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Issue 19, 2011
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Efficient and robust strong-field control of population transfer in sensitizer dyes with designed femtosecond laser pulses

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Abstract

We demonstrate control of electronic population transfer in molecules with the help of appropriately shaped femtosecond laser pulses. To this end we investigate two photosensitizer dyes in solution being prepared in the triplet ground state. Excitation within the triplet system is followed by intersystem crossing and the corresponding singlet fluorescence is monitored as a measure of population transfer in the triplet system. We record control landscapes with respect to the fluorescence intensity on both dyes by a systematic variation of laser pulse shapes combining second order and third order dispersion. In the strong-field regime we find highly structured topologies with large areas of maximum or minimum population transfer being insensitive over a certain range of applied laser intensities thus demonstrating robustness. We then compare our experimental results with simulations on generic molecular potentials by solving the time-dependent Schrödinger equation for excitation with shaped pulses. Control landscapes with respect to population transfer confirm the general trends from experiments. An analysis of regions with maximum or minimum population transfer indicates that coherent processes are responsible for the outcome of our excitation process. The physical mechanisms of joint motion of ground and excited state wave packets or population of a vibrational eigenstate in the excited state permit us to discuss the molecular dynamics in an atom-like picture.

Graphical abstract: Efficient and robust strong-field control of population transfer in sensitizer dyes with designed femtosecond laser pulses

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Publication details

The article was received on 30 Nov 2010, accepted on 01 Mar 2011 and first published on 25 Mar 2011


Article type: Paper
DOI: 10.1039/C0CP02723E
Citation: Phys. Chem. Chem. Phys., 2011,13, 8733-8746
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    Efficient and robust strong-field control of population transfer in sensitizer dyes with designed femtosecond laser pulses

    J. Schneider, M. Wollenhaupt, A. Winzenburg, T. Bayer, J. Köhler, R. Faust and T. Baumert, Phys. Chem. Chem. Phys., 2011, 13, 8733
    DOI: 10.1039/C0CP02723E

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