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Electron Dynamics and Its Control in Molecules: From Diatomics to Larger Molecular Systems

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4 Author(s)
von den Hoff, P. ; Dept. of Chem., Ludwig-Maximilians-Univ., München, Germany ; Siemering, R. ; Kowalewski, M. ; de Vivie-Riedle, R.

Electrons and their dynamics are involved in bond breaking and formation; thus, the idea to steer chemical reactions by localization of electronic wavepackets seems natural. The formation of a localized electronic wavepacket requires the superposition of two or more appropriate electronic states through, e.g., an external electric field. The guiding of such an electronic wavepacket is only possible within the coherence time of the system. In theoretical studies, we elucidate the role of electron wavepacket motion for the control of molecular processes. We analyze three examples of electron wavepacket-driven processes with direct connection to already performed or ongoing experiments. From these examples, we extract the system requirements defining the time window for intramolecular electronic coherence and efficient control. With this knowledge, we derived an appropriate molecular configuration in a photoreaction of a polyatomic molecule where a control by guiding electronic wavepackets is possible. For such a photoreaction, we designed a new control scheme with the carrier envelope phase as a control parameter that works at high efficiency.

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Selected Topics in Quantum Electronics, IEEE Journal of  (Volume:18 ,  Issue: 1 )