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We demonstrate how the depleted pump of an optical parametric amplifier canbe recycled for impulsive alignment of a molecular gas inside a hollow-corefiber and use such alignment for the broadening and frequency shift of thesignal pulse at a center wavelength of $\sim 1300$nm. Our results combinenon-adiabatic molecular alignment, self-phase modulation and Ramannon-linearities. We demonstrate spectral shifts of up to 204 nm and a spectralbroadening of more than one octave. We also report on the time delays at whichbroadening occurs, which do not coincide with any of the molecular rotationalconstants. Further, we encounter that maximum frequency shifts occur when thesignal and pump have perpendicular polarization instead of parallel.

Molecular alignment-assisted spectral broadening and shifting in the  near-infrared with a recycled depleted pump from an optical parametric  amplifier