We have investigated multiphoton multiple ionization dynamics of argon and xenon atoms using a new x-ray free electron laser (XFEL) facility, SPring-8Ångstrom Compact free electron LAser (SACLA) in Japan, and identified that Xe n+ with n up to 26 are produced predominantly via four-photon absorption as well as Ar n+ with n up to 10 are produced via two-photon absorption at a photon energy of 5.5 keV. The absolute fluence of the XFEL pulse, needed for comparison between theory and experiment, has been determined using two-photon processes in the argon atom with the help of benchmark ab initio calculations. Our experimental results, in combination with a newly developed theoretical model for heavy atoms, demonstrate the occurrence of multiphoton absorption involving deep inner shells.

Using electron spectroscopy, we have investigated nanoplasma formation from noble gas clusters exposed to high-intensity hard-x-ray pulses at ~5 keV. Our experiment was carried out at the SPring-8 Angstrom Compact free electron LAser (SACLA) facility in Japan. Dedicated theoretical simulations were performed with the molecular dynamics tool XMDYN. We found that in this unprecedented wavelength regime nanoplasma formation is a highly indirect process. In the argon clusters investigated, nanoplasma is mainly formed through secondary electron cascading initiated by slow Auger electrons. Energy is distributed within the sample entirely through Auger processes and secondary electron cascading following photoabsorption, as in the hard x-ray regime there is no direct energy transfer from the field to the plasma. This plasma formation mechanism is specific to the hard-x-ray regime and may, thus, also be important for XFEL-based molecular imaging studies. In xenon clusters, photo- and Auger electrons contribute more significantly to the nanoplasma formation. Good agreement between experiment and simulations validates our modelling approach. This has wide-ranging implications for our ability to quantitatively predict the behavior of complex molecular systems irradiated by high-intensity hard x-rays.

Sequential multiphoton multiple ionization of atomic argon and xenon irradiated by X-ray freeelectron laser pulses from SACLA. Abstract. We have investigated multiphoton multiple ionization of argon and xenon atoms at 5 keV using a new x-ray free electron laser (XFEL) facility, the SPring-8 Angstrom Compact free electron LAser (SACLA) in Japan. The experimental results are compared with new theoretical results presented here. The absolute fluence of the XFEL pulse has been determined with the help of the calculations utilizing twophoton processes in the argon atom. The high charge states up to +22 observed for Xe in comparison with the calculations point to the occurrence of sequential L-shell multiphoton absorption and of resonance-enabled x-ray multiple ionization. Journal of Physics

We report unambiguous experimental and theoretical evidence of intramolecular photoelectron diffraction in the collective vibrational excitation that accompanies high-energy photoionization of gas-phase CF 4 , BF 3 , and CH 4 from the 1s orbital of the central atom. We show that the ratios between vibrationally resolved photoionization cross sections (v-ratios) exhibit pronounced oscillations as a function of photon energy, which is the fingerprint of electron diffraction by the surrounding atomic centers. This interpretation is supported by the excellent agreement between first-principles static-exchange and time-dependent density functional theory calculations and high resolution measurements, as well as by qualitative agreement at high energies with a model in which atomic displacements are treated to first order of perturbation theory. The latter model allows us to rationalize the results for all the v-ratios in terms of a generalized v-ratio, which contains information on the structure of the above three molecules and the corresponding molecular cations. A fit of the measured v-ratios to a simple formula based on this model suggests that the method could be used to obtain structural information of both neutral and ionic molecular species.

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Since the degree of expertise of the observers with respect to reading eZIS did not influence the performance and an eZIS can use a common normal database by converting site-specific SPECT data to the core data, the eZIS was considered to be very useful for diagnosing early AD in routine studies in many institutions.

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