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A range-separated double-hybrid (RSDH) scheme which generalizes the usual range-separated hybrids and double hybrids is developed. This scheme consistently uses a two-parameter Coulomb-attenuating-method (CAM)-like decomposition of the…

Chemical Physics · Physics 2018-05-23 Cairedine Kalai , Julien Toulouse

Range-separated methods combining a short-range density functional with long-range random phase approximations RPAs with or without exchange response kernel are tested on rare-gas dimers and the S22 benchmark set of weakly interacting…

Chemical Physics · Physics 2014-04-10 Wuming Zhu , Julien Toulouse , Andreas Savin , János G. Angyán

We extend the range-separated double-hybrid RSH+MP2 method [J. G. Angyan et al., Phys. Rev. A 72, 012510 (2005)], combining long-range HF exchange and MP2 correlation with a short-range density functional, to a fully self-consistent version…

Chemical Physics · Physics 2019-12-24 Szymon Smiga , Ireneusz Grabowski , Mateusz Witkowski , Bastien Mussard , Julien Toulouse

We investigate the performance of the range-separated hybrid (RSH) scheme, which combines long-range Hartree-Fock (HF) and a short-range density-functional approximation (DFA), for calculating photoexcitation/photoionization spectra of the…

Chemical Physics · Physics 2019-07-24 Felipe Zapata , Eleonora Luppi , Julien Toulouse

Quantum chemistry methods exploiting density-functional approximations for short-range electron-electron interactions and second-order M{{\o}}ller-Plesset (MP2) perturbation theory for long-range electron-electron interactions have been…

Fractional-spin errors are inherent in all current approximate density functionals, including Hartree-Fock theory, and their origin has been related to strong static correlation effects. The conventional way to encode fractional-spin…

We examine fractional charge and spin errors in self-consistent Green's function theory within a second-order approximation (GF2). For GF2 it is known that the summation of diagrams resulting from the self-consistent solution of the Dyson…

Computational Physics · Physics 2016-11-15 Jordan J. Phillips , Alexei A. Kananenka , Dominika Zgid

We study linear-response time-dependent density-functional theory (DFT) based on the single-determinant range-separated hybrid (RSH) scheme, i.e. combining a long-range Hartree-Fock exchange kernel with a short-range DFT…

Chemical Physics · Physics 2015-06-15 Elisa Rebolini , Andreas Savin , Julien Toulouse

Screened range-separated hybrid (SRSH) functionals within generalized Kohn-Sham density functional theory (GKS-DFT) have been shown to restore a general $1/(r\varepsilon)$ asymptotic decay of the electrostatic interaction in dielectric…

Computational Physics · Physics 2023-06-26 Tammo van der Heide , Bálint Aradi , Ben Hourahine , Thomas Frauenheim , Thomas A. Niehaus

An alternative separation of short-range exchange and correlation energies is used in the framework of second-order range-separated density-functional perturbation theory. This alternative separation was initially proposed by Toulouse et…

Chemical Physics · Physics 2014-09-16 Yann Cornaton , Alexandrina Stoyanova , Hans Jørgen Aa. Jensen , Emmanuel Fromager

One of the most important open challenges in modern Kohn-Sham (KS) density-functional theory (DFT) is the correct treatment of fractional electron charges and spins. Approximate exchange-correlation (XC) functionals struggle to do this in a…

Chemical Physics · Physics 2015-12-24 Jonathan Nafziger , Adam Wasserman

We compare two different approaches to investigations of many-electron systems. The first is the Hartree-Fock (HF) method and the second is the Density Functional Theory (DFT). Overview of the main features and peculiar properties of the HF…

Materials Science · Physics 2009-11-07 M. Ya. Amusia , A. Z. Msezane , V. R. Shaginyan

Range-separated density-functional theory is an alternative approach to Kohn-Sham density-functional theory. The strategy of range-separated density-functional theory consists in separating the Coulomb electron-electron interaction into…

Chemical Physics · Physics 2015-02-20 Odile Franck , Bastien Mussard , Eleonora Luppi , Julien Toulouse

We develop a stochastic formulation of the optimally-tuned range-separated hybrid density functional theory which enables significant reduction of the computational effort and scaling of the non-local exchange operator at the price of…

Chemical Physics · Physics 2016-09-28 Daniel Neuhauser , Eran Rabani , Yael Cytter , Roi Baer

It is known for quite some time that approximate density functional (ADF) theories fail disastrously when describing the dis-sociative symmetric radical cations R2+. Considering this dissociation limit, previous work has shown that…

Materials Science · Physics 2016-09-28 Ester Livshits , Roi Baer

In this communication, we represent a self-consistent systematic optimization procedure for the development of optimally tuned (OT) range-separated hybrid (RSH) functionals from \emph{first principles}. This is an offshoot of our recent…

Chemical Physics · Physics 2022-05-24 Abhisek Ghosal , Amlan K. Roy

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

We construct range-separated double-hybrid schemes which combine coupled-cluster or random-phase approximations with a density functional based on a two-parameter Coulomb-attenuating-method-like decomposition of the electron-electron…

Chemical Physics · Physics 2020-01-29 Cairedine Kalai , Bastien Mussard , Julien Toulouse

We present a rigorous framework that combines single-particle Green's function theory with density functional theory based on a separation of electron-electron interactions into short-range and long-range components. Short-range…

Chemical Physics · Physics 2018-06-07 Alexei A. Kananenka , Dominika Zgid

Partial charges are a central concept in general chemistry and chemical biology, yet dozens of different computational definitions exist. In prior work [M. Cho et al., \textit{ChemPhysChem} {\bf 21}, 688-696 (2020)], we showed that these…

Chemical Physics · Physics 2024-04-05 Nisha Mehta , Jan M. L. Martin
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