We present an extreme ultraviolet (XUV) transient absorption apparatus tailored to attosecond and femtosecond measurements on bulk solid-state thin-film samples, specifically when the sample dynamics are sensitive to heating effects. The setup combines methodology for stabilizing sub-femtosecond time-resolution measurements over 48 h and techniques for mitigating heat buildup in temperature-dependent samples. Single-point beam stabilization in pump and probe arms and periodic time-zero reference measurements are described for accurate timing and stabilization. A hollow-shaft motor configuration for rapid sample rotation, raster scanning capability, and additional diagnostics are described for heat mitigation. Heat transfer simulations performed using a finite element analysis allow comparison of sample rotation and traditional raster scanning techniques for 100 Hz pulsed laser measurements on vanadium dioxide, a material that undergoes an insulator-to-metal transition at a modest temperature of 340 K. Experimental results are presented confirming that the vanadium dioxide (VO₂) sample cannot cool below its phase transition temperature between laser pulses without rapid rotation, in agreement with the simulations. The findings indicate the stringent conditions required to perform rigorous broadband XUV time-resolved absorption measurements on bulk solid-state samples, particularly those with temperature sensitivity, and elucidate a clear methodology to perform them.

The photoinduced insulator-to-metal phase transition in vanadium dioxide is experimentally investigated by attosecond transient absorption spectroscopy. Ultrafast changes cover a broad ~20-eV-wide spectral range, emphasizing core spectroscopic access and the importance of electron correlation effects.

Attosecond transient reflectivity in the extreme ultraviolet is developed for monitoring band-gap excitation dynamics in germanium. The investigations unravel the fastest carrierscattering processes on the few-femtosecond time scale, and carrier thermalization on longer time scales.

Attosecond transient reflectivity is developed to observe the photoexcitation dynamics in germanium. Attosecond time-resolved measurements of the dielectric function reveal a fewfemtosecond collective electronic response time, which renormalizes the Coulomb interaction between the excited carriers.

Coulomb correlations can manifest in exotic properties in solids, but how these properties can be accessed and ultimately manipulated in real time is not well understood. The insulator-to-metal phase transition in vanadium dioxide (VO₂) is a canonical example of such correlations. Here, few-femtosecond extreme UV transient absorption spectroscopy (FXTAS) at the vanadium M_2,3 edge is used to track the insulator-to-metal phase transition in VO₂ This technique allows observation of the bulk material in real time, follows the photoexcitation process in both the insulating and metallic phases, probes the subsequent relaxation in the metallic phase, and measures the phase-transition dynamics in the insulating phase. An understanding of the VO₂ absorption spectrum in the extreme UV is developed using atomic cluster model calculations, revealing V³⁺/d² character of the vanadium center. We find that the insulator-to-metal phase transition occurs on a timescale of 26 ± 6 fs and leaves the system in a long-lived excited state of the metallic phase, driven by a change in orbital occupation. Potential interpretations based on electronic screening effects and lattice dynamics are discussed. A Mott-Hubbard-type mechanism is favored, as the observed timescales and d² nature of the vanadium metal centers are inconsistent with a Peierls driving force. The findings provide a combined experimental and theoretical roadmap for using time-resolved extreme UV spectroscopy to investigate nonequilibrium dynamics in strongly correlated materials.

We developed and implemented an experimental setup for the generation of high-energy high-order harmonics in argon gas for nonlinear experiments in the extreme ultraviolet (XUV) spectral range. High-order harmonics were generated by loosely focusing a high-energy laser pulse centered around 800 nm into a gas cell filled with argon in a phase-matching condition. The wavefront distortions of the driving pulse were corrected by a deformable mirror, and the XUV conversion efficiency was significantly improved due to the excellent beam profile at focus. A high-damage-threshold beam splitter was used to eliminate high-energy driving pulses co-propagating with high-order harmonics. The setup has a potential to provide intense ultrashort XUV pulses reaching the intensity levels required for nonlinear experiments in the XUV spectral range.

It has been demonstrated in the past that high fluxes of extreme ultraviolet (XUV) light could be obtained by driving high harmonic generation (HHG) with high energy lasers. However, the peak intensity at the focal point of a femtosecond laser with more than 100 mJ can be too high for phase-matched HHG in gases. We propose a method to optimize the spatial profile at off-focus locations of the high energy driving laser to avoid fully ionizing the target atoms. The beam profile before or after the focal point depends on the wavefront quality of the laser beam and the near field intensity distribution. The beam spot diameter reaches three times that at the focus by adding customized wavefront terms. An XUV pulse energy of 5.6 μJ was obtained from HHG when a larger off-focus spot of a 500 mJ Ti: sapphire laser beam was applied in an argon gas cell.

Extreme ultraviolet (XUV) transient reflectivity around the germanium M4,5 edge (3d core-level to valence transition) at 30 eV is advanced to obtain the transient dielectric function of crystalline germanium [100] on femtosecond to picosecond time scales following photoexcitation by broadband visible-to-infrared (VIS/NIR) pulses. By fitting the transient dielectric function, carrier-phonon induced relaxations are extracted for the excited carrier distribution. The measurements reveal a hot electron relaxation rate of 3.2±0.2ps attributed to the X-L intervalley scattering and a hot hole relaxation rate of 600±300fs ascribed to intravalley scattering within the heavy hole (HH) band, both in good agreement with previous work. An overall energy shift of the XUV dielectric function is assigned to a thermally induced band gap shrinkage by formation of acoustic phonons, which is observed to be on a timescale of 4-5 ps, in agreement with previously measured optical phonon lifetimes. The results reveal that the transient reflectivity signal at an angle of 66 with respect to the surface normal is dominated by changes to the real part of the dielectric function, due to the near critical angle of incidence of the experiment (66-70 for the range of XUV energies used. This work provides a methodology for interpreting XUV transient reflectivity near core-level transitions, and it demonstrates the power of the XUV spectral region for measuring ultrafast excitation dynamics in solids.