Structured light in the short-wavelength regime opens exciting avenues for the study of ultrafast spin and electronic dynamics. Here, we demonstrate theoretically and experimentally the generation of vector-vortex beams (VVB) in the extreme ultraviolet through high-order harmonic generation (HHG). The up-conversion of VVB, which are spatially tailored in their spin and orbital angular momentum, is ruled by the conservation of the topological Pancharatnam charge in HHG. Despite the complex propagation of the driving beam, high-harmonic VVB are robustly generated with smooth propagation properties. Remarkably, we find out that the conversion efficiency of high-harmonic VVB increases with the driving topological charge. Our work opens the possibility to synthesize attosecond helical structures with spatially varying polarization, a unique tool to probe spatiotemporal dynamics in inhomogeneous media or polarization-dependent systems.

The landscape of ultrafast structured light pulses has significantly advanced thanks to the ability of high-order harmonic generation (HHG) to translate the spatial properties of infrared laser beams to the extreme-ultraviolet (EUV) spectral range. In particular, the up-conversion of orbital angular momentum (OAM) has enabled the generation of high-order harmonics whose OAM scales linearly with the harmonic order and the topological charge of the driving field. Having a well-defined OAM, each harmonic is emitted as an EUV femtosecond vortex pulse. However, the order-dependent OAM across the harmonic comb precludes the synthesis of attosecond vortex pulses. Here we demonstrate a method for generating attosecond vortex pulse trains, i.e., a succession of attosecond pulses with a helical wavefront, resulting from the coherent superposition of a comb of EUV high-order harmonics with the same OAM. By driving HHG with a polarization tilt-angle fork grating, two spatially separated circularly polarized high-order harmonic beams with order-independent OAM are created. Our work opens the route towards attosecond-resolved light-matter interactions with two extra degrees of freedom, spin and OAM, which are particularly interesting for probing chiral systems and magnetic materials.

Coherent control over electron dynamics in atoms and molecules using high-intensity circularly polarized laser pulses gives rise to current loops, resulting in the emission of magnetic fields. We propose, and demonstrate with ab initio calculations, "current-gating" schemes to generate direct or alternating-current magnetic pulses in the infrared spectral region, with highly tunable waveform and frequency, and showing femtosecond-to-attosecond pulse duration. In optimal conditions, the magnetic pulse can be highly isolated from the driving laser and exhibits a high flux density (∼1 T at a few hundred nanometers from the source, with a pulse duration of 787 attoseconds) for application in forefront experiments of ultrafast spectroscopy. Our work paves the way toward the generation of attosecond magnetic fields to probe ultrafast magnetization, chiral responses, and spin dynamics.

Few-electron atoms interacting with electromagnetic fields provide for privileged scenarios for disentangling elemental correlation mechanisms. We demonstrate that high-order harmonic generation (HHG) from neutral helium presents a distinctive trace of correlation back reaction in the electron dynamics prior to ionization. We identify a mechanism in which the field interacts with one of the electrons, while the second is excited to a Rydberg level through the Coulomb interaction. As back response to this correlated excitation, the first electron is knocked down to a lower level, from which it ionizes to generate high-order harmonics. Unlike other multielectron phenomena, where the electron-field interaction is modified by cross correlations with the rest of the interacting electrons, back reaction is a mechanism of autocorrelation. Our numerical simulations reveal back reaction as a relevant aspect in HHG from correlated two-electron systems, and paves the way to disentangle valence electron-electron correlation dynamics using high-harmonic spectroscopy.