Laser pump-X-ray probe experiments require control over the X-ray pulse pattern and timing. Here, the first use of pseudo-single-bunch mode at the Advanced Light Source in picosecond time-resolved X-ray absorption experiments on solutions and solids is reported. In this mode the X-ray repetition rate is fully adjustable from single shot to 500 kHz, allowing it to be matched to typical laser excitation pulse rates. Suppressing undesired X-ray pulses considerably reduces detector noise and improves signal to noise in time-resolved experiments. In addition, dose-induced sample damage is considerably reduced, easing experimental setup and allowing the investigation of less robust samples. Single-shot X-ray exposures of a streak camera detector using a conventional non-gated charge-coupled device (CCD) camera are also demonstrated.

Ultrafast studies of magnetization dynamics have revealed fundamental processes that govern spin dynamics, and the emergence of time-resolved x-ray techniques has extended these studies to long-range spin structures that result from interactions with competing symmetries. By combining time-resolved resonant x-ray scattering and ultrafast magneto-optical Kerr studies, we show that the dynamics of the core spins in the helical magnetic structure occur on much longer time scales than the excitation of conduction electrons in the lanthanide metal Dy. The observed spin behavior differs markedly from that observed in the ferromagnetic phase of other lanthanide metals or transition metals and is strongly dependent on temperature and excitation fluence. This unique behavior results from coupling of the real-space helical spin structure to the shape of the conduction electron Fermi surface in momentum space, which creates a bottleneck in spin scattering events that transfer the valence excitation to the core spins. The dependence of the dynamics on the intersite interactions renders the helical ordering much more robust to perturbations than simple ferromagnetic or antiferromagnetic ordering, where dynamics are driven primarily by on-site interactions.

The study of photoexcited strongly correlated materials is attracting growing interest since their rich phase diagram often translates into an equally rich out-of-equilibrium behaviour. With femtosecond optical pulses, electronic and lattice degrees of freedom can be transiently decoupled, giving the opportunity of stabilizing new states inaccessible by quasi-adiabatic pathways. Here we show that the prototype Mott-Hubbard material V₂O₃ presents a transient non-thermal phase developing immediately after ultrafast photoexcitation and lasting few picoseconds. For both the insulating and the metallic phase, the formation of the transient configuration is triggered by the excitation of electrons into the bonding a_1g orbital, and is then stabilized by a lattice distortion characterized by a hardening of the A_1g coherent phonon, in stark contrast with the softening observed upon heating. Our results show the importance of selective electron-lattice interplay for the ultrafast control of material parameters, and are relevant for the optical manipulation of strongly correlated systems.