Manipulating ultrafast charge migration in molecules with light

Exposing molecules to ultrashort pulses results typically in a coherent population of several and even many electronic states. This triggers ultrafast electron dynamics, which may lead to a redistribution of the charge even before the nuclei start to move and adjust – a process often referred to as charge migration [1,2]. The non-adiabatic coupling between the electronic and nuclear motion will eventually destroy the initial electronic coherence and trap the migrating charge. The time during which the electron coherence is maintained is an important parameter. This time can be used to modulate the charge migration process and thus predetermine the succeeding nuclear rearrangement in the molecule – the paradigm of the emerging field of attochemistry. In this talk, quantum simulations of ultrafast charge migration dynamics in polyatomic molecules [3-5] will be presented, and the possibility for a laser control of the electron-coherence time [6] and the effect of optical cavity will be discussed.

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[1] L. S. Cederbaum and J. Zobeley, Chem. Phys. Lett. 307, 205 (1999).

[2] A. I. Kuleff and L. S. Cederbaum, J. Phys. B 47, 124002 (2014).

[3] V. Despré, N. V. Golubev, and A. I. Kuleff, Phys. Rev. Lett. 121, 203002 (2018).

[4] N. V. Golubev, J. Vaníček, and A. I. Kuleff, Phys. Rev. Lett. 127, 123001 (2021).

[5] D. T. Matselyukh, V. Despré, N. V. Golubev, A. I. Kuleff, and H. J. Wörner, Nature Phys. 18, 1206 (2022).

[6] D. Dey, A. I. Kuleff, and G. A. Worth, Phys. Rev. Lett. 129, 173203 (2022).