculations. Usually the fraction alpha of Hartree-Fock exchange is kept fixed during the calculation, however there is no single (universal) value for alpha which…

Materials Science · Physics 2013-10-17 David Koller , Peter Blaha , Fabien Tran

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