Stuttgart 2012 – scientific programme

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MO: Fachverband Molekülphysik

MO 6: Femtosecond Spectroscopy I

MO 6.8: Talk

Monday, March 12, 2012, 18:15–18:30, V38.03

Efficient sub-cycle control of electron dynamics in molecules — •Hendrike Braun¹, Tim Bayer¹, Cristian Sarpe¹, Robert Siemering², Philipp von den Hoff², Regina de Vivie-Riedle², Matthias Wollenhaupt¹, and Thomas Baumert¹ — ¹University of Kassel, Institute of Physics and CINSaT, D-34132 Kassel, Germany — ²Ludwig-Maximilians-Universität München, Departement Chemie, D-81377 München, Germany

Shaped femtosecond laser pulses are a well established tool to control the dynamics of the nuclei within a molecule after electronic excitation. Here we demonstrate that the electron dynamics of a molecule can also be efficiently manipulated by controlling the temporal phase of a femtosecond laser pulse. Specifically, we show how temporal phase changes on the time scale of the electron motion, i.e. with sub-cycle precision, are used to manipulate the electron dynamics of molecules and eventually switch between different potential energy surfaces of the molecule. The underlying control mechanism is termed SPODS (Selective Population of Dressed States) and has already been demonstrated on atoms [1,2,3]. It relies on the resonant excitation of an electronic coherence and subcycle control of the phase relation of the corresponding electric dipole and the strong light field. Extension to molecular systems shows the prospect of various applications of SPODS in femtochemistry.

[1] M. Wollenhaupt et al., Phys. Rev. A 68, 0154011 (2003)

[2] M. Wollenhaupt et al., Phys. Rev. A 73, 063409-1 (2006)

[3] T. Bayer et al., Phys. Rev. Lett. 102, 023004 (2009)

[4] M. Wollenhaupt et al., JPPA 180, 248 (2006)