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We present a graphical analysis of the adiabatic connections underlying double-hybrid density-functional methods that employ second-order perturbation theory. Approximate adiabatic connection formulae relevant to the construction of these…

Chemical Physics · Physics 2013-06-26 Yann Cornaton , Odile Franck , Andrew M. Teale , Emmanuel Fromager

In contrast to the original Kohn-Sham (KS) formalism, we propose a density functional theory (DFT) with fractional orbital occupations for the study of ground states of many-electron systems, wherein strong static correlation is shown to be…

Chemical Physics · Physics 2015-06-03 Jeng-Da Chai

Time-dependent orbital-free density functional theory (TD-OFDFT) is an efficient ab-initio method for calculating the electronic dynamics of large systems. In comparison to standard TD-DFT, it computes only a single electronic state…

Chemical Physics · Physics 2021-12-15 Kaili Jiang , Xuecheng Shao , Michele Pavanello

Orbital-free density functional theory (OF-DFT) provides an alternative approach for calculating the molecular electronic energy, relying solely on the electron density. In OF-DFT, both the ground-state density is optimized variationally to…

Chemical Physics · Physics 2023-11-23 Alexandre de Camargo , Ricky T. Q. Chen , Rodrigo A. Vargas-Hernández

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

Linear-response time-dependent (TD) density-functional theory (DFT) has been implemented in the pseudopotential wavelet-based electronic structure program BigDFT and results are compared against those obtained with the all-electron…

We present a new efficient way to perform hybrid density functional theory (DFT) based electronic structure calculation. The new method uses an interpolative separable density fitting (ISDF) procedure to construct a set of numerical…

Computational Physics · Physics 2017-07-31 Wei Hu , Lin Lin , Chao Yang

In density functional theory (DFT), the exchange-correlation functional can be exactly expressed by the adiabatic connection integral. It has been noticed that as lambda goes to infinity, the lambda^(-1) term in the expansion of W(lambda)…

Other Condensed Matter · Physics 2015-05-13 Zhenfei Liu , Kieron Burke

The superadiabatic dynamical density functional theory (superadiabatic-DDFT) is a promising new method for the study of colloidal systems out-of-equilibrium. Within this approach the viscous forces arising from interparticle interactions…

Soft Condensed Matter · Physics 2024-06-10 S. M. Tschopp , J. M. Brader

Million-atom quantum simulations are in principle feasible with Orbital-Free Density Functional Theory (OF-DFT) because the algorithms only require simple functional minimizations with respect to the electron density function. In this…

Materials Science · Physics 2019-07-17 Wenhui Mi , Michele Pavanello

We develop and test a method that integrates many-electron weak-field asymptotic theory (ME-WFAT) [Phys. Rev. A 89, 013421 (2014)] in the integral representation (IR) into the density functional theory (DFT) framework. In particular, we…

Density functional theory (DFT), the most widely adopted method in modern computational chemistry, fails to describe accurately the electronic structure of strongly correlated systems. Here we show that DFT can be formally and practically…

Chemical Physics · Physics 2022-04-18 Daniel Gibney , Jan-Niklas Boyn , David A. Mazziotti

We investigate the adiabatic approximation to the exact-exchange kernel for calculating correlation energies within the adiabatic-connection fluctuation-dissipation framework of time-dependent density functional theory. A numerical study is…

Chemical Physics · Physics 2023-05-12 Maria Hellgren , Lucas Baguet

We extend to strongly correlated molecular systems the recently introduced basis-set incompleteness correction based on density-functional theory (DFT) [E. Giner et al., J. Chem. Phys. 149, 194301 (2018)]. This basis-set correction relies…

Chemical Physics · Physics 2020-05-20 Emmanuel Giner , Anthony Scemama , Pierre-François Loos , Julien Toulouse

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

Strong correlation can be essentially captured with multireference wavefunction methods such as complete active space self-consistent field (CASSCF) or density matrix renormalization group (DMRG). Still, an accurate description of the…

Strongly Correlated Electrons · Physics 2022-04-06 Daria Drwal , Pavel Beran , Michał Hapka , Marcin Modrzejewski , Adam Sokół , Libor Veis , Katarzyna Pernal

Density functional theory (DFT) offers a desirable balance between quantitative accuracy and computational efficiency in practical many-electron calculations. Its central component, the exchange-correlation energy functional, has been…

A decomposition of the exact exchange-correlation potential of time-dependent density functional theory into an interaction component and a kinetic component offers a new starting point for non- adiabatic approximations. The components are…

Chemical Physics · Physics 2018-11-14 Johanna I. Fuks , Lionel Lacombe , Soeren E. B. Nielsen , Neepa T. Maitra

We have combined our adaptive configuration interaction (ACI) [J.B. Schriber and F.A. Evangelista, J. Chem. Phys. 144, 161106 (2016)] with a density-fitted implementation of the second-order perturbative multireference driven similarity…

Chemical Physics · Physics 2018-08-29 Jeffrey B. Schriber , Kevin P. Hannon , Francesco A. Evangelista

We formulate a rigorous method for calculating a nonadiabatic (frequency-dependent) exchange-correlation (XC) kernel required for correct description of both equilibrium and nonequilibrium properties of strongly correlated systems within…

Strongly Correlated Electrons · Physics 2014-10-13 Volodymyr Turkowski , Talat S. Rahman