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This study investigates attosecond charge migration (ACM) in molecular ions using high-level correlated methods to simulate purely electronic dynamics induced by hole-mixing. The research reveals that the presence of an initial charge on a molecule can either enhance or diminish the likelihood of observing ACM. Furthermore, the existence of ACM is found to be correlated with the strength of electron correlation within the molecule.
Molecular ions can exhibit either enhanced or suppressed attosecond electron dynamics compared to their neutral counterparts, challenging the assumption that charge migration predictions from neutral species directly translate to charged molecules.
Attosecond chemistry involves developing strategies to manipulate electronic coherent waves in molecules, which can influence the outcome of photoinduced reactions. While recent progress in this field calls for investigations of increasingly complex isolated or embedded systems, theoretical predictions on attosecond charge migration have remained limited to native neutral species. Since molecules in nature often carry a native charge, there is potential biological and chemical interest in determining whether attosecond charge migration is affected by an additional charge. In this study, we employ high-level correlated methods to study purely electronic dynamics induced by hole-mixing in molecular ions. Our results, obtained for a series of neutral, protonated and deprotonated molecules, reveal that the likelihood of observing attosecond electron dynamics can either be degraded or improved by the presence of an initial charge, and that the existence of the dynamics is correlated with the strength of electron correlation. These findings will stimulate further experimental and theoretical investigations into this unexplored field of attosecond dynamics in molecular ions.