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The use of strong-field (i.e. intensities in excess of 10^13 Wcm-2) few-cycleultrafast (durations of 10 femtoseconds or less) laser pulses to create,manipulate and image vibrational wavepackets is investigated. Quasi-classicalmodelling of the initial superposition through tunnel ionization, wavepacketmodification by nonadiabatically altering the nuclear environment via thetransition dipole and the Stark effect, and measuring the control outcome byfragmenting the molecule is detailed. The influence of the laser intensity onstrong-field ultrafast wavepacket control is discussed in detail: by modifyingthe distribution of laser intensities imaged, we show that focal conditions canbe created that give preference to this three-pulse technique above processesinduced by the pulses alone. An experimental demonstration is presented, andthe nuclear dynamics inferred by the quasi-classical model discussed. Finally,we present the results of a systematic investigation of a dual-control pulsescheme, indicating that single vibrational states should be observable withhigh fidelity, and the populated state defined by varying the arrival time ofthe two control pulses. The relevance of such strong-field coherent controlmethods to the manipulation of electron localization and attosecond science isdiscussed.

Controlled redistribution of vibrational population by few-cycle strong-field laser pulses