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We introduce an energy functional for ground-state electronic structure calculations. Its variables are the natural spin-orbitals of singlet many-body wave functions and their joint occupation probabilities deriving from controlled…

Chemical Physics · Physics 2016-12-04 Ralph Gebauer , Morrel H. Cohen , Roberto Car

The $\Delta$NO two-electron density matrix (2-RDM) and energy expression are derived from a multideterminantal wave function. The approximate $\Delta$NO 2-RDM is combined with an on-top density functional and a double-counting correction to…

Chemical Physics · Physics 2022-03-14 Ismael A. Elayan , Rishabh Gupta , Joshua W. Hollett

We extend the previously proposed one-parameter double-hybrid density-functional theory [K. Sharkas, J. Toulouse, and A. Savin, J. Chem. Phys. 134, 064113 (2011)] to meta-generalized-gradient-approximation (meta-GGA) exchange-correlation…

Chemical Physics · Physics 2014-02-27 Sidi Ould Souvi , Kamal Sharkas , Julien Toulouse

Semilocal exchange-correlation functionals are the most accurate, realistic and widely used ones to describe the complex many-electron effects of two-dimensional quantum systems. Beyond local density approximation, the generalized gradient…

Materials Science · Physics 2017-04-12 Subrata Jana , Prasanjit samal

In modeling low-dimensional electronic nanostructures, the evaluation of the electron-electron interaction is a challenging task. Here we present an accurate and practical density-functional approach to the two-dimensional many-electron…

Strongly Correlated Electrons · Physics 2010-10-29 S. Pittalis , E. Rasanen

We have compared the performance of Grimme style DH/DSD and Zhang-Xu-Goddard type xDH/xDSD forms for double hybrids. In the DH and DSD forms, KS orbitals with elevated HF exchange and damped DFT correlation are used, while in the xDH and…

Chemical Physics · Physics 2015-11-12 Manoj Kumar Kesharwani , Sebastian Kozuch , Jan M. L. Martin

Long-range corrected (LC) hybrid functionals and asymptotically corrected (AC) model potentials are two distinct density functional methods with correct asymptotic behavior. They are known to be accurate for properties that are sensitive to…

Chemical Physics · Physics 2017-09-13 Chen-Wei Tsai , Yu-Chuan Su , Guan-De Li , Jeng-Da Chai

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…

Density functional theory has been an essential analysis tool for both theoretical and experimental chemists since accurate hybrid functionals were developed. Here we propose a local hybrid method derived from the optimized effective…

Chemical Physics · Physics 2017-03-24 Jaewook Kim , Kwangwoo Hong , Sang-Yeon Hwang , Seongok Ryu , Sunghwan Choi , Woo Youn Kim

A framework for developing new approximate electronic structure methods is presented, in which the correlation energy of a many-electron system in the ground state is computed as in the single-reference second-order many-body perturbation…

Chemical Physics · Physics 2011-06-15 Dimitri Laikov

Density functionals with a range-separated treatment of the exchange energy are known to improve upon their semilocal forerunners and fixed-fraction hybrids. The conversion of a given semilocal functional into its short-range analog is not…

Chemical Physics · Physics 2019-09-09 Dimitri N. Laikov

The original formulation (Phys. Rev. Lett. 119, 063002, 2017) of the natural orbital functional - second-order M{\o}ller-Plesset (NOF-MP2) method is based on the MP2 that uses the canonical Hartree-Fock molecular orbitals. The current work…

Chemical Physics · Physics 2018-08-22 Mario Piris

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 present an accurate and efficient framework for real-space Hubbard-corrected density functional theory. In particular, we obtain expressions for the energy, atomic forces, and stress tensor suitable for real-space finite-difference…

Computational Physics · Physics 2025-10-20 Sayan Bhowmik , Andrew J. Medford , Phanish Suryanarayana

By reverse-engineering from exact solutions we obtain Hartree-exchange-correlation (Hxc) potentials for a double quantum dot subject to generic density-density interactions and Hund's rule coupling. We find ubiquitous step structures of the…

Mesoscale and Nanoscale Physics · Physics 2020-08-10 Nahual Sobrino , Stefan Kurth , David Jacob

We consider density functionals for exchange and correlation energies in two-dimensional systems. The functionals are constructed by making use of exact constraints for the angular averages of the corresponding exchange and correlation…

Strongly Correlated Electrons · Physics 2010-02-25 E. Rasanen , S. Pittalis

Hybrid density functional approximations (DFAs) offer compelling accuracy for ab initio electronic-structure simulations of molecules, nanosystems, and bulk materials, addressing some deficiencies of computationally cheaper, frequently used…

Double hybrid (DH) density functionals are amongst the most accurate density functional approximations developed so far, largely due to incorporation of correlation effects from unoccupied orbitals via second order perturbation theory…

Chemical Physics · Physics 2018-05-07 Diptarka Hait , Martin Head-Gordon

The variational determination of the two-particle density matrix is an interesting, but not yet fully explored technique that allows to obtain ground-state properties of a quantum many-body system without reference to an $N$-particle wave…

Strongly Correlated Electrons · Physics 2012-05-22 Brecht Verstichel , Helen van Aggelen , Ward Poelmans , Dimitri Van Neck

Semi-local density functionals for the exchange-correlation energy of electrons are extensively used as it produce realistic and accurate results for finite and extended systems. The choice of techniques play crucial role in constructing…

Materials Science · Physics 2017-11-01 Subrata Jana , Prasanjit Samal