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Attosecond Charge Migration with TDDFT: Accurate Dynamics from a Well Defined Initial State

Banff International Research Station for Mathematical Innovation and Discovery

We investigate the ability of time-dependent density functional theory (TDDFT) to capture attosecond valence electron dynamics resulting from sudden X-ray ionization of a core electron. In this special case the initial state can be constructed unambiguously, allowing for a simple test of the accuracy of the dynamics. The response following nitrogen K-edge ionization in nitrosobenzene shows excellent agreement with fourth order algebraic diagrammatic construction (ADC(4)) results, suggesting that a properly chosen initial state allows TDDFT to adequately capture attosecond charge migration. Visualizing hole motion using an electron localization picture (ELF), we provide an intuitive chemical interpretation of the charge migration as a time-dependent superposition of Lewis-dot resonance structures. Coupled with the initial state solution to obtain such dynamics with TDDFT, this chemical picture facilitates interpretation of electron .

Mathematics; Quantum theory; Optics, electromagnetic theory; Mathematical physics

video/mp4

Author affiliation: Louisiana State University

2019-03-06

Attribution-NonCommercial-NoDerivatives 4.0 International

http://hdl.handle.net/2429/68494

Unreviewed

http://creativecommons.org/licenses/by-nc-nd/4.0/