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A combined density and first-order reduced-density-matrix (1RDM) functional method is proposed for the calculation of potential energy curves (PECs) of molecular multibond dissociation. Its 1RDM functional part, a pair density functional,…

Chemical Physics · Physics 2020-09-23 Robert van Meer , Oleg Gritsenko , Jeng-Da Chai

We present an accurate local density-functional for electronic-structure calculations within the density functional theory (DFT). The functional is derived by analyzing the structure of the standard perturbative expansion of the correlation…

Materials Science · Physics 2024-11-28 Mario Benites , Angel Rosado , Efstratios Manousakis

One-body reduced density matrix functional theory (RDMFT) provides an alternative to Density Functional Theory (DFT), able to treat static correlation while keeping a relatively low computation scaling. Its disadvantageous cost comes mainly…

Chemical Physics · Physics 2024-05-07 Nicolas G. Cartier , Klaas J. H. Giesbertz

Recently, an approximate theoretical framework was introduced, called local reduced density matrix functional theory (local-RDMFT), where functionals of the one-body reduced density matrix (1-RDM) are minimized under the additional…

Reduced density matrix functional theory (RDMFT) calculations are usually implemented in a decoupled manner, where the orbital and occupation optimizations are repeated alternately. Typically, orbital updates are performed using the unitary…

Chemical Physics · Physics 2024-09-04 Yi-Fan Yao , Neil Qiang Su

We present fully empirical exchange-correlation functionals to be used within reduced density matrix functional theory (RDMFT). These are of the popular J-K form, where the function of the occupation numbers that multiplies the Fock orbital…

Computational Physics · Physics 2017-03-03 Miguel A. L. Marques , N. N. Lathiotakis

The present work proposes to use density-functional theory (DFT) to correct for the basis-set error of wave-function theory (WFT). One of the key ideas developed here is to define a range-separation parameter which automatically adapts to a…

We consider a system of particles interacting via a purely repulsive, soft-core potential recently introduced to model effective pair interactions between dendrimers, which is expected to lead to the formation of crystals with multiple…

Soft Condensed Matter · Physics 2015-05-11 Davide Pini

Strongly correlated systems containing d/f-electrons present a challenge to conventional density functional theory (DFT), such as the widely used local density approximation (LDA) or generalized gradient approximation (GGA). In this work,…

Strongly Correlated Electrons · Physics 2024-01-19 Bei-Lei Liu , Yue-Chao Wang , Yu Liu , Hai-Feng Liu , Hai-Feng Song

This work presents a theory to unify the two independent theoretical frameworks of Kohn-Sham (KS) density functional theory (DFT) and reduced density matrix functional theory (RDMFT). The generalization of the KS orbitals to hypercomplex…

Chemical Physics · Physics 2021-11-18 Neil Qiang Su

Density functional theory (DFT) is an indispensable ab initio method in both quantum chemistry and condensed matter physics. Based on recent advancements in reduced density matrix functional theory (RDMFT), a variant of DFT that is believed…

Quantum Physics · Physics 2026-04-02 Chih-Chun Wang

A variational formulation for the calculation of interacting fermion systems based on the density-matrix functional theory is presented. Our formalism provides for a natural integration of explicit many-particle effects into standard…

Strongly Correlated Electrons · Physics 2013-05-29 Peter E. Bloechl , Christian F. J. Walther , Thomas Pruschke

A crucial theorem in Reduced Density Matrix Functional Theory (RDMFT) suggests that the universal pure and ensemble functional coincide on their common domain of pure N-representable one-matrices. We refute this by a comprehensive analysis…

Quantum Physics · Physics 2018-12-24 Christian Schilling

We propose and work out a reduced density matrix functional theory (RDMFT) for calculating energies of eigenstates of interacting many-electron systems beyond the ground state. Various obstacles which historically have doomed such an…

Quantum Physics · Physics 2021-07-08 Christian Schilling , Stefano Pittalis

Real-time time-dependent density functional theory (RT-TDDFT) is a powerful approach for investigating various ultrafast phenomena in materials. However, most existing RT-TDDFT studies rely on adiabatic local or semi-local approximations,…

Materials Science · Physics 2025-12-23 Yuyang Ji , Haotian Zhao , Peize Lin , Xinguo Ren , Lixin He

Standard density functional approximations often give questionable results for odd-electron radical complexes, with the error typically attributed to self-interaction. In density corrected density functional theory (DC-DFT), certain classes…

Chemical Physics · Physics 2015-06-19 Min-Cheol Kim , Eunji Sim , Kieron Burke

We recently introduced an efficient methodology to perform density-corrected Hartree-Fock density functional theory (DC(HF)-DFT) calculations and an extension to it we called "corrected" HF DFT (C(HF)-DFT). In this work, we take a further…

Chemical Physics · Physics 2023-11-10 Daniel Graf , Alex J. W. Thom

The one-particle reduced density-matrix (1-RDM) functional theory is a promising alternative to density-functional theory (DFT) that uses the 1-RDM rather than the electronic density as a basic variable. However, long-standing challenges…

Quantum Physics · Physics 2024-08-20 Matthieu Vladaj , Quentin Marécat , Bruno Senjean , Matthieu Saubanère

Multi-center transition metal complexes (MCTMs) with magnetically interacting ions have been proposed as components for information processing devices and storage units. For any practical application of MCTMs as magnetic units, it is…

Chemical Physics · Physics 2023-04-03 Henry C. Fitzhugh , James W. Furness , Mark R. Pederson , Juan E. Peralta , Jianwei Sun

Predicting interfacial thermodynamics across molecular and continuum scales remains a central challenge in computational science. Classical density functional theory (cDFT) provides a first-principles route to connect microscopic…

Computational Physics · Physics 2026-01-01 Edoardo Monti , Peter Yatsyshin , Konstantinos Gkagkas , Andrew B. Duncan