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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

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…

A system of electrons in a local or nonlocal external potential can be studied with 1-matrix functional theory (1MFT), which is similar to density functional theory (DFT) but takes the one-particle reduced density matrix (1-matrix) instead…

Strongly Correlated Electrons · Physics 2008-07-23 Ryan Requist , Oleg Pankratov

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

In this work we explore the performance of approximations to electron correlation in reduced density-matrix functional theory (RDMFT) and of approximations to the observables calculated within this theory. Our analysis focuses on the…

Strongly Correlated Electrons · Physics 2015-02-26 Stefano Di Sabatino , Jan A. Berger , Lucia Reining , Pina Romaniello

We study the accuracy of Kohn-Sham density functional theory (DFT) for warm- and hot-dense matter (WDM and HDM). Specifically, considering a wide range of systems, we perform accurate ab initio molecular dynamics simulations with…

Computational Physics · Physics 2024-11-21 Phanish Suryanarayana , Arpit Bhardwaj , Xin Jing , Shashikant Kumar , John E. Pask

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

Due to efficient scaling with electron number N, density functional theory (DFT) is widely used for studies of large molecules and solids. Restriction of an exact mean-field theory to local potential functions has recently been questioned.…

Other Condensed Matter · Physics 2015-06-24 Robert K. Nesbet

Aspects of Density Functional Resonance Theory (DFRT) [Phys. Rev. Lett. \textbf{107}, 163002 (2011)], a recently developed complex-scaled version of ground-state Density Functional Theory (DFT), are studied in detail. The asymptotic…

Quantum Physics · Physics 2015-06-04 Daniel L. Whitenack , Adam Wasserman

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

A hybrid Kohn-Sham Density Functional Theory (KS-DFT) and 1-electron Reduced Density Matrix Functional Theory (1-RDMFT) has recently been developed to describe strongly correlated systems at mean-field computational cost. This approach…

Computational Physics · Physics 2025-04-14 Daniel Gibney , Jan-Niklas Boyn

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

Reduced density-matrix functional theory (RDMFT) has become an appealing alternative to density-functional theory to describe electronic properties of highly-correlated systems. Here we derive exact conditions for the suitability of RDMFT…

Strongly Correlated Electrons · Physics 2012-04-19 A. Putaja , E. Rasanen

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

We develop a method in which the electronic densities of small fragments determined by Kohn-Sham density functional theory (DFT) are embedded using stochastic DFT to form the exact density of the full system. The new method preserves the…

Chemical Physics · Physics 2015-06-19 Daniel Neuhauser , Roi Baer , Eran Rabani

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

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

In the recent work of S. Sharma \emph{et al.}, (arxiv.org: arxiv:0912.1118), a single-electron spectrum associated with the natural orbitals was defined as the derivative of the total energy with respect to the occupation numbers at half…

Chemical Physics · Physics 2012-03-07 E. N. Zarkadoula , S. Sharma , J. K. Dewhurst , E. K. U. Gross , N. N. Lathiotakis

The Hubbard model provides a test bed to investigate the complex behaviour arising from electron-electron interaction in strongly-correlated systems and naturally emerges as the foundation model for lattice density functional theory (DFT).…

Strongly Correlated Electrons · Physics 2025-01-29 Eoghan Cronin , Rajarshi Tiwari , Stefano Sanvito

Density functional theory (DFT) offers a desirable balance between quantitative accuracy and computational efficiency in practical many-electron calculations. Its central component, the exchange-correlation energy functional, has been…

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