A liquid carbon (-C) sample is generated through constant volume heating exposing an amorphous carbon foil to an intense ultrashort laser pulse. Time-resolved x-ray absorption spectroscopy at the C edge is used to monitor the dynamics of the melting process revealing a subpicosecond rearrangement of the electronic structure associated with a sudden change of the C bonding hybridization. The obtained -C sample, resulting from a nonthermal melting mechanism, reaches a transient equilibrium condition with a temperature of about 14 200 K and pressure in the order of 0.5 Mbar in about 0.3 ps, prior to hydrodynamic expansion. A detailed analysis of the atomic and electronic structure in solid-density -C based on time-resolved x-ray absorption spectroscopy and theoretical simulations is presented. The method can be fruitfully used for extending the experimental investigation of the C phase diagram in a vast unexplored region covering the temperature range with pressures up to 1 Mbar.
Ultrafast optical-domain spectroscopies allow to monitor in real time the motion of nuclei in molecules. Achieving element-selectivity had to await the advent of time resolved X-ray spectroscopy, which is now commonly carried at X-ray free electron lasers. However, detecting light element that are commonly encountered in organic molecules, remained elusive due to the need to work under vacuum. Here, we present an impulsive stimulated Raman scattering (ISRS) pump/carbon K-edge absorption probe investigation, which allowed observation of the low-frequency vibrational modes involving specific selected carbon atoms in the Ibuprofen RS dimer. Remarkably, by controlling the probe light polarization we can preferentially access the enantiomer of the dimer to which the carbon atoms belong.
Stimulated emission is a fundamental process in nature that deserves to be investigated and understood in the extreme ultra-violet (EUV) and x-ray regimes. Today, this is definitely possible through high energy density free electron laser (FEL) beams. In this context, we give evidence for soft-x-ray stimulated emission from a magnesium oxide solid target pumped by EUV FEL pulses formed in the regime of travelling-wave amplified spontaneous emission in backward geometry. Our results combine two effects separately reported in previous works: emission in a privileged direction and existence of a material-dependent threshold for the stimulated emission. We develop a novel theoretical framework, based on coupled rate and transport equations taking into account the solid-density plasma state of the target. Our model accounts for both observed mechanisms that are the privileged direction for the stimulated emission of the Mg L2,3 characteristic emission and the pumping threshold.
FERMI@Elettra is a new free-electron-laser (FEL) facility, presently under commissioning, able to generate subpicosecond photon pulses of high intensity in the far ultraviolet and soft X-ray range (λ=100-20 nm for the present FEL1 source, extended in future to 4 nm with the FEL2 source). Here we briefly describe the present status of the TIMEX end-station, devoted to perform experiments on condensed matter under extreme conditions. The layout of the end-station, presently in the final stages of construction, is reported showing the details of the optics and sample environment. The potential for transmission, reflection, scattering, as well as pump-and-probe experiments is discussed taking into account that FEL pulses can heat thin samples up to the warm dense matter (WDM) regime. The calculated deposited energy in selected elemental films, including saturation effects, shows that homogeneous heating up to very high temperatures (1-10 eV for the electrons) can be easily reached with a suitable tuning of the energy and focus of the soft x-ray pulses of FERMI@Elettra. The results of the first test of the TIMEX end-station are also reported.
Intense femtosecond infrared laser pulses induce a nonequilibrium between thousands of Kelvin hot valence electrons and room-temperature ions in a germanium sample foil. The evolution of this exotic state of matter is monitored with time-resolved extreme ultraviolet absorption spectroscopy across the Ge M-2,M-3 edge (similar or equal to 30 eV) using the FERMI free-electron laser. We analyze two distinct regimes in the ultrafast dynamics in laser-excited Ge: First, on a subpicosecond time scale, the electron energy distribution thermalizes to an extreme temperature unreachable in equilibrium solid germanium; then, during the following picoseconds, the lattice reacts strongly altering the electronic structure and resulting in melting to a metallic state alongside a breakdown of the local atomic order. Data analysis, based on a hybrid approach including both numerical and analytical calculations, provides an estimation of the electron and ion temperatures, the electron density of states, the carrier-phonon relaxation time, as well as the carrier density and lattice heat capacity under those extreme nonequilibrium conditions. Related structural anomalies, such as the occurrence of a transient low-density liquid phase and the possible drop in lattice heat capacity are discussed.