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The performance of time-independent, orbital optimized calculations of excited states is assessed with respect to charge transfer excitations in organic molecules in comparison to the linear-response time-dependent density functional theory…

Chemical Physics · Physics 2024-05-22 Elli Selenius , Alec Elías Sigurdarson , Yorick L. A. Schmerwitz , Gianluca Levi

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

Quantum optimal control theory is a powerful tool for engineering quantum systems subject to external fields such as the ones created by intense lasers. The formulation relies on a suitable definition for a target functional, that…

Quantum Physics · Physics 2015-05-20 David Kammerlander , Alberto Castro , Miguel A. L. Marques

Orbital-optimized density functional theory (DFT) has emerged as an alternative to time-dependent (TD) DFT capable of describing difficult excited states with significant electron density redistribution, such as charge-transfer, Rydberg,…

Chemical Physics · Physics 2025-01-22 Hanh D. M. Pham , Rustam Z. Khaliullin

We study ultrafast ionization dynamics using orthogonally polarized two-color (OTC) laser pulses involving the resonant "first plus second" ($\omega+2\omega$) scheme. The scheme is illustrated by numerical simulations of the time-dependent…

Atomic Physics · Physics 2019-12-16 Hicham Agueny

An approximate solution to the time-dependent density functional theory (TDDFT) response equations for finite systems is developed, yielding corrections to the single-pole approximation. These explain why allowed Kohn-Sham transition…

Materials Science · Physics 2009-11-07 H. Appel , E. K. U. Gross , K. Burke

We investigate the numerical stability of time-dependent coupled-cluster theory for many-electron dynamics in intense laser pulses, comparing two coupled-cluster formulations with full configuration interaction theory. Our numerical…

Time dependent quantum systems are the subject of intense inquiry, in mathematics, science, and engineering, particularly at the atomic and molecular levels. In 1984, Runge and Gross introduced time dependent density functional theory…

Analysis of PDEs · Mathematics 2021-02-24 Joseph W. Jerome

The exact exchange potential in time-dependent density-functional theory is defined as an orbital functional through the time-dependent optimized effective potential (TDOEP) method. We numerically solve the TDOEP integral equation for the…

Mesoscale and Nanoscale Physics · Physics 2009-11-13 H. O. Wijewardane , C. A. Ullrich

We present an implementation of optimal control theory for the first-principles non-adiabatic Ehrenfest Molecular Dynamics model, which describes a condensed matter system by considering classical point-particle nuclei, and quantum…

Atomic and Molecular Clusters · Physics 2017-02-27 Adrián Gómez Pueyo , Jorge A. Budagosky M. , Alberto Castro

Ultra-fast electronic phenomena originating from finite temperature, such as nonlinear optical excitation, can be simulated with high fidelity via real-time time dependent density functional theory (rt-TDDFT) calculations with hybrid…

Materials Science · Physics 2025-01-07 Rongrong Liu , Zhuoqiang Guo , Qiuchen Sha , Tong Zhao , Haibo Li , Wei Hu , Lijun Liu , Guangming Tan , Weile Jia

Time-dependent density functional theory (TDDFT) is a standard approach for calculating optical excitations of molecules and solids, while ensemble DFT (EDFT) is a promising alternative under development. We introduce ensemble TDDFT…

Chemical Physics · Physics 2026-05-22 Kimberly J. Daas , Steven Crisostomo , Kieron Burke

We present an implementation of time-dependent density-functional theory (TDDFT) in the linear response formalism enabling the calculation of low energy optical absorption spectra for large molecules and nanostructures. The method avoids…

Despite the variety of available computational approaches, state-of-the-art methods for calculating excitation energies such as time-dependent density functional theory (TDDFT), are computationally demanding and thus limited to moderate…

Chemical Physics · Physics 2022-03-10 Martina Stella , Kritam Thapa , Luigi Genovese , Laura E. Ratcliff

In this work we have studied a new functional for the correlation energy obtained from the exact-exchange (EXX) approximation within time-dependent density functional theory (TDDFT). Correlation energies have been calculated for a number of…

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

In ion irradiation processes, electronic stopping power describes the energy transfer rate from the irradiating ion to the target material's electrons. Due to the scarcity and significant uncertainties in experimental electronic stopping…

Materials Science · Physics 2018-05-04 Dillon C. Yost , Yi Yao , Yosuke Kanai

Using the Runge-Gross theorem that establishes the foundation of Time-dependent Density Functional Theory (TDDFT) we prove that for a given electronic Hamiltonian, choice of initial state, and choice of fragmentation, there is a unique…

Chemical Physics · Physics 2015-06-15 Martin A. Mosquera , Daniel Jensen , Adam Wasserman

A decade ago Rhie \et (Phys. Rev. Lett. {\bf 90}, 247201 (2003)) reported that when ferromagnetic nickel is subject to an intense ultrashort laser pulse, its exchange splitting is reduced quickly. But to simulate such reduction remains a…

Materials Science · Physics 2016-11-15 G. P. Zhang , Y. H. Bai , Thomas F. George

If one-electron observables of a many-electron system are of interest, a many-electron dynamics can be represented exactly by a one-electron dynamics with effective potentials. The formalism for this reduction is provided by the Exact…

Chemical Physics · Physics 2021-01-04 Jakub Kocák , Axel Schild

We review time-dependent multiconfiguration self-consistent-field (TD-MCSCF) method and time-dependent optimized coupled-cluster (TD-OCC) method for first-principles simulations of high-field phenomena such as tunneling ionization and…

Chemical Physics · Physics 2022-11-21 Takeshi Sato , Himadri Pathak , Yuki Orimo , Kenichi L. Ishikawa
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