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Extreme ultraviolet frequency combs are a versatile tool with applicationsincluding precision measurement, strong-field physics, and solid-state physics.Here we report on an application of extreme ultraviolet frequency combs andtheir driving lasers for studying strong-field effects in molecular systems. Weperform field-free molecular alignment and high-order harmonic generation withaligned molecules in a gas jet at a repetition rate of 154 MHz using ahigh-powered optical frequency comb inside a femtosecond enhancement cavity.The cavity-enhanced system provides a means to reach suitable intensities tostudy field-free molecular alignment and enhance the observable effects of themolecule-field interaction. We observe modulations of the driving field,arising from the nature of impulsive stimulated Raman scattering responsiblefor coherent molecular rotations. We foresee the impact of this work on thestudy of molecule-based strong-field physics, with improved precision and amore fundamental understanding of the interaction effects on both the field andmolecules.

Cavity-enhanced field-free molecular alignment at a high repetition rate