The Interplay of Nuclear and Electron Wavepacket Motion in the Control of Molecular Processes: A Theoretical Perspective

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The concept of coherent control of molecular processes with light is introduced, sketching the way from single parameter to the multiparameter control in the time domain. Optimal control theory is by now a widespread and well-recognized method to solve a variety of control tasks ranging from chemical to physical applications. The underlying concepts and tools with their links to the experiment will be introduced with the focus on chemical reactions. As they include the motion of the nuclei, their time scale ranges from femtoseconds to picoseconds and longer and requires the solution of the time-dependent Schrodinger equation for the nuclear motion. Recent developments that enter the sub-femtosecond domain and open the prospect for direct control of the faster electron motion will be addressed. Two strategies—already realized experimentally—are presented: control of electron dynamics via the carrier envelope phase (CEP) in few-cycle pulses and via the temporal phase of a femtosecond laser pulse with attosecond precision. The issue of nuclear and electronic wavepacket synchronization to achieve control on a chemical reaction is raised. A theoretical method to answer these questions is presented. Finally, a proposal how the electron dynamics can be used as an additional control parameter for a chemical reaction is made.