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Density functional theory (DFT) is the de facto approach for predicting self-consistent-field electronic structures of ground-state configurations of complex atoms, molecules, and solids and providing their property data for materials…

Materials Science · Physics 2024-01-30 Zi-Kui Liu

A self-consistent calculation scheme for correlated electron systems is created based on the density-functional theory (DFT). Our scheme is a multi-reference DFT (MR-DFT) calculation in which the electron charge density is reproduced by an…

Strongly Correlated Electrons · Physics 2009-11-13 Koichi Kusakabe , Naoshi Suzuki , Shusuke Yamanaka , Kizashi Yamaguchi

The stochastic density functional theory (DFT) [Phys. Rev. Lett. 111, 106402 (2013)] is a valuable linear scaling approach to Kohn-Sham DFT that does not rely on the sparsity of the density matrix. Linear (and often sub-linear) scaling is…

Chemical Physics · Physics 2019-02-20 Ming Chen , Roi Baer , Daniel Neuhauser , Eran Rabani

Due to several attractive features, the meta-generalized-gradient approximations (meta-GGAs) are considered to be the most advanced and potentially accurate semilocal exchange-correlation functionals in the rungs of the Jacob's ladder of…

Atomic and Molecular Clusters · Physics 2020-04-28 Abhilash Patra , Subrata Jana , Lucian A. Constantin , Prasanjit Samal

The systematic underestimation of band gaps is one of the most fundamental challenges in semilocal density functional theory (DFT). In addition to hindering the application of DFT to predicting electronic properties, the band gap problem is…

Chemical Physics · Physics 2024-08-27 Kyle Bystrom , Stefano Falletta , Boris Kozinsky

The multi-configurational self-consistent field theory is considered the standard starting point for almost all multireference approaches required for strongly-correlated molecular problems. The limitation of the approach is generally given…

Chemical Physics · Physics 2015-10-14 Robert E. Thomas , Qiming Sun , Ali Alavi , George H. Booth

Hybrid functionals' non-local exchange-correlation potential contains a derivative discontinuity that improves on standard semi-local density functional theory (DFT) band gaps. Moreover, by careful parameterization, hybrid functionals can…

Materials Science · Physics 2017-11-06 Viktor Ivády , Adam Gali , Igor A. Abrikosov

The calculation of the band-gap by density-functional theory (DFT) methods is examined by considering the behavior of the energy as a function of number of electrons. It is found that the incorrect band-gap prediction with most approximate…

Materials Science · Physics 2009-11-13 Aron J. Cohen , Paula Mori-Sánchez , Weitao Yang

We develop a semiclassical density functional theory in the context of quantum dots. Coulomb blockade conductance oscillations have been measured in several experiments using nanostructured quantum dots. The statistical properties of these…

Mesoscale and Nanoscale Physics · Physics 2009-10-31 Denis Ullmo , Tatsuro Nagano , Steven Tomsovic , Harold U. Baranger

We reexamine the recently introduced basis-set correction theory based on density-functional theory consisting in correcting the basis-set incompleteness error of wave-function methods using a density functional. We use a one-dimensional…

Chemical Physics · Physics 2022-02-16 Diata Traore , Emmanuel Giner , Julien Toulouse

We present two efficient and intruder-free methods for treating dynamic correlation on top of general multi-configuration reference wave functions---including such as obtained by the density matrix renormalization group (DMRG) with large…

Chemical Physics · Physics 2016-09-13 Sandeep Sharma , Gerald Knizia , Sheng Guo , Ali Alavi

The computationally expensive evaluation and storage of high-rank reduced density matrices (RDMs) has been the bottleneck in the calculation of dynamic correlation for multireference wave functions in large active spaces. We present a…

Chemical Physics · Physics 2020-01-08 Ankit Mahajan , Nick S. Blunt , Iliya Sabzevari , Sandeep Sharma

Multi-configurational electronic structure theory delivers the most versatile approximations to many-electron wavefunctions, flexible enough to deal with all sorts of transformations, ranging from electronic excitations, to open-shell…

Chemical Physics · Physics 2024-05-07 Kalman Szenes , Maximilian Moerchen , Paul Fischill , Markus Reiher

Molecular Density Functional Theory (MDFT) offers an efficient implicit- solvent method to estimate molecule solvation free-energies whereas conserving a fully molecular representation of the solvent. Even within a second order ap-…

Soft Condensed Matter · Physics 2014-06-12 Volodymyr P. Sergiievskyi , Guillaume Jeanmairet , Maximilien Levesque , Daniel Borgis

Qualitatively incorrect results are obtained for the Mn dimer in density functional theory calculations using the generalized gradient approximation (GGA) and similar results are obtained from local density and meta-GGA functionals. The…

Chemical Physics · Physics 2021-05-18 Aleksei V. Ivanov , Tushar K. Ghosh , Elvar Ö. Jónsson , Hannes Jónsson

Combining classical density functional theory (cDFT) with quantum mechanics (QM) methods offers a computationally efficient alternative to traditional QM/molecular mechanics (MM) approaches for modeling mixed quantum-classical systems at…

Statistical Mechanics · Physics 2026-02-17 Guillaume Jeanmairet , Maxime Labat , Emmanuel Giner

We showcase the advantages of orbital-free density-potential functional theory (DPFT), a more flexible variant of Hohenberg-Kohn density functional theory. DPFT resolves the usual trouble with the gradient-expanded kinetic energy functional…

Quantum Gases · Physics 2021-06-16 Martin-Isbjörn Trappe , Jun Hao Hue , Berthold-Georg Englert

Methods based on propagation of the one-body reduced density-matrix hold much promise for the simulation of correlated many-electron dynamics far from equilibrium, but difficulties with finding good approximations for the interaction term…

Chemical Physics · Physics 2016-02-12 Peter Elliott , Neepa T. Maitra

Density functional theory (DFT) provides a theoretical framework for efficient and fairly accurate calculations of the electronic structure of molecules and crystals. The main features of density functional theory are described and DFT…

Chemical Physics · Physics 2012-06-12 Hauke Paulsen , Alfred Xaver Trautwein

A critical challenge for density functional theory (DFT) in practice is its limited ability to treat static electron correlation, leading to errors in its prediction of charges, multiradicals, and reaction barriers. Recently, we combined…

Chemical Physics · Physics 2024-11-05 Daniel Gibney , Jan-Niklas Boyn , David A. Mazziotti