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Fractional occupation numbers can be used in density functional theory to create a symmetric Kohn-Sham potential, resulting in orbitals with degenerate eigenvalues. We develop the corresponding perturbation theory and apply it to a system…

Materials Science · Physics 2016-09-09 Mark C. Palenik , Brett I. Dunlap

Selective configuration interaction methods approximate correlated molecular ground- and excited states by considering only the most relevant Slater determinants in the expansion. While a recently proposed neural-network-assisted approach…

We report equations of motion for the occupation numbers of natural spin orbitals and show that adiabatic extensions of common functionals employed in ground-state reduced-density-matrix-functional theory have the shortcoming of leading…

Materials Science · Physics 2012-12-27 H. Appel , E. K. U. Gross

Despite recent advances, systematic quantitative treatment of the electron correlation problem in extended systems remains a formidable task. Systematically improvable Green's function methods capable of quantitatively describing weak and…

Chemical Physics · Physics 2016-11-15 Alexander A. Rusakov , Dominika Zgid

Natural orbital functional (NOF) theory offers a promising approach for studying strongly correlated systems at an affordable computational cost, with an accuracy comparable to highly demanding wavefunction-based methods. However, its…

Strongly Correlated Electrons · Physics 2025-01-31 Juan Felipe Huan Lew-Yee , Jorge M. del Campo , Mario Piris

To explore the applicability of orbital-free density functional theory (OF-DFT) in nuclear physics, we perform a systematic benchmark of 36 one-point kinetic energy density functionals, which are originally developed for electron systems in…

Nuclear Theory · Physics 2026-05-20 Tian Shuai Shang , Jian Li , Haozhao Liang , Xinhui Wu , Cheng Ma , Wenhui Mi , Xuecheng Shao , Yanchao Wang

The current work presents a new single-reference method for capturing at the same time the static and dynamic electron correlation. The starting-point is a determinant wavefunction formed with natural orbitals obtained from a new…

Chemical Physics · Physics 2017-08-16 Mario Piris

Perdew et al. [Phys. Rev. Lett 49, 1691 (1982)] discovered and proved two different properties of exact Kohn-Sham density functional theory (DFT): (i) The exact total energy versus particle number is a series of linear segments between…

Other Condensed Matter · Physics 2015-03-13 Tamar Stein , Jochen Autschbach , Niranjan Govind , Leeor Kronik , Roi Baer

We develop a second order correction to commonly used density functional approximations (DFA) to eliminate the systematic delocalization error. The method, based on the previously developed global scaling correction (GSC), is an exact…

Chemical Physics · Physics 2021-07-22 Yuncai Mei , Zehua Chen , Weitao Yang

The nuclear-electronic orbital (NEO) method is a well-established approach for treating nuclei quantum mechanically in molecular systems beyond the usual Born-Oppenheimer approximation. In this work, we present a strategy to implement the…

Computational Physics · Physics 2022-06-29 Jianhang Xu , Ruiyi Zhou , Zhen Tao , Christopher Malbon , Volker Blum , Sharon Hammes-Schiffer , Yosuke Kanai

In this work, atomic calculations were performed within the local-density and generalized-gradient approximations of exchange and correlation density functionals within density-functional theory to provide accurate periodic trends of first…

Atomic Physics · Physics 2016-11-04 Mauro Ribeiro

Large atomic-orbital (AO) basis sets of at least triple and preferably quadruple-zeta (QZ) size are required to adequately converge Kohn-Sham density functional theory (DFT) calculations towards the complete basis set limit. However,…

Chemical Physics · Physics 2025-12-02 Anthony O. Lara , Justin J. Talbot , Zhe Wang , Martin Head-Gordon

Orbital-free Density Functional Theory (OF-DFT) has been used when studying atoms, molecules and solids. In nuclear physics, there has been basically no application of OF-DFT so far, as the Density Functional Theory (DFT) has been widely…

Nuclear Theory · Physics 2023-08-03 Gianluca Colo' , Kouichi Hagino

Incorporating nuclear shell effects within the framework of orbital-free density functional theory (DFT) has remained a longstanding challenge in nuclear physics. While the Hohenberg-Kohn theorem formally guarantees the existence of an…

Nuclear Theory · Physics 2026-03-03 Xinhui Wu , Gianluca Colò , Kouichi Hagino , Pengwei Zhao

We report the development of the theory and computer program for analytical nuclear energy gradients for (extended) multi-state complete active space perturbation theory (CASPT2) with full internal contraction. The vertical shifts are also…

Chemical Physics · Physics 2017-03-20 Bess Vlaisavljevich , Toru Shiozaki

This work presents a novel approach to distribute orbitals into subspaces within electron-pairing-based natural orbital functionals (NOFs). This approach modifies the coupling between weakly and strongly occupied orbitals by applying an…

Chemical Physics · Physics 2025-02-05 Élodie Boutou , Juan Felipe Huan Lew-Yee , Jose Maria Mercero , Mario Piris

Ab initio calculations face the challenge of describing a complex multiscale quantum many-body system. The nuclear wave function has both strong short-range correlations and long-range contributions. Natural orbitals provide a means of…

Nuclear Theory · Physics 2017-04-11 Chrysovalantis Constantinou

We propose an exact algorithm for computing the analytical gradient within the framework of the orbital-specific-virtual (OSV) second-order M{\o}ller-Plesset (MP2) theory in resolution-of-identity (RI) approximation. We implement the exact…

Chemical Physics · Physics 2019-12-17 Ruiyi Zhou , Qiujiang Liang , Jun Yang

We introduce Effective Atom Theory (EAT), a framework that transforms combinatorial materials design into a smooth, gradient-driven optimization within density functional theory (DFT). Atoms are represented as probabilistic mixtures of…

Materials Science · Physics 2025-09-10 Justin Tahmassebpur , Brandon Li , Boris Barron , Héctor Abruña , Peter Frazier , Tomás Arias

We investigate the properties of natural orbitals and their occupation numbers of the ground state of two non-interacting anyons characterised by the fractional statistics parameter $\alpha$ and confined in a harmonic trap. We work in the…

Quantum Gases · Physics 2024-02-13 Jerzy Cioslowski , Oliver M. Brown , Tomasz Maciazek