We report on the direct experimental observation of pulse-splitting dynamics along a femtosecond filament. The fundamental pulse experiences a significant self-shortening during the propagation leading to pulse durations of 5.3 fs, corresponding to sub-3 cycles, which is measured without external pulse compression. A compression factor of eight could be achieved in a single filamentary stage. Theoretical modeling of the fundamental pulse propagation confirms our observed pulse structures and durations and gives further insight into the nonlinear dynamics during filamentation.

We demonstrate a dispersion scan (d-scan) pulse characterization scheme employing cross-polarized wave (XPW) generation as a nonlinear optical process. XPW generation is a degenerate four-wave mixing process with no phase-matching limitations. Therefore, its implementation in the d-scan method is a good choice for the characterization of few-cycle pulses in remote spectral regions. We fully characterize 5-10 fs pulses delivered through a hollow-core fiber in the near-IR region and compare the results with the second-harmonic generation (SHG) frequency-resolved optical gating and SHG d-scan characterization methods.

High-order harmonic spectroscopy allows one to extract information on fundamental quantum processes, such as the exit time in the tunneling of an electron through a barrier with attosecond time resolution and molecular structure with angstrom spatial resolution. Here, we study the spatial motion of the electron during high-order harmonic generation in an in situ pump-probe measurement using highdensity liquid water droplets as a target. We show that molecules adjacent to the emitting electron-ion pair can disrupt the electron's trajectory when positioned within the range of the maximum electronic excursion distance. This allows us to use the parent ion and the neighboring molecules as boundaries for the electronic motion to measure the maximum electronic excursion distance during the high-order harmonic generation process. Our analysis of the process is relevant for optimizing high-harmonic yields in dense media.

We report on high-order-harmonic generation from micrometer-sized liquid water droplets. In pump-probe experiments, the influence of the time delay onto the emission of harmonic radiation is systematically studied. Phase-matching aspects are observed by controlling the focal position and the intensity of the probe pulse. The spatiotemporal dynamics of the droplet during interaction with intense laser pulses are studied by controlling the intensity of the pump pulse. We find transient phase-matching conditions and the expansion dynamics of the droplet to be of major influence on the harmonic yield.