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In this work we get insight into the impact of reduced density matrix functionals on the quality of removal/addition energies obtained using the Extended Koopmans' Theorem (EKT). Within reduced density matrix functional theory (RDMFT) the…

Strongly Correlated Electrons · Physics 2022-12-26 S. Di Sabatino , J. Koskelo , J. A. Berger , P. Romaniello

In this paper, we apply the recently developed ab initio renormalized excitonic method (REM) to the excitation energy calculations of various molecular aggregates, through the extension of REM to the time-dependent density functional theory…

Chemical Physics · Physics 2013-05-07 Yingjin Ma , Haibo Ma

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

Understanding the properties of warm dense hydrogen is of key importance for the modeling of compact astrophysical objects and to understand and further optimize inertial confinement fusion (ICF) applications. The work horse of warm dense…

The very good performance of modern density functional theory for molecular geometries and harmonic vibrational frequencies has been well established. We investigate the performance of density functional theory (DFT) for quartic force…

Chemical Physics · Physics 2007-05-23 A. Daniel Boese , Wim Klopper , Jan M. L. Martin

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

Efficiently recovering dynamic correlation in strongly correlated systems without incurring prohibitive computational costs remains a central challenge in quantum chemistry. In this Perspective, we review and benchmark methods capable of…

Chemical Physics · Physics 2026-05-22 Michał Hapka , Aleksandra Tucholska , Katarzyna Pernal

A density functional theory (DFT) of lattice fermion models is presented, which uses the single-particle density matrix gamma_{ij} as basic variable. A simple, explicit approximation to the interaction-energy functional W[gamma] of the…

Strongly Correlated Electrons · Physics 2009-11-07 R. Lopez-Sandoval , G. M. Pastor

Density functional theory (DFT) embedding provides a formally exact framework for interfacing correlated wave-function theory (WFT) methods with lower-level descriptions of electronic structure. Here, we report techniques to improve the…

Chemical Physics · Physics 2015-06-12 Jason D. Goodpaster , Taylor A. Barnes , Frederick R. Manby , Thomas F. Miller

While in principle exact, Kohn-Sham density functional theory -- the workhorse of computational chemistry -- must rely on approximations for the exchange-correlation functional. Despite staggering successes, present-day approximations still…

In the exact Kohn-Sham density-functional theory (DFT), the total energy versus the number of electrons is a series of linear segments between integer points. However, commonly used approximate density functionals produce total energies…

Materials Science · Physics 2013-04-03 Eli Kraisler , Leeor Kronik

We propose a method that incorporates explicit derivative discontinuity of the total energy with respect to the number of electrons and treats both delocalization and static correlation effects in density functional calculations. Our…

Strongly Correlated Electrons · Physics 2018-03-08 Fei Zhou , Vidvuds Ozolins

A new approach for calculating spectral density functions of strongly correlated electron systems is proposed within the exact diagonalization method of dynamical mean-field theory (DMFT). This approach is based on the analytic continuation…

Strongly Correlated Electrons · Physics 2016-10-05 Song-Jin O , Hak-Chol Pak , Kwang-Il Ryom , Song-Jin Im

It is shown that the DFT exchange and correlation functionals satisfy an expression that couples exchange and correlation functionals and functional derivatives evaluated at three different densities and for two particle numbers. This…

Materials Science · Physics 2015-05-30 Daniel P. Joubert

Multicomponent density functional theory (DFT) enables the consistent quantum mechanical treatment of both electrons and protons. A major challenge has been the design of electron-proton correlation functionals that produce even…

Chemical Physics · Physics 2017-09-26 Yang Yang , Kurt R. Brorsen , Tanner Culpitt , Michael V. Pak , Sharon Hammes-Schiffer

We present a novel method for calculating the fundamental gap. To this end, reduced-density-matrix-functional theory is generalized to fractional particle number. For each fixed particle number, $M$, the total energy is minimized with…

Strongly Correlated Electrons · Physics 2009-11-11 N. Helbig , N. N. Lathiotakis , M. Albrecht , E. K. U. Gross

We introduced a new electron density n({\epsilon}) by projecting the spatial electron density n(r) onto the energy coordinate {\epsilon} defined with the external potential \upsion (r) of interest. Then, a density functional theory (DFT)…

Chemical Physics · Physics 2018-02-20 Hideaki Takahashi

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 introduce an orbital free electron density functional approximation based on alchemical perturbation theory. Given convergent perturbations of a suitable reference system, the accuracy of popular self-consistent Kohn-Sham density…

Chemical Physics · Physics 2020-05-27 Guido Falk von Rudorff , O. Anatole von Lilienfeld

We combine density-functional theory with density-matrix functional theory to get the best of both worlds. This is achieved by range separation of the electronic interaction which permits to rigorously combine a short-range density…

Chemical Physics · Physics 2015-05-19 Daniel R. Rohr , Julien Toulouse , Katarzyna Pernal
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