ECAMP 15

In a molecular system, the correlation-driven charge migration [1] (CDCM) is a purely electronic process that involves the ultrafast dynamics of electrons originating from coherent superposition of eigenstates followed by the ionization of a single molecular orbital [2]. The possibility of observing CDCM has been a driving force behind theoretical and experimental developments in the field of attosecond molecular science since its inception. Although X-ray free-electron lasers (XFELs) have recently emerged as a promising tool for experimentally observing CDCM, the unambiguous observation of CDCM, or more generally, charge migration dynamics triggered by ionization, remains elusive. In this work [3], we present a method to selectively trigger such dynamics using molecules predicted to exhibit long-lived electron coherence. We show that these dynamics can be selectively triggered using infrared multi-photon ionization and probed using the spacial resolution of X-ray free-electron laser, proposing a promising experimental scheme to study these pivotal dynamics. Additionally, we demonstrate that real-time time-dependent density-functional theory can describe correlation-driven charge migration resulting from a hole-mixing structure involving the HOMO of a molecule.

References
[1] A. I. Kuleff, L. S. Cederbaum, J. Phys. B: At. Mol. Opt. Phys., 47(12), 124002, (2014).
[2] J. Breidbach, L. S. Cederbaum, J. Chem. Phys., 118(9), 3983, (2003)
[3] C. Guiot du Doignon, R. Sinha-Roy, F. Rabilloud, V. Despré, arXiv:2410.04978, (2024)