Coherent Control of Quantum Phenomena Using Shaped UV Pulses

Marcus Motzkus
Philipps-Universität Marburg

Coherent control of quantum phenomena aims at steering molecular systems into specific product states or optimizing the performance of nonlinear optical processes by adjusting the phases of multiple quantum pathways to different product channels via adapted excitation light.[1] Many successful demonstrations of this approach on a multitude of atomic and molecular systems have been presented in the last few years. It has been even shown that coherent control can be exercised on biological samples, as demonstrated in the control of the energy flow in the LH2 antenna complex.[2,3] These studies illustrate that coherent control effected by a combination of open and closed loop experiments is well suited to uncover the structure and dynamics of complex molecules. Almost all of the these control experiments have been performed so far with laser pulses in the visible or near infrared spectral region, mainly because of the less operative expense for the generation of high pulse energies and the lack of modulators for the extended spectral regions. One way to circumvent this problem takes advantage of nonlinear optical mixing processes which generates the shaped light in an indirect process. However, novel adaptive micromirrors offer even the possibility to directly generate arbitrarily shaped pulses [3] and allow for coherent control experiments on important organic chemical and biological systems which typically have absorption spectra below 400 nm. Furthermore, the availability of shaped pulses in the UV offers new approaches to the control of electronic responses of atoms and molecules.

[1] H. Rabitz, R. deVivie-Riedle, M. Motzkus, and K.-L. Kompa, Science 288 (2000) 824.
[2] J.L. Herek, W. Wohlleben, R. Cogdell, D. Zeidler, and M. Motzkus, Nature 417 (2002) 533.
[3] Wohlleben, T. Buckup, J.L. Herek, and M. Motzkus, ChemPhysChem 6 (2005) 850.
[4] M. Hacker, G. Stobrawa, R. Sauerbrey, T. Buckup, M. Motzkus, M. Wildenhain, A. Gehner, Appl. Phys. B 76 (2003) 711.