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In this comparative study we benchmark a recently developed non-adiabatic exchange-correlation potential within time-dependent density functional theory (TDDFT) (Phys.\ Rev.\ Lett.\ {\bf 120}, 157701 (2018)) by (a) validating the transient…

Statistical Mechanics · Physics 2019-02-20 Niklas Dittmann , Nicole Helbig , Dante M. Kennes

We formulate a time-dependent density functional theory for the coupled dynamics of electrons and nuclei that goes beyond the Born-Oppenheimer (BO) approximation. We prove that the time-dependent marginal nuclear probability density…

Chemical Physics · Physics 2025-11-14 Chen Li , Ryan Requist , E. K. U. Gross

Modern density functional theory (DFT) calculations employ the Kohn-Sham (KS) system of non-interacting electrons as a reference, with all complications buried in the exchange-correlation energy (Exc). The adiabatic connection formula gives…

Other Condensed Matter · Physics 2009-10-02 Zhenfei Liu , Kieron Burke

In time-dependent density-functional theory, exchange and correlation (xc) beyond the adiabatic local density approximation can be described in terms of viscoelastic stresses in the electron liquid. In the time domain, this leads to a…

Mesoscale and Nanoscale Physics · Physics 2009-11-10 H. O. Wijewardane , C. A. Ullrich

Due to efficient scaling with electron number N, density functional theory (DFT) is widely used for studies of large molecules and solids. Restriction of an exact mean-field theory to local potential functions has recently been questioned.…

Other Condensed Matter · Physics 2015-06-24 Robert K. Nesbet

Starting from exact expression for the dynamical spin susceptibility in the time-dependent density functional theory a controversial issue about exchange interaction parameters and spin-wave excitation spectra of itinerant electron…

Materials Science · Physics 2009-11-10 M. I. Katsnelson , A. I. Lichtenstein

Lack of memory (locality in time) is a major limitation of almost all present time-dependent density functional approximations. By using semiclassical dynamics to compute correlation effects within a density-matrix functional approach, we…

Chemical Physics · Physics 2015-05-18 A. K. Rajam , I. Raczkowska , N. T. Maitra

We construct a nonlocal density functional approximation with full exact exchange, while preserving the constraint-satisfaction approach and justified error cancellations of simpler semilocal functionals. This is achieved by interpolating…

Chemical Physics · Physics 2009-11-13 John P. Perdew , Viktor N. Staroverov , Jianmin Tao , Gustavo E. Scuseria

We address and quantify the role of non-adiabaticity ("memory effects") in the exchange-correlation (xc) functional of time-dependent density functional theory (TDDFT) for describing non-linear dynamics of many-body systems. Time-dependent…

Other Condensed Matter · Physics 2015-06-18 Johanna I. Fuks , Mehdi Farzanehpour , Ilya V. Tokatly , Heiko Appel , Stefan Kurth , Angel Rubio

A time-dependent current-density-functional theory for many-particle systems in interaction with arbitrary external baths is developed. We prove that, given the initial quantum state $|\Psi_0>$ and the particle-bath interaction operator,…

Mesoscale and Nanoscale Physics · Physics 2007-06-13 Massimiliano Di Ventra , Roberto D'Agosta

The exact exchange-correlation (xc) potential of time-dependent density functional theory has been shown to have striking features. For example, step and peak features are generically found when the system is far from its ground-state, and…

Chemical Physics · Physics 2014-03-11 Kai Luo , Johanna I. Fuks , Ernesto D. Sandoval , Peter Elliott , Neepa T. Maitra

Motivated by the considerable importance of material properties in modern condensed matter physics research, and using techniques of the $N_{e}$ -electron systems in terms of the electron density $n_{\sigma e}\left( r\right) $ needed to…

Materials Science · Physics 2024-07-19 A. Belhaj , S. E. Ennadifi

We propose a practical approximation to the exchange-correlation functional of (time-dependent) density functional theory for many-electron systems coupled to photons. The (time non-local) optimized effective potential (OEP) equation for…

Mesoscale and Nanoscale Physics · Physics 2015-09-02 Camilla Pellegrini , Johannes Flick , Ilya V. Tokatly , Heiko Appel , Angel Rubio

The dynamics of a localized molecular spin under the influence of external voltage pulses is addressed using a generalized spin equation of motion. The approach incorporates anisotropic fields, non-equilibrium conditions, and non-adiabatic…

Mesoscale and Nanoscale Physics · Physics 2018-12-05 Henning Hammar , Jonas Fransson

The relative merits of current-spin-density- and spin-density-functional theory are investigated for solids treated within the exact-exchange-only approximation. Spin-orbit splittings and orbital magnetic moments are determined at zero…

Materials Science · Physics 2009-11-13 S. Sharma , S. Pittalis , S. Kurth , S. Shallcross , J. K. Dewhurst , E. K. U. Gross

The possibility of finding multistability in the density and current of an interacting nanoscale junction coupled to semi-infinite leads is studied at various levels of approximation. The system is driven out of equilibrium by an external…

Mesoscale and Nanoscale Physics · Physics 2015-06-03 E. Khosravi , A. -M. Uimonen , A. Stan , G. Stefanucci , S. Kurth , R. van Leeuwen , E. K. U. Gross

This note summarizes the motivation for extending current density-functional theory to include nonlocal one-electron potentials, and proposes methodology for practical calculations. The theoretical model, orbital functional theory, has been…

Condensed Matter · Physics 2007-05-23 R. K. Nesbet

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

An exchange-correlation energy functional $ E_{\mathrm xc} $ and the resultant exchange-correlation potential $ v_{\mathrm xc}({\bf r}) $ in density-functional theory are proposed using orbital-dependent coupling-constant-averaged pair…

Strongly Correlated Electrons · Physics 2007-05-23 Hiroshi Yasuhara , Masahiko Higuchi , Yoshiyuki Kawazoe

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