We present studies of high-order harmonic generation (HHG) in laser ablation plumes of the ribonucleic acid nucleobase uracil and its deoxyribonucleic acid counterpart thymine. Harmonics were generated using 780 nm, 30 fs and 1300 nm, 40 fs radiation upon ablation with 1064 nm, 10 ns or 780 nm, 160 ps pulses. Strong HHG signals were observed from uracil plumes with harmonics emitted with photon energies >55 eV. Results obtained in uracil plumes were compared with those from thymine, which did not yield signs of harmonic generation. The ablation plumes of the two compounds were examined by collection of the ablation debris on a silicon substrate placed in close proximity to the target and by time-of-flight mass spectrometry. From this evidence we conclude that the differences in HHG signal are due to the different fragmentation dynamics of the molecules in the plasma plume. These studies constitute the first attempt to analyse differences in structural properties of complex molecules through plasma ablation-induced HHG spectroscopy.

Ultrashort optical pulses can trigger a variety of non-equilibrium processes in magnetic thin films affecting electrons and spins on femtosecond timescales. In order to probe the charge and magnetic degrees of freedom simultaneously, we developed an X-ray streaking technique that has the advantage of providing a jitter-free picture of absorption cross-section changes. In this paper, we present an experiment based on this approach, which we performed using five photon probing energies at the Ni M2,3-edges. This allowed us to retrieve the absorption and magnetic circular dichroism time traces, yielding detailed information on transient modifications of electron and spin populations close to the Fermi level. Our findings suggest that the observed absorption and magnetic circular dichroism dynamics both depend on the extreme ultraviolet (XUV) probing wavelength, and can be described, at least qualitatively, by assuming ultrafast energy shifts of the electronic and magnetic elemental absorption resonances, as reported in recent work. However, our analysis also hints at more complex changes, highlighting the need for further experimental and theoretical studies in order to gain a thorough understanding of the interplay of electronic and spin degrees of freedom in optically excited magnetic thin films.

High-order harmonic generation in graphite-ablated plasmas was systematically studied using ultrashort (3.5 and 30 fs) laser pulses. We observed the efficient frequency conversion of 3.5 fs Ti:sapphire laser pulses in the range of 15–26 eV. Stabilization of the harmonic yield at a 1 kHz pulse repetition rate was accomplished using a rotating graphite target. We also show the results of harmonic generation in carbon plasma using 1300 nm, 40 ps pulses, which allowed the extension of the harmonic cutoff while maintaining a comparable conversion efficiency to the case of 780 nm driving radiation. The time-of-flight mass spectrometric analysis of the plasma components and the scanning electron microscopy of plasma debris under optimal conditions for harmonic generation suggest the presence of small carbon clusters (C10–C30) in the plasma plume at the moment of femtosecond pulse propagation, which further aggregate on nearby substrates. We present the results of plasma spectroscopy obtained under unoptimized plasma conditions that elucidate the reduction in harmonic signal. We also present calculations of plasma concentration under different excitation conditions of the ablated graphite target.

Enhanced single harmonic generation is analyzed in indium laser ablation plasmas at excitation conditions of multicycle (30 fs) and few-cycle (3.5 fs) pulses. We demonstrate the strong influence of pulse duration, on the emission spectra from the indium plasma. For few-cycle pulses, the enhanced emissions do not coincide with the expected harmonic wavelengths, which is the case for multicycle pulses. We test the coherent properties of an enhanced emission around 20 eV using polarization and double-slit interference techniques. We also characterize the dynamics of the emissions from the indium plasma by tuning the laser pulse duration. A theoretical analysis is presented to describe the indium plasma emission upon excitation by few-cycle pulses.

The use of structured ultrashort pulses with coupled spatiotemporal properties is emerging as a key tool for ultrafast manipulation. Ultrafast vector beams are opening exciting opportunities in different fields such as microscopy, time-resolved imaging, nonlinear optics, particle acceleration or attosecond science. Here, we implement a technique for the full characterization of structured time-dependent polarization light waveforms with spatiotemporal resolution, using a compact twofold spectral interferometer, based on in-line bulk interferometry and fibre-optic coupler assisted interferometry. We measure structured infrared femtosecond vector beams, including radially polarized beams and complex-shaped beams exhibiting both temporal and spatial evolving polarization. Our measurements confirm that light waveforms with polarization evolving at the micrometer and femtosecond scales can be achieved through the use of structured waveplates and polarization gates. This new scale of measurement achieved will open the way to predict, check and optimize applications of structured vector beams at the femtosecond and micrometer scales.