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While industrial-grade Yb-based amplifiers have become very prevalent, their limited gain bandwidth has created a large demand for robust spectral broadening techniques that allow for few-cycle pulse compression. In this work, we perform a comparative study between several atomic and molecular gases as media for spectral broadening in a hollow-core fiber geometry. Exploiting nonlinearities such as self-phase modulation, self-steepening, and stimulated Raman scattering, we explore the extent of spectral broadening and its dependence on gas pressure, the critical power for self-focusing, and the optimal regime for few-cycle pulse compression. Using a 3-mJ, 200-fs input laser pulses, we achieve 17 fs, few-cycle pulses with 80% fiber energy transmission efficiency. The optimal parameters can be scaled for higher or lower input pulse energies with appropriate gas parameters and fiber geometry. 

Abstract Metrology of electron wavepackets is often conducted with the technique of photoelectron interferometry. However, the ultrashort light pulses employed in this method place a limit on the energy resolution. Here, weadvance ultrafast photoelectron interferometry access both high temporal and spectral resolution. The key to our approach lies in stimulating Raman interferences with a probe pulse and while monitoring the modification of the autoionizing electron yield in a separate delayed detection step. As a proof of the principle, we demonstrated this technique to obtain the components of an autoionizing nf′ wavepacket between the spin-orbit split ionization thresholds in argon. We extracted the amplitudes and phases from the interferogram and compared the experimental results with second-order perturbation theory calculations. This high resolution probing and metrology of electron dynamics opens the path for study of molecular wavepackets.