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The present work demonstrates a robust protocol for probing localized electronic structure in condensed-phase systems, operating in terms of a recently proposed theory for decomposing the results of Kohn-Sham density functional theory in a…

Chemical Physics · Physics 2021-06-29 Janus J. Eriksen

Real-time time-dependent density functional theory (TDDFT) is widely considered to be the most accurate available method for calculating electronic stopping powers from first principles, but there have been relatively few assessments of the…

Computational Physics · Physics 2024-01-18 Alina Kononov , Alexander J. White , Katarina A. Nichols , S. X. Hu , Andrew D. Baczewski

We present a numerical modeling workflow based on machine learning (ML) which reproduces the the total energies produced by Kohn-Sham density functional theory (DFT) at finite electronic temperature to within chemical accuracy at negligible…

We show that the energetics and lifetimes of resonances of finite systems under an external electric field can be captured by Kohn--Sham density functional theory (DFT) within the formalism of uniform complex scaling. Properties of…

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

Nuclear Density Functional Theory (DFT) plays a prominent role in the understanding of nuclear structure, being the approach with the widest range of applications. Hohenberg and Kohn theorems warrant the existence of a nuclear Energy…

Nuclear Theory · Physics 2020-03-03 G. Accorto , P. Brandolini , F. Marino , A. Porro , A. Scalesi , G. Colò , X. Roca-Maza , E. Vigezzi

Density functional theory is currently the most widely applied method in electronic structure theory. The Kohn-Sham method, based on a fictitious system of non-interacting particles, is the work horse of the theory. The particular form of…

Chemical Physics · Physics 2016-06-01 Hubertus J J van Dam

Gross--Oliveira--Kohn (GOK) ensemble density-functional theory (GOK-DFT) is a time-\textit{independent} extension of density-functional theory (DFT) which allows to compute excited-state energies via the derivatives of the ensemble energy…

Chemical Physics · Physics 2020-06-18 Clotilde Marut , Bruno Senjean , Emmanuel Fromager , Pierre-François Loos

Localized molecular orbitals are often used for the analysis of chemical bonds, but they can also serve to efficiently and comprehensibly compute linear response properties. While conventional canonical molecular orbitals provide an…

Chemical Physics · Physics 2023-02-08 Souloke Sen , Bruno Senjean , Lucas Visscher

Nanoscale electronic transport is of intense technological interest, with applications ranging from semiconducting devices and molecular junctions to charge migration in biological systems. Most explicit theoretical approaches treat…

Mesoscale and Nanoscale Physics · Physics 2014-08-08 Justin E. Elenewski , Hanning Chen

In this contribution, we extend our framework for analyzing and visualizing correlated many-electron dynamics to non-variational, highly scalable electronic structure method. Specifically, an explicitly time-dependent electronic wave packet…

Chemical Physics · Physics 2017-04-27 Gunter Hermann , Vincent Pohl , Jean Christophe Tremblay

X-ray Thomson scattering (XRTS) constitutes an essential technique for diagnosing material properties under extreme conditions, such as high pressures and intense laser heating. Time-dependent density functional theory (TDDFT) is one of the…

The response of an extended periodic system to a homogeneous field (of wave-vector $q=0$) cannot be obtained from a $q=0$ time-dependent density functional theory (TDDFT) calculation, because the Runge-Gross theorem does not apply.…

Materials Science · Physics 2016-08-31 Neepa T. Maitra , Ivo Souza , Kieron Burke

This paper gives an introduction to the Keldysh formalism, with emphasis on its usefulness in time-dependent density functional theory. In the first part we introduce the Keldysh contour and the one-particle Green function defined on this…

Mesoscale and Nanoscale Physics · Physics 2007-05-23 Robert van Leeuwen , Nils Erik Dahlen , Gianluca Stefanucci , Carl-Olof Almbladh , Ulf von Barth

Variational excited-state density functional theory (DFT) enables the calculation of excited states at a cost comparable to ground-state calculations, but single-configuration approaches often suffer from spin contamination. We implement…

Chemical Physics · Physics 2026-05-28 Michael J. Sahre , Marco Romanelli , Martijn Marsman , Leticia González , Georg Kresse

We develop a generalization of the Kohn-Sham density functional theory (KS-DFT) + Hubbard $U$ (DFT+$U$) method to the excited-state regime. This has the form of Hubbard $U$ corrected linear-response time-dependent DFT, or `TDDFT+$U$'.…

Strongly Correlated Electrons · Physics 2019-04-24 Okan K. Orhan , David D. O'Regan

Quantum mechanical methods based on the density functional theory (DFT) offer a realistic possibility of first-principles design of organic donor-acceptor systems and engineered band-gap materials. This promise is contingent upon the…

Chemical Physics · Physics 2013-12-03 Marcin Modrzejewski , Grzegorz Chałasiński , Małgorzata M. Szczęśniak

Ultrafast electronic dynamics in solids lies at the core of modern condensed matter and materials physics. To build up a practical ab initio method for studying solids under photoexcitation, we develop a momentum-resolved real-time time…

Materials Science · Physics 2018-10-17 Chao Lian , Shi-Qi Hu , Meng-Xue Guan , Sheng Meng

We present a $\Delta$-machine learning model for obtaining Kohn-Sham accuracy from orbital-free density functional theory (DFT) calculations. In particular, we employ a machine learned force field (MLFF) scheme based on the kernel method to…

Chemical Physics · Physics 2023-10-11 Shashikant Kumar , Xin Jing , John E. Pask , Andrew J. Medford , Phanish Suryanarayana

In this work we review the mapping from densities to potentials in quantum mechanics, which is the basic building block of time-dependent density-functional theory and the Kohn-Sham construction. We first present detailed conditions such…

Other Condensed Matter · Physics 2015-05-20 Michael Ruggenthaler , Markus Penz , Robert van Leeuwen
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