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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

To advance the foundation of one-particle reduced density matrix functional theory (1RDMFT) we refine and relate some of its fundamental features and underlying concepts. We define by concise means the scope of a 1RDMFT, identify its…

Quantum Physics · Physics 2023-10-10 Julia Liebert , Adam Yanis Chaou , Christian Schilling

In [Phys. Rev. Lett. 127, 023001 (2021)] a reduced density matrix functional theory (RDMFT) has been proposed for calculating energies of selected eigenstates of interacting many-fermion systems. Here, we develop a solid foundation for this…

Quantum Physics · Physics 2022-05-06 Julia Liebert , Federico Castillo , Jean-Philippe Labbé , Christian Schilling

For translationally invariant one-band lattice models, we exploit the ab initio knowledge of the natural orbitals to simplify reduced density matrix functional theory (RDMFT). Striking underlying features are discovered: First, within each…

Quantum Physics · Physics 2019-01-08 Christian Schilling , Rolf Schilling

Density functional theory constitutes the workhorse of modern electronic structure calculations due to its favourable computational cost despite the fact that it usually fails to describe strongly correlated systems. A particularly…

Quantum Gases · Physics 2022-05-06 Julia Liebert

A mathematical framework for reduced density matrix functional theory (RDMFT) is proposed. The work is inspired by and generalizes the work by E.H.~Lieb [E.H. Lieb, Int. J. Quant. Chem. 24(1983), pp.243--277] on density-functional theory…

Mathematical Physics · Physics 2026-01-06 Håkon R. Fredheim , Simen Kvaal

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

As a new approach to efficiently describe correlation effects in the relativistic quantum world we propose to consider reduced density matrix functional theory, where the key quantity is the first-order reduced density matrix (1-RDM). In…

Chemical Physics · Physics 2022-05-05 M. Rodríguez-Mayorga , K. J. H. Giesbertz , L. Visscher

Density functional theory (DFT), one of the most widely utilized methods available to computational chemistry, fails to describe systems with statically correlated electrons. To address this shortcoming, in previous work we transformed DFT…

Chemical Physics · Physics 2023-01-02 Daniel Gibney , Jan-Niklas Boyn , David A. Mazziotti

The $N$-representability problem places fundamental constraints on reduced density matrices (RDMs) that originate from physical many-fermion quantum states. Motivated by recent developments in functional theories, we introduce a hierarchy…

Quantum Physics · Physics 2026-04-28 Julia Liebert , Anna O. Schouten , Irma Avdic , Christian Schilling , David A. Mazziotti

Reduced density-matrix functional theory (RDMFT) is a promising alternative approach to the problem of electron correlation. Like standard density functional theory, it contains an unknown exchange-correlation functional, for which several…

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

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 establish one-body reduced density-matrix functional theory for the canonical ensemble in a finite basis set at an elevated temperature. Including temperature guarantees differentiability of the universal functional by occupying all…

Mathematical Physics · Physics 2023-02-22 Sarina M. Sutter , Klaas J. H. Giesbertz

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

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

We propose a novel scheme to bring reduced density matrix functional theory (RDMFT) into the realm of density functional theory (DFT) that preserves the accurate density functional description at equilibrium, while incorporating accurately…

Chemical Physics · Physics 2014-11-07 Nektarios N. Lathiotakis , Nicole Helbig , Angel Rubio , Nikitas I. Gidopoulos

Reduced density-matrix functional theory (RDMFT) provides a variational route to electronic correlations beyond conventional density-functional approximations, but explicit evaluations of density-matrix functionals still scale exponentially…

Chemical Physics · Physics 2026-05-19 Konstantin Tamoev , Robert Schade , Thomas D. Kühne

We establish necessary and sufficient conditions for the N-representability of the universal one-electron reduced density matrix functional. Functionals satisfying these conditions are guaranteed to yield variational upper bounds on the…

Quantum Physics · Physics 2026-04-08 Jannis Erhard , Paul W. Ayers

We initiate the recently proposed $\boldsymbol{w}$-ensemble one-particle reduced density matrix functional theory ($\boldsymbol{w}$-RDMFT) by deriving the first functional approximations and illustrate how excitation energies can be…

Quantum Gases · Physics 2023-05-22 Julia Liebert , Christian Schilling

In many of the approximate functionals in one-body reduced density matrix (1RDM) functional theory, the approximate two-body reduced density matrix (2RDM) in the natural orbital representation only depends on the natural occupation numbers.…

Chemical Physics · Physics 2020-11-24 Klaas J. H. Giesbertz
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