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With the help of femtosecond pulse shaping techniques, nonperturbative (resonant) light matter interactions can be implemented on the time scale of electron dynamics. In addition positive and negative Stark shifts in the order of 100 meV can be achieved. Nonperturbative interactions are also the basis for efficient and (if adiabatic) robust population transfer to excited states [1].
In the talk I will discuss two different experiments along this line:
i) In a gas phase experiment on K2 I will demonstrate and discuss that the coupled electron and nuclear dynamics of a molecule is efficiently steered by controlling the interplay of a driving femtosecond laser pulse with the photoinduced charge oscillation. These oscillations have a typical Bohr period of around 1 fs for valence electrons; therefore, control has to be exerted on a shorter time scale. The presented strong-field coherent control mechanism is understood in terms of a simple classical picture and at the same time verified by solving the time-dependent Schroedinger equation [2].
ii) In a liquid phase experiment on a sensitizer dye molecule I will demonstrate efficient population transfer and discuss joint motion of ground and excited state vibrational wave packets as well as population of a vibrational eigenstate as a building block for adiabatic population transfer. This approach permits us to discuss the molecular dynamics in an atom-like picture [3].
As a perspective I will shortly present our results on chiral recognition in the gas phase [4].
1. M. Wollenhaupt and T. Baumert, Faraday Discuss 153, 9 (2011).
2. T. Bayer et al., Phys Rev Lett 110, 123003 (2013).
3. J. Schneider et al., Phys Chem Chem Phys 13, 8733 (2011).
4. C. Lux et al. Angewandte Chemie International Edition 51, 5001 (2012).
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