High-Harmonic Spectroscopy of Charge Migration Simulated with TDDFT

Attosecond spectroscopic tools are now offering perspectives for measuring ultrafast coherent electron dynamics in molecules, such as charge migration, on their natural timescale. However, the corresponding numerical simulations remain extremely challenging since they require both an accurate description of the correlated electron/hole dynamics as well as the associated spectroscopic signals themselves. In this talk, I will present the results of recent high-harmonic-spectroscopy simulations using real-space TDDFT. I will discuss how these harmonic-spectroscopy simulations can be applied to molecular systems that undergo charge migration. Specifically, using the example of a conjugated halogenated alkyne linear molecule, I will show how periodic charge-migration motions in the molecule's pi system shape the harmonic-generation signal. Finally, I will discuss possible implications of these signatures for experimental measurements of molecular charge migration.