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A self-consistent calculation scheme for correlated electron systems is created based on the density-functional theory (DFT). Our scheme is a multi-reference DFT (MR-DFT) calculation in which the electron charge density is reproduced by an…

Strongly Correlated Electrons · Physics 2009-11-13 Koichi Kusakabe , Naoshi Suzuki , Shusuke Yamanaka , Kizashi Yamaguchi

The finite basis optimized effective potential (OEP) method within density functional theory is examined as an ill-posed problem. It is shown that the generation of nonphysical potentials is a controllable manifestation of the use of…

Materials Science · Physics 2009-11-11 Tim Heaton-Burgess , Felipe A. Bulat , Weitao Yang

An explicitly orbital-dependent correlation energy functional is proposed, which is to be used in combination with the orbital-dependent exchange energy functional in energy-band calculations. It bears a close resemblance to the…

Strongly Correlated Electrons · Physics 2009-11-10 Masahiko Higuchi , Hiroshi Yasuhara

We introduce affordable computational strategies for calculating orbital and pair-orbital energies in atomic and molecular systems. Our methods are based on the pair Coupled Cluster Doubles (pCCD) ansatz and its orbital-optimized variant.…

Chemical Physics · Physics 2025-02-06 Seyedehdelaram Jahani , Somayeh Ahmadkhani , Katharina Boguslawski , Paweł Tecmer

The general procedure underlying Hartree-Fock and Kohn-Sham density functional theory calculations consists in optimizing orbitals for a self-consistent solution of the Roothaan-Hall equations in an iterative process. It is often ignored…

Chemical Physics · Physics 2017-03-16 Alain C. Vaucher , Markus Reiher

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 double ionization potential (DIP) equation-of-motion (EOM) coupled-cluster (CC) method with a full treatment of 4-hole-2-particle (4$h$-2$p$) correlations and triply excited clusters, abbreviated as DIP-EOMCCSDT(4$h$-2$p$), and its…

Chemical Physics · Physics 2025-02-12 Karthik Gururangan , Achintya Kumar Dutta , Piotr Piecuch

Construction of hybrid atomic orbitals is proposed as the approximate common eigen states of finite first moment matrices. Their hybridization and orientation can be a-priori tunned as per their anticipated neighbourhood. Their Wannier…

Materials Science · Physics 2021-09-15 Manoar Hossain , Joydev De , Joydeep Bhattacharjee

We propose a multiconfigurational hybrid density-functional theory which rigorously combines a multiconfiguration self-consistent-field calculation with a density-functional approximation based on a linear decomposition of the…

Chemical Physics · Physics 2012-08-20 Kamal Sharkas , Andreas Savin , Hans Jørgen Aa. Jensen , Julien Toulouse

Polymer self-consistent field theory techniques are used to derive quantum density functional theory without the use of the theorems of density functional theory. Instead, a free energy is obtained from a partition function that is…

Chemical Physics · Physics 2022-11-29 Russell B. Thompson

In the density functional (DF) theory of Kohn and Sham, the kinetic energy of the ground state of a system of noninteracting electrons in a general external field is calculated using a set of orbitals. Orbital free methods attempt to…

Strongly Correlated Electrons · Physics 2009-11-13 Jeng-Da Chai , John D Weeks

Quantum mechanical calculations of core electron binding energies (CEBEs) leading to 2p hole states are relevant to interpreting L-edge x-ray photo-electron spectroscopy (XPS), as well as higher edges. Orbital-optimized density functional…

Chemical Physics · Physics 2025-07-31 Richard Kang , Leonardo A. Cunha , Diptarka Hait , Martin Head-Gordon

Local density approximation (LDA) to the density functional theory (DFT) has continuous derivative of total energy as a number of electrons function and continuous exchange-correlation potential, while in exact DFT both should be…

Strongly Correlated Electrons · Physics 2010-06-28 V. I. Anisimov , A. V. Kozhevnikov , M. A. Korotin , A. V. Lukoyanov , D. A. Khafizullin

This work presents a new class of hybrid density functional theory (DFT) approximations, incorporating nonlocal exact exchange in predefined states such as core atomic orbitals (AOs). These projected hybrid density functionals are a…

Chemical Physics · Physics 2023-05-16 Benjamin G. Janesko

We apply the optimized effective potential method (OPM) to the multiplet energies of the 3d$^n$ transition metal atoms, where the orbital dependence of the energy functional with respect to orbital wave function is the single-configuration…

Atomic Physics · Physics 2009-11-10 N. Hamamoto , C. Satoko

We study static correlation and delocalisation errors and show that even methods with good energies can yield significant delocalization errors that affect the density, leading to large errors in predicting {\em e.g.} dipole moments. We…

Chemical Physics · Physics 2020-06-01 Maria Hellgren , Tim Gould

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

The exchange-correlation energy in Kohn-Sham density functional theory is expressed as a functional of the electronic density and the Kohn-Sham orbitals. An alternative to Kohn-Sham theory is to express the energy as a functional of the…

Computational Physics · Physics 2009-10-31 S. Goedecker , C. Umrigar

Motivated by various benefits of multi-energy integration, this paper establishes a bi-level framework based on transactive control to realize energy optimization among multiple interconnected energy hubs (EHs). A storage-energy-equivalent…

Optimization and Control · Mathematics 2019-02-05 Yizhi Cheng , Peichao Zhang

Orbital-free density functional theory as an extension of traditional Thomas-Fermi theory has attracted a lot of interest in the past decade because of developments in both more accurate kinetic energy functionals and highly efficient…

Materials Science · Physics 2009-11-10 Hong Jiang , Weitao Yang