Ultrabroadband supercontinuum and third-harmonic generation in bulk solids with two optical-cycle carrier-envelope phase-stable pulses at 2 μm.

We report on the generation of ultrabroadband supercontinuum (SC) by filamentation of two optical-cycle, carrier-envelope phase-stable pulses at 2 μm in fused silica, sapphire, CaF₂ and YAG. The SC spectra extend from 450 nm to more than 2500 nm, and their particular shapes depend on dispersive properties of the materials. Prior to spectral super-broadening, we observe third-harmonic generation, which occurs in the condition of large phase and group velocity mismatch and consists of free and driven components. A double-peaked third-harmonic structure coexists with the SC pulse as demonstrated by the numerical simulations and verified experimentally. The SC pulses have stable carrier envelope phase with short-term rms fluctuations of ∼ 300 mrad, as simultaneously measured in YAG crystal by f-2f and f-3f interferometry, where the latter makes use of intrinsic third-harmonic generation.