We report on an experimental study of supercontinuum generation in photonic crystal fibers with low-intensity femtosecond pulses, which provides evidence for a novel spectral broadening mechanism. The observed results agree with our theoretical calculations carried out without making the slowly varying envelope approximation. Peculiarities of the measured spectra and their theoretical explanation demonstrate that the reason for the white-light generation in photonic crystal fibers is fission of higher-order solitons into redshifted fundamental solitons and blueshifted nonsolitonic radiation.

Reversible structural changes of a nanostructure were measured nondestructively with subpicometer spatial and subpicosecond temporal resolution via x-ray diffraction (XRD). The spatially periodic femtosecond excitation of a gallium arsenide/aluminum gallium arsenide superlattice results in coherent lattice motions with a 3.5-picosecond period, which was directly monitored by femtosecond x-ray pulses at a 1-kilohertz repetition rate. Small changes (DeltaR/R = 0.01) of weak Bragg reflexes (R = 0.005) were detected. The phase and amplitude of the oscillatory XRD signal around a new equilibrium demonstrate that displacive excitation of the zone-folded acoustic phonons is the dominant mechanism for strong excitation.

We analyze pulse self-compression in femtosecond filaments, both experimentally and numerically. We experimentally demonstrate the compression of 45 fs pulses down to a duration of 7.4 fs at millijoule pulse energies. This sixfold compression in a self-generated filament does not require any means for dispersion compensation and is highly efficient. We compare our results to numerical simulations, providing a complete propagation model that accounts for full dispersion, pressure variations, Kerr nonlinearity and plasma generation in multiphoton and tunnel regimes. The equations are numerically integrated and allow for a quantitative comparison with the experiment. Our experiments and numerical simulations reveal a characteristic spectrotemporal structure of the self-compressed pulses, consisting of a compressible blue wing and an incompressible red pedestal. We explain the underlying mechanism that leads to this structure and examine the scalability of filament self-compression with respect to pulse energy and gas pressure.

We report the first analysis of the polarization and lattice dynamics in a metal/ferroelectric/metal nanolayer system by femtosecond x-ray diffraction. Two Bragg reflections provide information on the coupled dynamics of the two relevant phonon modes for ferroelectricity in perovskites, the tetragonal distortion and the soft mode. Optical excitation of the SrRuO(3) metal layers generates giant stress (>1 GPa) compressing the PbZr(0.2)Ti(0.8)O(3) layers by up to 2%. The resulting change of tetragonality reaches a maximum after 1.3 ps. As a result, the ferroelectric polarization P is reduced by up to 100% with a slight delay that is due to the anharmonic coupling of the two modes.

Observing the crucial first few femtoseconds of photochemical reactions requires tools typically not available in the femtochemistry toolkit. Such dynamics are now within reach with the instruments provided by attosecond science. Here, we apply experimental and theoretical methods to assess the ultrafast nonadiabatic vibronic processes in a prototypical complex system—the excited benzene cation. We use few-femtosecond duration extreme ultraviolet and visible/near-infrared laser pulses to prepare and probe excited cationic states and observe two relaxation timescales of 11 ± 3 fs and 110 ± 20 fs. These are interpreted in terms of population transfer via two sequential conical intersections. The experimental results are quantitatively compared with state-of-the-art multi-configuration time-dependent Hartree calculations showing convincing agreement in the timescales. By characterising one of the fastest internal conversion processes studied to date, we enter an extreme regime of ultrafast molecular dynamics, paving the way to tracking and controlling purely electronic dynamics in complex molecules.

We demonstrate a novel technique for pulse compression of few-millijoule pulses with shorter than 10 fs duration. Our technique relies on spectral broadening in a white-light filament generated in a noble gas. In this filament we observe self-compression of 45 fs pulses down to below 8 fs duration without the need for any additional dispersion compensation. Using input pulses of 5 mJ, we generate compressed pulses with up to 3.8 mJ pulse energy. Therefore this method is much more efficient than previously demonstrated compression schemes. The generated peak powers of more than 100 GW at a kilohertz repetition rate open up a perspective for compression of few-cycle pulses with energies well beyond the capacity of hollow-fiber compressors.

Pulses with durations below 4 fs have been generated using the method of ultrafast molecular phase modulation. A laser pulse shorter than the molecular vibrational or rotational period obtains spectral broadening during propagation along a hollow waveguide filled with previously impulsively excited Raman active gases. The induced time dependent phase, frequency, and frequency chirp are controllable by changing the delay between excitation and probe pulse within the molecular vibrational period.

We develop theoretically and confirm both numerically and experimentally a comprehensive analytical model which describes the propensity rules in the emission of circularly polarized high harmonics by systems driven by two-color counter-rotating fields, a fundamental and its second harmonic. We identify and confirm the three propensity rules responsible for the contrast between the 3N+1 and 3N+2 harmonic lines in the HHG spectra of noble gas atoms. We demonstrate how these rules depend on the laser parameters and how they can be used in the experiment to shape the polarization properties of the emitted attosecond pulses.