Tuneable ultrafast laser pulses are a powerful tool for measuring difficult-to-access degrees of freedom in materials science. In general these experiments require the ability to address resonances and excitations both above and below the bandgap of materials, and to probe their response at the timescale of the fastest non-trivial internal dynamics. This drives the need for ultrafast sources capable of delivering 10-15 fs duration pulses tuneable across the entire visible (VIS) and near infrared (NIR) range, 500-3000 nm, as well as the characterization of these sources. Here we present a single frequency-resolved optical gating (FROG) system capable of self-referenced characterization of pulses with 10 fs duration across the entire VIS-NIR spectral range. Our system does not require auxiliary beams and only minor reconfiguration for different wavelengths. We demonstrate the system with measurements of pulses across the entire tuning range.

In solids, the response of the lattice to photo-excitation is often described by the inertial evolution on an impulsively modified potential energy surface which leads to coherent motion. However, it remains unknown if vibrational coherence is sustained through a phase transition, during which coupling between modes can be strong and may lead to rapid loss of coherence. Here we use coherent phonon spectroscopy to track lattice coherence in the structural phase transition of V2O3. In both the low and high symmetry phases unique coherent phonon modes are generated at low fluence. However, coherence is lost when driving between the low and high symmetry phases. Our results suggest strongly-damped non-inertial dynamics dominate during phase transition due to disorder and multi-mode coupling.

In this work, we present an achromatic pump-probe setup covering the visible (VIS) to near-infrared (NIR) wavelength regions (500-3000 nm) for few-cycle pulses. Both the pump and probe arms can work either in the VIS or the NIR wavelength regions, making our setup suitable for multi-color, broadband pump-probe measurements. In particular, our setup minimizes time-smearing due to the phase front curvature, an aspect of ultrafast spectroscopy that has been missing from previous works and allowing us to achieve sub-20-fs temporal resolution. We demonstrate the capabilities of our setup by performing measurements on Pr 0.5 Ca 1.5 MnO 4 . We pump and probe in both wavelength regions with a range of pump fluences and demonstrate how the observed dynamics depend strongly on the probe wavelength. Furthermore, the observation of a 16.5 THz phonon demonstrates the high temporal resolution of the setup.

Differentially pumped capillaries, i.e., capillaries operated in a pressure gradient environment, are widely used for nonlinear pulse compression. In this work, we show that strong pressure gradients and high gas throughputs can cause spatiotemporal instabilities of the output beam profile. The instabilities occur with a sudden onset as the flow evolves from laminar to turbulent. Based on the experimental and numerical results, we derive guidelines to predict the onset of those instabilities and discuss possible applications in the context of nonlinear flow dynamics.