Title
Attosecond Charge Migration with TDDFT: Accurate Dynamics from a Well-Defined Initial State
Document Type
Article
Publication Date
9-7-2017
Abstract
© 2017 American Chemical Society. 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 superposition of Lewis dot resonance structures.
Publication Source (Journal or Book title)
Journal of Physical Chemistry Letters
First Page
3991
Last Page
3996
Recommended Citation
Bruner, A., Hernandez, S., Mauger, F., Abanador, P., LaMaster, D., Gaarde, M., Schafer, K., & Lopata, K. (2017). Attosecond Charge Migration with TDDFT: Accurate Dynamics from a Well-Defined Initial State. Journal of Physical Chemistry Letters, 8 (17), 3991-3996. https://doi.org/10.1021/acs.jpclett.7b01652