Title: High-power femtosecond molecular broadening and the effects of ro-vibrational coupling

Abstract: Scaling spectral broadening to higher pulse energies and average powers, respectively, is a critical step in ultrafast science, especially for narrowband Yb based solid state lasers which become the new state of the art. Despite their high nonlinearity, molecular gases as the broadening medium inside hollow core fibers have been limited to 25 W, at best. We demonstrate spectral broadening in nitrogen at ten-fold average powers up to 250W with repetition rates from 25 to 200kHz. The observed ten-fold spectral broadening is stronger compared to the more expensive krypton gas and enables pulse compression from 1.3ps to 120fs. We identified an intuitive explanation for the observed average power scaling based on the density of molecular ro vibrational states of Raman active molecules. To verify this ansatz, spectral broadening limitations in O2 and N2O are experimentally measured and agree well. On these grounds we propose a new perspective on the role, suitability, and limits of stimulated Raman scattering at high average and peak powers. Finally, high harmonic generation is demonstrated at 200 kHz.