We present a demonstration of two-photon double ionization of neon using an intense extreme ultraviolet (XUV) attosecond pulse train (APT) in a photon energy regime where both direct and sequential mechanisms are allowed. For an APT generated through high-order harmonic generation (HHG) in argon we achieve a total pulse energy close to $1\mu \mathrm{J}$, a central energy of 35 eV, and a total bandwidth of $\sim 30$ eV. The APT is focused by broadband optics in a neon gas target to an intensity of $3\times {10}^{12}\mathrm{W}{\mathrm{cm}}^{-2}$. By tuning the photon energy across the threshold for the sequential process the double ionization signal can be turned on and off, indicating that the two-photon double ionization predominantly occurs through a sequential process. The demonstrated performance opens up possibilities for future XUV-XUV pump-probe experiments with attosecond temporal resolution in a photon energy range where it is possible to unravel the dynamics behind direct versus sequential double ionization and the associated electron correlation effects.

The dynamics following laser-induced molecular photodissociation of gas-phase ${\mathrm{CH}}_2\mathrm{BrI}$ at 271.6 nm were investigated by time-resolved Coulomb-explosion imaging using intense near-IR femtosecond laser pulses. The observed delay-dependent photofragment momenta reveal that ${\mathrm{CH}}_2\mathrm{BrI}$ undergoes C-I cleavage, depositing 65.6% of the available energy into internal product states, and that absorption of a second UV photon breaks the C-Br bond of ${\mathrm{CH}}_2\mathrm{Br}$. Simulations confirm that this mechanism is consistent with previous data recorded at 248 nm, demonstrating the sensitivity of Coulomb-explosion imaging as a real-time probe of chemical dynamics.

The photodissociation dynamics of CH₃I and CH₂ClI at 272 nm were investigated by time-resolved Coulomb explosion imaging, with an intense non-resonant 815 nm probe pulse. Fragment ion momenta over a wide m/z range were recorded simultaneously by coupling a velocity map imaging spectrometer with a pixel imaging mass spectrometry camera. For both molecules, delay-dependent pump-probe features were assigned to ultraviolet-induced carbon-iodine bond cleavage followed by Coulomb explosion. Multi-mass imaging also allowed the sequential cleavage of both carbon-halogen bonds in CH₂ClI to be investigated. Furthermore, delay-dependent relative fragment momenta of a pair of ions were directly determined using recoil-frame covariance analysis. These results are complementary to conventional velocity map imaging experiments and demonstrate the application of time-resolved Coulomb explosion imaging to photoinduced real-time molecular motion.

Due to its element and site specificity, inner-shell photoelectron spectroscopy is a widely used technique to probe the chemical structure of matter. Here, we show that time-resolved inner-shell photoelectron spectroscopy can be employed to observe ultrafast chemical reactions and the electronic response to the nuclear motion with high sensitivity. The ultraviolet dissociation of iodomethane (${\mathrm{CH}}_3\mathrm{I}$) is investigated by ionization above the iodine $4d$ edge, using time-resolved inner-shell photoelectron and photoion spectroscopy. The dynamics observed in the photoelectron spectra appear earlier and are faster than those seen in the iodine fragments. The experimental results are interpreted using crystal-field and spin-orbit configuration interaction calculations, and demonstrate that time-resolved inner-shell photoelectron spectroscopy is a powerful tool to directly track ultrafast structural and electronic transformations in gas-phase molecules.

Time-resolved photoelectron spectroscopy is applied to study the excited state dynamics of the DNA base adenine and its ribonucleoside adenosine in aqueous solution for pump and probe photon energies in the range between 4.66 eV and 5.21 eV. We follow the evolution of the prepared excited state on the potential energy surface and retrieve lifetimes of the S₁ state under different excitation conditions.

We present an optical system based on two toroidal mirrors in a Wolter configuration to focus broadband extreme ultraviolet (XUV) radiation. Optimization of the focusing optics alignment is carried out with the aid of an XUV wavefront sensor. Back-propagation of the optimized wavefront to the focus yields a focal spot of 3.6 × 4.0 µm² full width at half maximum, which is consistent with ray-tracing simulations that predict a minimum size of 3.0 × 3.2 µm². This work is important for optimizing the intensity of focused high-order harmonics in order to reach the nonlinear interaction regime.