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The particle-hole interaction problem is longstanding within time-dependent density functional theory (TDDFT) and leads to extreme errors in the prediction of K-edge X-ray absorption spectra (XAS). We derive a linear-response formalism that…

Chemical Physics · Physics 2022-10-18 Kevin Carter-Fenk , Leonardo A. Cunha , Juan E. Arias-Martinez , Martin Head-Gordon

We prove that the electron density function of a real physical system can be uniquely determined by its values on any finite subsystem. This establishes the existence of a rigorous density-functional theory for any open electronic system.…

Quantum Physics · Physics 2007-05-23 Xiao Zheng , Fan Wang , GuanHua Chen

Due to its favorable computational efficiency time-dependent (TD) density functional theory (DFT) enables the prediction of electronic spectra in a high-throughput manner across chemical space. Its predictions, however, can be quite…

Time-dependent density functional theory is extended to include dissipative systems evolving under a master equation, providing a Hamiltonian treatment for molecular electronics. For weak electric fields, the isothermal conductivity is…

Materials Science · Physics 2007-05-23 Kieron Burke , Roberto Car , Ralph Gebauer

We discuss issues related to pairing dynamics in nuclear large amplitude collective motion. The examples of effects which are not properly described within BCS theory are presented. In the second part we review properties of TDDFT and in…

Nuclear Theory · Physics 2018-07-03 P. Magierski , J. Grineviciute , K. Sekizawa

By introducing the self-energy density functionals for the dissipative interactions between the reduced system and its environment, we develop a time-dependent density-functional theory formalism based on an equation of motion for the…

Quantum Physics · Physics 2009-11-13 Xiao Zheng , Fan Wang , Chi Yung Yam , Yan Mo , GuanHua Chen

A simple approximate solution to the linear response equations of time-dependent density functional theory (TDDFT) is given. This extends the single-pole approximation (SPA) to two strongly-coupled poles. The analysis provides both an…

Materials Science · Physics 2009-11-11 H. Appel , E. K. U. Gross , K. Burke

The self consistent version of the density functional theory (DFT) is presented, which allows to calculate the ground state and dynamic properties of finite multi-electron systems such as atoms, molecules and clusters. The exact functional…

Condensed Matter · Physics 2007-05-23 M. Ya. Amusia , V. R. Shaginyan

Density Functional Theory (DFT) calculations of electrode material properties in high energy density storage devices like lithium batteries have been standard practice for decades. In contrast, DFT modelling of explicit interfaces in…

Materials Science · Physics 2020-06-24 Kevin Leung

Multiscale plasmonic systems e.g. extended metallic nanostructures with sub-nanometer inter-distances) play a key role in the development of next-generation nano-photonic devices. An accurate modeling of the optical interactions in these…

Mesoscale and Nanoscale Physics · Physics 2016-05-11 Cristian Ciracì , Fabio Della Sala

The van Leeuwen proof of linear-response time-dependent density functional theory (TDDFT) is generalized to thermal ensembles. This allows generalization to finite temperatures of the Gross-Kohn relation, the exchange-correlation kernel of…

Chemical Physics · Physics 2016-06-15 Aurora Pribram-Jones , Paul E. Grabowski , Kieron Burke

Electron dispersion forces play a crucial role in determining the structure and properties of biomolecules, molecular crystals and many other systems. However, an accurate description of dispersion is highly challenging, with the most…

Materials Science · Physics 2013-01-30 Jiří Klimeš , Angelos Michaelides

Density functional theory (DFT) is an incredible success story. The low computational cost, combined with useful (but not yet chemical) accuracy, has made DFT a standard technique in most branches of chemistry and materials science.…

Chemical Physics · Physics 2015-06-03 Kieron Burke

Following a previous paper [Y. Shi, Phys. Rev. C 98, 014329(2018)], we present an extension of the density-functional theory to allow for dynamic calculations based on the obtained static Hartree-Fock results. We perform extensive benchmark…

Nuclear Theory · Physics 2020-11-04 Yue Shi , Nobuo Hinohara , Bastian Schuetrumpf

Density functional theory (DFT), the most widely adopted method in modern computational chemistry, fails to describe accurately the electronic structure of strongly correlated systems. Here we show that DFT can be formally and practically…

Chemical Physics · Physics 2022-04-18 Daniel Gibney , Jan-Niklas Boyn , David A. Mazziotti

Effective field theory (EFT) methods are applied to density functional theory (DFT) as part of a program to systematically go beyond mean-field approaches to medium and heavy nuclei. A system of fermions with short-range, natural…

Nuclear Theory · Physics 2007-05-23 S. J. Puglia , A. Bhattacharyya , R. J. Furnstahl

Quantum effects of plasmonic phenomena have been explored through ab-initio studies, but only for exceedingly small metallic nanostructures, leaving most experimentally relevant structures too large to handle. We propose instead an…

Mesoscale and Nanoscale Physics · Physics 2015-09-24 Wei Yan , Martijn Wubs , N. Asger Mortensen

Warm dense matter (WMD) describes an intermediate phase, between condensed matter and classical plasmas, found in natural and man-made systems. In a laboratory setting, WDM needs to be created dynamically. It is typically laser or…

Plasma Physics · Physics 2022-03-14 Alexander J. White , Lee A. Collins , Katarina Nichols , S. X. Hu

The primary computational challenge when simulating nonadiabatic ab initio molecular dynamics is the unfavorable compute costs of electronic structure calculations with molecular size. Simple electronic structure theories, like…

Chemical Physics · Physics 2023-06-28 Justin J. Talbot , Martin Head-Gordon , Stephen J. Cotton

Classical dynamical density functional theory (DDFT) is one of the cornerstones of modern statistical mechanics. It is an extension of the highly successful method of classical density functional theory (DFT) to nonequilibrium systems.…

Soft Condensed Matter · Physics 2020-12-29 Michael te Vrugt , Hartmut Löwen , Raphael Wittkowski