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The general expectation that, in principle, time-dependent density functional theory (TDDFT) be an exact formulation of the time-evolution of an interacting N-electron system is critically reexamined. It is demonstrated that the previous…

Other Condensed Matter · Physics 2007-08-13 J. Schirmer , A. Dreuw

Linear-response time-dependent (TD) density-functional theory (DFT) has been implemented in the pseudopotential wavelet-based electronic structure program BigDFT and results are compared against those obtained with the all-electron…

Spectroscopic properties of molecules holds great importance for the description of the molecular response under the effect of an UV/Vis electromagnetic radiation. Computationally expensive ab initio (e.g. MultiConfigurational SCF, Coupled…

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

Time-dependent density functional theory (TDDFT) simulations of transient core-level spectroscopies require a balanced treatment of both valence- and core-electron excitations. To this end, tuned range-separated hybrid exchange-correlation…

Materials Science · Physics 2020-06-04 C. D. Pemmaraju

We propose a computationally efficient approach to the nonadiabatic time-dependent density functional theory (TDDFT) which is based on a representation of the frequency-dependent exchange correlation kernel as a response of a set of damped…

Mesoscale and Nanoscale Physics · Physics 2019-12-18 Dmitry R. Gulevich , Yaroslav V. Zhumagulov , Alexei V. Vagov , Vasili Perebeinos

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

Systems whose underlying classical dynamics are chaotic exhibit signatures of the chaos in their quantum mechanics. We investigate the possibility of using time-dependent density functional theory (TDDFT) to study the case when chaos is…

Other Condensed Matter · Physics 2009-11-13 Adam Wasserman , Neepa T. Maitra , Eric J. Heller

Energy transfer processes from a high-intensity ultrashort laser pulse to electrons in simple dielectrics, silicon, diamond, and $\alpha$-quartz are theoretically investigated by first-principles calculations based on time-dependent density…

Optics · Physics 2019-05-22 Atsushi Yamada , Kazuhiro Yabana

In principle, we should not need the time-dependent extension of density-functional theory (TDDFT) for excitations, and in particular not for Molecular Dynamics (MD) studies: the theorem by Hohenberg and Kohn teaches us that for any…

Strongly Correlated Electrons · Physics 2015-05-27 J. L. Alonso , Alberto Castro , Pablo Echenique , Angel Rubio

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

The formalism of density functional theory (DFT) can be easily extended to the time dependent case (TDDFT). However, while in the static case the theory is well established and is expected to be, at least in principle, an exact approach for…

Condensed Matter · Physics 2007-05-23 Sandro Stringari

The time-dependent density functional theory (TDDFT) is the leading computationally feasible theory to treat excitations by strong electromagnetic fields. Here the theory is applied to coherent optical phonon generation produced by intense…

Materials Science · Physics 2015-06-05 Y. Shinohara , S. A. Sato , K. Yabana , J. -I. Iwata , T. Otobe , G. F. Bertsch

Time-dependent density-functional theory (TDDFT) treats dynamical exchange and correlation (xc) via a single-particle potential, Vxc(r,t), defined as a nonlocal functional of the density n(r',t'). The popular adiabatic local-density…

Mesoscale and Nanoscale Physics · Physics 2009-11-11 C. A. Ullrich , I. V. Tokatly

We show that by nullifying the short-wave response to the long-wave excitation (local-field-effects), the adiabatic time-dependent density-functional theory (TDDFT) of optics of semiconductors and insulators can be brought into excellent…

Materials Science · Physics 2013-08-15 V. U. Nazarov , S. Kais

An atomic-orbital basis set framework is presented for carrying out velocity- gauge real-time time-dependent density functional theory (TDDFT) simulations in periodic systems employing range-separated hybrid functionals. Linear optical…

Materials Science · Physics 2018-10-02 C. D. Pemmaraju

To examine the applicability of the time-dependent density-functional theory (TDDFT) for treating the electron-nucleus coupling in excited states, we calculate the strength distribution associated with the pi-pi* transition in ethylene. The…

Chemical Physics · Physics 2007-05-23 G. F. Bertsch , J. Giansiracusa , K. Yabana

The development of analytic-gradient methodology for excited states within conventional time-dependent density-functional theory (TDDFT) would seem to offer a relatively inexpensive alternative to better established quantum-chemical…

Other Condensed Matter · Physics 2010-08-11 Felipe Cordova , L. Joubert Doriol , Andrei Ipatov , Mark E. Casida , Claudia Filippi , Alberto Vela

We prove the existence of the exact density-functional theory formalism for open electronic systems, and develop subsequently an exact time-dependent density-functional theory (TDDFT) formulation for the dynamic response. The TDDFT…

Chemical Physics · Physics 2007-05-23 Xiao Zheng , GuanHua Chen

We investigate plasmon-assisted photoelectron emission using a one-dimensional time-dependent density-functional theory (TDDFT) model. Photoelectron spectra are computed with the time-dependent surface-flux (t-SURFF) method. In addition to…

Quantum Physics · Physics 2025-10-14 Mikhail Bednov , Waqas Pervez , Ingo Barke , Dieter Bauer