Elliptically polarized high-harmonic radiation for production of isolated attosecond pulses.

Circularly polarized attosecond pulses are powerful tool to study chiral light-matter interaction via chiral electron dynamics. However, access to isolated circularly polarized attosecond pulses enabling straightforward interpretation of measurements, still remains a challenge. In this work, we experimentally demonstrate the generation of highly elliptically polarized high-harmonics in a two-color, bi-circular, collinear laser field.

Extended ellipticity control for attosecond pulses by high harmonic generation.

Attosecond (1  as=10  s) pulses produced through high harmonic generation (HHG) are a basis for studies of electron dynamics during light-matter interaction on an electron's natural time scale. Extensively exploited HHG technology has, however, a few unsolved problems, where producing of circularly polarized or chiral attosecond pulses belongs to them. We have demonstrated experimentally a way to control the ellipticity of attosecond pulse trains produced via HHG in two-color, bi-circular laser fields.

Few-femtosecond passage of conical intersections in the benzene cation.

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.

Time-resolved high harmonic spectroscopy of dynamical symmetry breaking in bi-circular laser fields: the role of Rydberg states.

The bi-circular scheme for high harmonic generation, which combines two counter-rotating circular fields with frequency ratio 2:1, has recently permitted to generate high harmonics with essentially circular polarization, opening the way for ultrafast chiral studies. This scheme produces harmonic lines at 3N + 1 and 3N + 2 multiples of the fundamental driving frequency, while the 3N lines are forbidden owing to the three-fold symmetry of the field. It is generally established that the routinely observed signals at these forbidden harmonic lines come from a slight ellipticity in the driving fields, which breaks the three-fold symmetry.

XUV-induced reactions in benzene on sub-10 fs timescale: nonadiabatic relaxation and proton migration.

Unraveling ultrafast dynamical processes in highly excited molecular species has an impact on our understanding of chemical processes such as combustion or the chemical composition of molecular clouds in the universe. In this article we use short (<7 fs) XUV pulses to produce excited cationic states of benzene molecules and probe their dynamics using few-cycle VIS/NIR laser pulses. The excited states produced by the XUV pulses lie in an especially complex spectral region where multi-electronic effects play a dominant role.