We present an experimental demonstration of nonresonant manipulation of vibrational states in a molecule by an intense ultrashort laser pulse. A vibrational wave packet is generated in ${\mathrm{D}}_2{}^{+}$ through tunnel ionization of ${\mathrm{D}}_2$ by a few-cycle pump pulse. A similar control pulse is applied as the wave packet begins to dephase so that the dynamic Stark effect distorts the electronic environment of the nuclei, transferring vibrational population. The time evolution of the modified wave packet is probed via the ${\mathrm{D}}_2{}^{+}$ photodissociation yield that results from the application of an intense probe pulse. Comparing the measured yield with a quasiclassical trajectory model allows us to determine the redistribution of vibrational population caused by the control pulse.

• Received 3 November 2010

DOI:https://doi.org/10.1103/PhysRevA.83.021406

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