Multiple-Pulse Control of Rotational Wavepackets in Molecules

Kevin F. Lee, P. W. Dooley
(Steacie Institute for Molecular Sciences, National Research Council of Canada and Department of Physics and Astronomy, McMaster University),

I. V Litvinyuk
(Department of Physics, Kansas State University),

D. M. Villeneuve, P. B. Corkum
(Steacie Institute for Molecular Sciences, National Research Council of Canada)

Field-free aligned molecules are now being used in novel experiments ranging from recoil electron diffraction to electronic state tomography and high harmonic generation. These experiments use a single short laser pulse to create rotational wavepackets in molecules. This is a nonresonant, strong-field effect which only rotates the molecules, leading to periodically recurring instances of field-free molecular alignment. We show that a second laser pulse can controllably modify the normal evolution of a rotational wavepacket. Depending on the timing and intensity of the pulses, the following revivals in alignment can be enhanced or suppressed.

This work was supported by the Chemical Sciences, Geosciences and Biosciences Division,
Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy.

Submitted to DAMOP, May 2004 in Tucson, AZ.

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