Orateur
Description
Attosecond XUV pulses provide a powerful tool to trigger pure electron dynamics in molecules, such as the so-called cahrge migration [1,2]. While charge migration has been extensively studied in neutral molecules following ionization [3], its counterpart in pre-charged systems (molecular ions) remains largely unexplored. Such systems are ubiquitous in chemical and biochemical environments, and understanding their intrinsic electron dynamics offers new opportunities to control and probe electron correlation effects in realistic settings.
In this work, we investigate correlation-driven charge migration in molecular ions using non-Dyson algebraic diagrammatic construction [4] combined with multi-electronic wave-packet propagation [5]. We consider a series of systems with different native charges by examining protonated and deprotonated derivatives of molecules exhibiting strong outer-valence electron correlation (hole mixing).
Our results demonstrate that protonation and deprotonation affect outer-valence electronic structure and dynamics in markedly different ways. Protonation suppresses correlated dynamics by strongly altering the preferred ionization sites, whereas deprotonation reduces correlation strength while significantly accelerating charge migration. In both cases, these effects are rationalized in terms of the spatial distribution of the excess charge prior to ionization. Furthermore, comparison across different molecules suggests that systems with similar structures (geometry and functional groups) respond in a consistent manner to the added charge. These findings highlight how molecular charge state can be used to tailor electron correlation and ultrafast charge dynamics, opening new perspectives for the design of systems with controlled electronic behavior.
References:
[1] Cederbaum L. S., and Zobeley J., Chem. Phys. Lett. , Vol. 307, No. 3-4 (1999)
[2] Kuleff A. I., and Cederbaum, Lorenz S., J. Phys. B: At. Mol. Opt. Phys. , Vol. 47, No. 12 (2014)
[3] Calegari F. et al, J. Phys. B: At. Mol. Opt. Phys. , Vol. 49, No. 14 (2016)
[4] Schirmer J., Trofimov A. B., and Stelter G., J. Chem. Phys. , Vol. 109, No. 12 (1998)
[5] Kuleff A. I., Breidbach J., and Cederbaum L. S., J. Chem. Phys. , Vol. 123, No. 4 (2005)
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