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The accuracy of applying density functional theory to noncovalent interactions is hindered by errors arising from low-density regions of interaction-induced change in the density gradient, error compensation between correlation and exchange…

Chemical Physics · Physics 2014-10-22 Marcin Modrzejewski , Grzegorz Chałasiński , Małgorzata M. Szczęśniak

One-electron self-interaction and an incorrect asymptotic behavior of the Kohn-Sham exchange-correlation potential are among the most prominent limitations of many present-day density functionals. However, a one-electron…

Chemical Physics · Physics 2016-07-06 Tobias Schmidt , Eli Kraisler , Leeor Kronik , Stephan Kümmel

The numerical implementation of an exchange-correlation functional is not always an accurate reproduction of its theoretical specification. For example, density functionals for exchange and correlation can be defined by an exchange or…

Materials Science · Physics 2012-11-01 Jonathan E. Moussa , Peter A. Schultz

Density functional theory (DFT) exploits an independent-particle-system construction to replicate the densities and current of an interacting system. This construction is used here to access the exact effective potential and bias of…

Mesoscale and Nanoscale Physics · Physics 2018-03-30 Daniel Karlsson , Miroslav Hopjan , Claudio Verdozzi

Most applications of time-dependent density-functional theory (TDDFT) use the adiabatic local-density approximation (ALDA) for the dynamical exchange-correlation potential Vxc(r,t). An exact (i.e., nonadiabatic) extension of the…

Mesoscale and Nanoscale Physics · Physics 2015-06-25 C. A. Ullrich

This study investigates the influence of quantum effects on Coulomb explosion dynamics using time-dependent density functional theory (TDDFT) simulations, comparing classical, semi-classical, and quantum approaches. The goal is to elucidate…

Chemical Physics · Physics 2024-12-10 Samuel S. Taylor , Cody Covington , Kálmán Varga

The Skyrme effective interaction, with its multitude of parameterisations, along with its implemen- tation using the static and time-dependent density functional (TDHF) formalism have allowed for a range of microscopic calculations of…

Nuclear Theory · Physics 2018-12-05 P. D. Stevenson , M. C. Barton

To investigate inelastic electron scattering, which is ubiquitous in various fields of study, we carry out ab initio study of the real-time dynamics of a one-dimensional electron wave packet scattered by a hydrogen atom using different…

Atomic Physics · Physics 2020-06-24 Yeonghun Lee , Xiaolong Yao , Massimo V. Fischetti , Kyeongjae Cho

The time-dependent exchange-correlation potential has an unusual task in directing fictitious non-interacting electrons to move with exactly the same probability density as true interacting electrons. This has intriguing implications for…

Chemical Physics · Physics 2024-06-19 Davood Dar , Lionel Lacombe , Neepa T. Maitra

Approximate density functional theory (DFT) suffers from many-electron self- interaction error, otherwise known as delocalization error, that may be diagnosed and then corrected through elimination of the deviation from exact piecewise…

Materials Science · Physics 2016-11-08 Terry Z. H. Gani , Heather J. Kulik

Long-range charge transfer excited states are notoriously badly underestimated in time-dependent density functional theory (TDDFT). We resolve how {\it exact} TDDFT captures charge transfer between open-shell species: in particular the role…

Chemical Physics · Physics 2009-11-11 Neepa T. Maitra

A decomposition of the exact exchange-correlation potential of time-dependent density functional theory into an interaction component and a kinetic component offers a new starting point for non- adiabatic approximations. The components are…

Chemical Physics · Physics 2018-11-14 Johanna I. Fuks , Lionel Lacombe , Soeren E. B. Nielsen , Neepa T. Maitra

The complex nature of electron-electron correlations is made manifest in the very simple but non-trivial problem of two electrons confined within a sphere. The description of highly non-local correlation and self-interaction effects by…

Other Condensed Matter · Physics 2016-08-16 J. Jung , P. García-González , J. E. Alvarellos , R. W. Godby

The dynamic electron-ion collisions play an important rolein determining the static and transport properties of warmdense matter (WDM). Electron force field (eFF) method is applied to study the ionic transport properties of warm…

Computational Physics · Physics 2021-01-15 Yunpeng Yao , Qiyu Zeng , Ke Chen , Dongdong Kang , Yong Hou , Qian Ma , Jiayu Dai

We investigate the time an electronic excitation travels in a supermolecular setup using a measurement process in an open quantum-system framework. The approach is based on the stochastic Schr\"odinger equation and uses a Hamiltonian from…

Materials Science · Physics 2013-12-09 Dirk Hofmann , Heiko Appel , Massimiliano Di Ventra , Stephan Kümmel

To explore whether the density-functional theory non-equilibrium Green's function formalism (DFT-NEGF) provides a rigorous framework for quantum transport, we carried out time-dependent density functional theory (TDDFT) calculations of the…

Materials Science · Physics 2011-07-01 ChiYung Yam , Xiao Zheng , GuanHua Chen , Yong Wang , Thomas Frauenheim , Thomas A. Niehaus

In this work we have calculated excitation energies and photoionization cross sections of Be and Ne in the exact-exchange (EXX) approximation of time-dependent density functional theory (TDDFT). The main focus has been on the frequency…

Mesoscale and Nanoscale Physics · Physics 2015-05-14 Maria Hellgren , Ulf von Barth

First principles simulation of x-ray photoemission spectroscopy (XPS) is an important tool in the challenging interpretation and assignment of XPS data of metal-organic interfaces. We investigate the origin of the disagreement between XPS…

Materials Science · Physics 2021-12-03 Samuel J. Hall , Benedikt P. Klein , Reinhard J. Maurer

Simulating electron-ion dynamics using time-dependent density functional theory within an Ehrenfest dynamics scheme can be done in two ways that are in principle exact and identical: propagating time-dependent electronic Kohn-Sham equations…

Chemical Physics · Physics 2021-07-01 Lionel Lacombe , Neepa T. Maitra

The charging of insulating samples degrades the quality and complicates the interpretation of images in scanning electron microscopy and is important in other applications, such as particle detectors. In this paper we analyze this…

Classical Physics · Physics 2020-06-19 Behrouz Raftari , Neil Budko , Kees Vuik