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During the last two decades density functional based linear response approaches have become the de facto standard for the calculation of optical properties of small and medium-sized molecules. At the heart of these methods is the solution…

Chemical Physics · Physics 2015-01-23 Robert Rüger , Erik van Lenthe , You Lu , Johannes Frenzel , Thomas Heine , Lucas Visscher

This article generalizes the notion of the local density of a many-body system to introduce collective coordinates as explicit degrees of freedom. It is shown that the energy of the system can be expressed as a functional of this object.…

Nuclear Theory · Physics 2014-04-23 Thomas Lesinski

Kohn-Sham density functional theory (DFT) is nowadays widely used for electronic structure theory simulations, and the accuracy and efficiency of DFT rely on approximations of the exchange-correlation functional. By inclusion of the kinetic…

Materials Science · Physics 2023-06-01 Renxi Liu , Daye Zheng , Xinyuan Liang , Xinguo Ren , Mohan Chen , Wenfei Li

A density functional theory (DFT) framework is presented that links functional derivatives of free-energy functionals to non-linear static density response functions in quantum many-body systems. Within this framework, explicit expressions…

The generalized density matrix (GDM) method is used to calculate microscopically the parameters of the collective Hamiltonian. Higher order anharmonicities are obtained consistently with the lowest order results, the mean field…

Nuclear Theory · Physics 2011-09-23 L. Y. Jia

The generalized time-dependent generator coordinate method (TD-GCM) is extended to include pairing correlations. The correlated GCM nuclear wave function is expressed in terms of time-dependent generator states and weight functions. The…

Nuclear Theory · Physics 2024-02-05 B. Li , D. Vretenar , T. Nikšić , J. Zhao , P. W. Zhao , J. Meng

The response part of the exchange-correlation potential of Kohn-Sham density functional theory plays a very important role, for example for the calculation of accurate band gaps and excitation energies. Here we analyze this part of the…

Chemical Physics · Physics 2018-08-29 Sara Giarrusso , Paola Gori-Giorgi , Klaas J. H. Giesbertz

This article addresses a fundamental problem faced by the ab initio community: the lack of an effective formalism for the rapid exploration and exchange of new methods. To rectify this, we introduce a novel, basis-set independent,…

Materials Science · Physics 2009-10-31 Sohrab Ismail-Beigi , T. A. Arias

We proposed in Ref. [arXiv:1812.09285v2] a way to improve energy density functionals in the density functional theory based on the combination of the inverse Kohn-Sham method and the density functional perturbation theory. In this…

Chemical Physics · Physics 2020-12-24 Tomoya Naito , Daisuke Ohashi , Haozhao Liang

We use the exact strong-interaction limit of the Hohenberg-Kohn energy density functional to approximate the exchange-correlation energy of the restricted Kohn-Sham scheme. Our approximation corresponds to a highly non-local density…

Strongly Correlated Electrons · Physics 2012-12-12 Francesc Malet , Paola Gori-Giorgi

We present a computationally efficient approach to perform large-scale all-electron density functional theory calculations by enriching the classical finite element basis with compactly supported atom-centered numerical basis functions that…

Computational Physics · Physics 2017-01-11 Bikash Kanungo , Vikram Gavini

Using the Kohn-Sham (KS) inversion method of Hollins et al. [J. Phys.: Condens. Matter 29, 04LT01 (2017)], we invert densities from variational and diffusion quantum Monte Carlo (QMC) calculations to obtain benchmark QMC-KS potentials for a…

Kohn-Sham density functional theory (DFT) has long struggled with the accurate description of strongly correlated and open shell systems and improvements have been minor even in the newest hybrid functionals. In this Letter we treat the…

Chemical Physics · Physics 2021-04-01 Danny Gibney , Jan-Niklas Boyn , David A. Mazziotti

Recent experimental findings reveal non-conventional fluorescence emission in biological systems devoid of conjugated bonds or aromatic compounds, termed \textit{Non-Aromatic Fluorescence} (NAF). This phenomenon is exclusive to aggregated…

One of the most important open challenges in modern Kohn-Sham (KS) density-functional theory (DFT) is the correct treatment of fractional electron charges and spins. Approximate exchange-correlation (XC) functionals struggle to do this in a…

Chemical Physics · Physics 2015-12-24 Jonathan Nafziger , Adam Wasserman

The density functional scheme for calculating the pair density is presented by means of the constrained-search technique. The resultant single-particle equation takes the form of the modified Hartree-Fock equation which contains the kinetic…

Strongly Correlated Electrons · Physics 2015-06-25 Masahiko Higuchi , Katsuhiko Higuchi

In a recent Comment (arXiv:0710.0018), Maitra, Burke, and van Leeuwen (MBL) attempt to refute our criticism of the foundations of TDDFT (see Phys. Rev. A 75, 022513 (2007)). However, their arguments miss the essence of our position. This is…

Other Condensed Matter · Physics 2008-11-26 J. Schirmer , A. Dreuw

We propose a systematic procedure for the approximation of density functionals in density functional theory that consists of two parts. First, for the efficient approximation of a general density functional, we introduce an efficient ansatz…

Strongly Correlated Electrons · Physics 2016-08-29 Michael Lubasch , Johanna I. Fuks , Heiko Appel , Angel Rubio , J. Ignacio Cirac , Mari-Carmen Bañuls

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

We present a numerical method for grand canonical density functional theory (DFT) tailored to solid-state systems, employing Gaussian-type orbitals as the primary basis. Our approach directly minimizes the grand canonical free energy using…

Chemical Physics · Physics 2025-10-09 Anton Z. Ni , Adam Rettig , Joonho Lee