Ultrafast intermodal third harmonic generation in a liquid core step-index fiber filled with C₂Cl₄

Third harmonic generation in a circular liquid core step-index fiber filled with a highly transparent inorganic solvent is demonstrated experimentally using ultrafast pump pulses of different durations in the telecom domain for the first time. Specifically we achieve intermodal phase matching to the HE₁₃ higher order mode at the harmonic wavelength and found clear indications of a non-instantaneous molecular contribution to the total nonlinearity in the spectral broadening of the pump. Spectral power evolution and efficiency of the conversion process is studied for all pulse parameters, while we found the greatest photon yield for the longest pulses as well as an unexpected blue-shift of the third harmonic wavelength with increasing pump power. Our results provide the basis for future studies aiming at using this tunable fiber platform with a sophisticated nonlinear response in the context of harmonic generation.