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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

It was recently shown [Y. Suzuki, L. Lacombe, K. Watanabe, and N. T. Maitra, Phys. Rev. Lett. 119, 263401 (2017)] that peak and valley structures in the exact exchange-correlation potential of time-dependent density functional theory are…

Chemical Physics · Physics 2018-07-04 Lionel Lacombe , Yasumitsu Suzuki , Kazuyuki Watanabe , Neepa T. Maitra

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

We investigate the possibility to deduce momentum space properties from time-dependent density functional calculations. Electron and ion momentum distributions after double ionization of a model Helium atom in a strong few-cycle laser pulse…

Atomic Physics · Physics 2009-11-13 F. Wilken , D. Bauer

Time-dependent (current) density functional theory for many-electron systems strongly coupled to quantized electromagnetic modes of a microcavity is proposed. It is shown that the electron-photon wave function is a unique functional of the…

Mesoscale and Nanoscale Physics · Physics 2013-12-10 I. V. Tokatly

The real-time electronic dynamics on material surfaces is critically important to a variety of applications. However, their simulations have remained challenging for conventional methods such as the time-dependent density-functional theory…

Chemical Physics · Physics 2015-06-16 Rulin Wang , Dong Hou , Xiao Zheng

Phase shifts for single-channel elastic electron-atom scattering are derived from time-dependent density functional theory. The H$^-$ ion is placed in a spherical box, its discrete spectrum found, and phase shifts deduced. Exact-exchange…

Materials Science · Physics 2009-11-13 Meta van Faassen , Adam Wasserman , Eberhard Engel , Fan Zhang , Kieron Burke

Given the time-evolution of an electron charge density, the local potential in Kohn-Sham time-dependent density functional theory (KS-TDDFT) can be modeled as a sum of instantaneous and dynamic contributions by assuming a certain form of…

Computational Physics · Physics 2016-11-09 R. J. Magyar

The atomistic resolution recently achieved by ultrafast spectroscopies demands corresponding theoretical advances. Real-time time-dependent density-functional theory (RT-TDDFT) with Ehrenfest dynamics offers an optimal trade-off between…

Materials Science · Physics 2022-10-19 Jannis Krumland , Matheus Jacobs , Caterina Cocchi

Most present applications of time-dependent density functional theory use adiabatic functionals, i.e. the effective potential at time t is determined solely by the density at the same time. This paper discusses a method that aims to go…

Strongly Correlated Electrons · Physics 2009-11-10 Yair Kurzweil , Roi Baer

We propose a way to improve energy density functionals (EDFs) in the density functional theory based on the combination of the inverse Kohn--Sham method and the density functional perturbation theory. Difference between the known EDF and…

Chemical Physics · Physics 2019-11-22 Tomoya Naito , Daisuke Ohashi , Haozhao Liang

An efficient algorithm for time propagation of the time-dependent Kohn-Sham equations is presented. The algorithm is based on dividing the Hamiltonian into small time steps and assuming that it is constant over these steps. This allows for…

Computational Physics · Physics 2014-12-03 J. K. Dewhurst , K. Krieger , S. Sharma , E. K. U. Gross

Real-time time-dependent density functional theory, in conjunction with the Ehrenfest molecular dynamics scheme, is becoming a popular methodology to investigate ultrafast phenomena on the nanoscale. Thanks to recent developments, it is…

Materials Science · Physics 2020-08-18 Jannis Krumland , Ana M. Valencia , Stefano Pittalis , Carlo A. Rozzi , Caterina Cocchi

By inverting the time-dependent Kohn-Sham equation for a numerically exact dynamics of the helium atom, we show that the dynamical step and peak features of the exact correlation potential found previously in one-dimensional models persist…

Chemical Physics · Physics 2022-07-28 Davood Dar , Lionel Lacombe , Johannes Feist , Neepa Maitra

We introduce a new functional for simulating ground-state and time-dependent electronic systems within density-functional theory. The functional combines an expression for the exact Kohn-Sham (KS) potential in the limit of complete electron…

Mesoscale and Nanoscale Physics · Physics 2021-01-15 M. J. P. Hodgson , J. D. Ramsden , T. R. Durrant , R. W. Godby

This chapter provides a basic introduction to excited-state extensions of density functional theory (DFT), including time-dependent (TD-)DFT in both its linear-response and its explicitly time-dependent formulations. As applied to the…

Chemical Physics · Physics 2023-05-02 John M. Herbert

Due to a beneficial balance of computational cost and accuracy, real-time time-dependent density functional theory has emerged as a promising first-principles framework to describe electron real-time dynamics. Here we discuss recent…

The Kohn-Sham approach to time-dependent density-functional theory (TDDFT) can be formulated, in principle exactly, by invoking the force-balance equation for the density, which leads to an explicit expression for the exchange-correlation…

Chemical Physics · Physics 2021-09-15 Walter Tarantino , Carsten A. Ullrich

Reliable and robust convergence to the electronic ground state within density functional theory (DFT) Kohn-Sham (KS) calculations remains a thorny issue in many systems of interest. In such cases, charge sloshing can delay or completely…

Computational Physics · Physics 2020-04-07 Cedric Flamant , Grigory Kolesov , Efstratios Manousakis , Efthimios Kaxiras

We discuss two problems which are particularly challenging for approximations in time-dependent density functional theory (TDDFT) to capture: momentum-distributions in ionization processes, and memory-dependence in real-time dynamics. We…

Materials Science · Physics 2010-03-22 Arun K. Rajam , Paul Hessler , Christian Gaun , Neepa T. Maitra
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