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Attochemistry Regulation of Charge Migration.

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  • 1Department of Physics, University of Virginia, Charlottesville, Virginia 22904, United States.

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Charge migration (CM) is a rapid electron hole movement across molecules. Functional group strength, measured by Hammett σ values, dictates the hole

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Area of Science:

  • Physical Chemistry
  • Quantum Chemistry
  • Attosecond Science

Background:

  • Charge migration (CM) describes coherent, attosecond-scale electron hole movement within molecules.
  • Understanding CM dynamics is crucial for predicting molecular behavior after ionization.

Purpose of the Study:

  • To investigate the relationship between molecular structure and charge migration dynamics.
  • To explore how functional groups influence the charge migration process in bromobenzene derivatives.

Main Methods:

  • Real-time time-dependent density functional theory (TD-DFT) was employed.
  • Systematic studies were performed on para-functionalized bromobenzene molecules (X-C6H4-R).
  • Valence-electron dynamics were initiated by emulating strong-field ionization, localizing a hole on bromine.

Main Results:

  • Charge migration occurs on a femtosecond timescale via a localized hole delocalization-relocalization mechanism.
  • The hole contrast on acceptor functional groups increases with electron-donating strength.
  • This trend correlates well with Hammett σ values, quantifying substituent effects.

Conclusions:

  • Attochemistry principles and density-based models can predict and explain charge migration dynamics.
  • Molecular functionalization significantly impacts the pathway and extent of charge migration.
  • The study provides insights into controlling ultrafast electron dynamics in molecules.