Enhancing High-Order Harmonic Generation in Light Molecules by Using Chirped Pulses

One of the current challenges in high-harmonic generation is to extend the harmonic cutoff to increasingly high energies while maintaining or even increasing the efficiency of the high-harmonic emission. Here we show that the combined effect of down-chirped pulses and nuclear dynamics in light molecules allows one to achieve this goal, provided that long enough IR pulses are used to allow the nuclei to move well outside the Franck-Condon region. We also show that, by varying the duration of the chirped pulse or by performing isotopic substitution while keeping the pulse duration constant, one can control the extension of the harmonic plateau.