Non-perturbative generation of DUV/VUV harmonics from crystal surfaces at 108 MHz repetition rate

We demonstrate non-perturbative 3rd (267 nm) and 5th (160 nm) harmonic generation in solids from a Ti:sapphire frequency comb (800 nm) at 108 MHz repetition rate. The experiments show that non-perturbative low harmonics are dominantly generated on the surface and on the interface between solids, and that they are not produced by bulk processes from the near-surface layer of the material. Measurements reveal that due to the lack of phase matching, the generated harmonics in bulk are suppressed by orders of magnitude compared to the signal generated on the surface. Our results pave the way for the development of all-solid-state high repetition rate harmonic sources for vacuum ultraviolet spectroscopy and high precision frequency comb metrology.