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Related Experiment Video

Updated: Feb 25, 2026

All-electronic Nanosecond-resolved Scanning Tunneling Microscopy: Facilitating the Investigation of Single Dopant Charge Dynamics
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Attosecond Charge Migration with TDDFT: Accurate Dynamics from a Well-Defined Initial State.

Adam Bruner1, Samuel Hernandez1, François Mauger2

  • 1Department of Chemistry, Louisiana State University , Baton Rouge, Louisiana 70803, United States.

The Journal of Physical Chemistry Letters
|August 10, 2017
PubMed
Summary

Time-dependent density functional theory (TDDFT) accurately captures attosecond electron dynamics after X-ray ionization. This method provides a reliable way to study ultrafast charge migration in molecules.

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Area of Science:

  • Quantum Chemistry
  • Attosecond Science
  • Computational Physics

Background:

  • Ultrafast electron dynamics are crucial for understanding chemical reactions.
  • Accurate theoretical methods are needed to model these dynamics.
  • Core electron ionization provides a unique starting point for studying electron response.

Purpose of the Study:

  • To evaluate the accuracy of time-dependent density functional theory (TDDFT) for attosecond valence electron dynamics.
  • To investigate charge migration following core electron ionization.
  • To provide a chemical interpretation of electron hole motion.

Main Methods:

  • Simulating X-ray ionization of nitrosobenzene at the nitrogen K-edge.
  • Employing time-dependent density functional theory (TDDFT).
  • Comparing TDDFT results with fourth-order algebraic diagrammatic construction (ADC(4)).
  • Utilizing the electron localization function (ELF) to visualize hole motion.

Main Results:

  • TDDFT accurately captures attosecond valence electron dynamics after core ionization.
  • Excellent agreement was found between TDDFT and ADC(4) calculations.
  • Electron localization function (ELF) analysis revealed charge migration as a superposition of resonance structures.

Conclusions:

  • TDDFT is a suitable method for studying attosecond charge migration dynamics.
  • A well-defined initial state is key for accurate TDDFT simulations.
  • The study offers an intuitive chemical picture of ultrafast electronic processes.