The steering of electron motion in molecules is accessible with waveform-controlled few-cycle laser light and may control the outcome of light-induced chemical reactions. An optical cycle of light, however, is much shorter than the duration of the fastest dissociation reactions, severely limiting the degree of control that can be achieved. To overcome this limitation, we extended the control metrology to the midinfrared studying the prototypical dissociative ionization of D(2) at 2.1 μm. Pronounced subcycle control of the directional D(+) ion emission from the fragmentation of D(2)(+) is observed, demonstrating unprecedented charge-directed reactivity. Two reaction pathways, showing directional ion emission, could be observed and controlled simultaneously for the first time. Quantum-dynamical calculations elucidate the dissociation channels, their observed phase relation, and the control mechanisms.

We produce carrier-envelope-phase-stable 15.7-fs (2-cycle) 740-microJ pulses at the 2.1-microm carrier wavelength, from a three-stage optical parametric chirped-pulse amplifier system, pumped by an optically synchronized 49-ps 11-mJ Nd:YLF laser. A novel seed pulse spectral shaping method is used to ascertain the true amplified seed energy and the parametric superfluorescence levels.

We produce 1.5 cycle (10.5 fs), 1.2 mJ, 3 kHz carrier-envelope-phase-stable pulses at 2.1 μm carrier wavelength, from a three-stage optical parametric chirped-pulse amplifier system, pumped by an optically synchronized 1.6 ps Yb:YAG thin disk laser. A chirped periodically poled lithium niobate crystal is used to generate the ultrabroad spectrum needed for a 1.5 cycle pulse through difference frequency mixing of spectrally broadened pulse from a Ti:sapphire amplifier. It will be an ideal tool for producing isolated attosecond pulses with high photon energies.

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