| 概 要 |
With attosecond pulses direct access to electron dynamics has become possible. We focus on the control of chemical reactions by steering electronic wavepackets where the synchronization of the slower nuclear wavepacket motion with the fast electron dynamics is of critical importance.
We developed an efficient approach, which exploits quantum dynamics and quantum chemistry in a new way to simultaneously describe the dynamics of nuclear and electron motion and allows for the treatment of multi-electron systems. We tested our method first for the photodissociation of D2+ to check against more rigorous theories [1,2] as well as experiments [3] and achieved excellent agreement. The same approach was used for the laser induced dissociation of the CO+ and the control via electronic wavepacket dynamics in K2. In CO+ the directional emission of the ionic fragments is controllable via the carrier-envelope phase. These results compare well with recent experiments from the Kling group [4] and are encouraging for the prospects of electron control affecting molecular reactions. In K2 we could show that the implementation of SPODS (selective population of dressed states), developed in the Kassel group [5] should be successful also in molecules.
[1] J. Levesque, S. Chelkowski and A. Bandrauk J. Mod. Opt. 50, 497 (2003).
[2] X. M. Tong and C. D. Lin Phys. Rev. Lett. 98, 123002 (2007).
[3] M. F. Kling, C. Siedschlag, A. J. Verhoef, J. I. Khan, M. Schultze, T.Uphues, Y. Ni, M. Uiberacker, M. Drescher, F. Krausz and M. J. J. Vrakking Science 312, 246 (2006).
[4] I. Znakovskaya, P. von den Hoff, S. Zherebtsov, A. Wirth, O. Herrwerth, M. J. J. Vrakking, R. de Vivie-Riedle, and M. F. Kling Phys. Rev. Lett. 103, 103002 (2009).
[5] M. Wollenhaupt, A. Pr¨akelt, C. Sarpe-Tudoran, D. Liese, T. Baumert, Appl. Phys. B 82, 183 (2006).
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