Nonlinear spectroscopy in the extreme ultraviolet (EUV) and soft x-ray spectral range offers the opportunity for element selective probing of ultrafast dynamics using core-valence transitions (Mukamel et al., Acc. Chem. Res. 42, 553 (2009)). We demon
strate a step on this path showing core-valence sensitivity in transient grating spectroscopy with EUV probing. We study the optically induced insulator-to-metal transition (IMT) of a VO2 film with EUV diffraction from the optically excited sample. The VO2 exhibits a change in the 3p-3d resonance of V accompanied by an acoustic response. Due to the broadband probing we are able to separate the two features.
We describe a setup to study ultrafast dynamics in gas-phase molecules using time-resolved photoelectron and photoion spectroscopy. The vacuum ultraviolet (VUV) probe pulses are generated via strong field high-order harmonic generation from infrared
femtosecond laser pulses. The band pass characteristic in transmission of thin indium (In) metal foil is exploited to isolate the $9^{text{th}}$ harmonic of the 800 nm fundamental (H9, 14 eV, 89 nm) from all other high harmonics. The $9^{text{th}}$ harmonic is obtained with high conversion efficiencies and has sufficient photon energy to access the complete set of valence electron levels in most molecules. The setup also allows for direct comparison of VUV single-photon probe with 800 nm multi-photon probe without influencing the delay of excitation and probe pulse or the beam geometry. We use a magnetic bottle spectrometer with high collection efficiency for electrons, serving at the same time as a time of flight spectrometer for ions. Characterization measurements on Xe reveal the spectral width of H9 to be $190pm60$ meV and a photon flux of $sim1cdot10^{7}$ photons/pulse after spectral filtering. As a first application, we investigate the S$_1$ excitation of perylene using time-resolved ion spectra obtained with multi-photon probing and time-resolved electron spectra from VUV single-photon probing. The time resolution extracted from cross-correlation measurements is $65pm10$ fs for both probing schemes and the pulse duration of H9 is found to be $35pm8$ fs.
High harmonic generation is a convenient way to obtain extreme ultraviolet light from table-top laser systems and the experimental tools to exploit this simple and powerful light source for time-resolved spectroscopy are being developed by several gr
oups. For these applications, brightness and stability of the high harmonic generation is a key feature. This article focuses on practical aspects in the generation of extreme ultraviolet pulses with ultrafast commercial lasers, namely generation parameters and online monitoring as well as analysis of generation yield and stability.
