Vector momentum distributions of Ne(n+) (n = 1,2,3) ions created by 30 fs, approximately 1 PW/cm(2) laser pulses at 795 nm have been measured using recoil-ion momentum spectroscopy. Distinct maxima along the light polarization axis are observed at 4.0 and 7.5 a.u. for Ne2+ and Ne3+ production, respectively. Hence, mechanisms based on an instantaneous release of two (or more) electrons can be ruled out as a dominant contribution to nonsequential strong-field multiple ionization. The positions of the maxima are in accord with kinematical constraints set by the classical "rescattering model."

Understanding molecular femtosecond dynamics under intense X-ray exposure is critical to progress in biomolecular imaging and matter under extreme conditions. Imaging viruses and proteins at an atomic spatial scale and on the time scale of atomic motion requires rigorous, quantitative understanding of dynamical effects of intense X-ray exposure. Here we present an experimental and theoretical study of C 60 molecules interacting with intense X-ray pulses from a free-electron laser, revealing the influence of processes not previously reported. Our work illustrates the successful use of classical mechanics to describe all moving particles in C 60 , an approach that scales well to larger systems, for example, biomolecules. Comparisons of the model with experimental data on C 60 ion fragmentation show excellent agreement under a variety of laser conditions. The results indicate that this modelling is applicable for X-ray interactions with any extended system, even at higher X-ray dose rates expected with future light sources.

The photoelectron spectra of C60 ionized using a 790 nm laser with pulse durations varying from 25 fs to 5 ps have been determined. For 25 fs pulses, in the absence of fragmentation, the ionization mechanism is direct multiphoton ionization with clear observation of above threshold ionization. As the pulse duration is increased, this becomes dominated by a statistical ionization due to equilibration among the electronic degrees of freedom. For pulse durations on the order of a ps coupling to the vibrational degrees of freedom occurs and the well-known phenomenon of delayed (&mgr;s) ionization is observed.

We compare theoretical results on statistical electron emission from electronically hot but vibrationally cold C60 with recent experimental results involving excitation with ultrashort laser pulses. Both photoelectron spectra and ion yields of C60 as well as fragment ions are compared with the predictions of the statistical electron emission model. Quantitative agreement is obtained between the calculations and the experimentally measured photoelectron spectra, total ion yields and singly-doubly charged branching ratio. The electron-phonon coupling time is fitted to a few hundred femtoseconds, consistent with independent measurements. The data allow a determination of the thermal properties of the electron system, which are consistent with the theoretical input. The data also allow a fit of the averaged photon absorption cross section.

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The first highly resolved electronic spectra of small non-alkali metal clusters embedded in nanoscopic helium droplets (N ≈ 20 000) are presented. The helium droplets serve as an extremely cold liquid matrix with a temperature of 0.37 K. Resonant two-photon-ionization is used for size-selective spectroscopy on a silver cluster distribution (N ≤ 10). Results are reported for Ag 2 , Ag 3 and for Ag 8 . For the latter, a very narrow absorption spectrum is resolved corresponding to the Ag 8 plasmon resonance. The linewidth of the observed resonance is a factor of two smaller than theoretical zero-temperature predictions for the plasmon line width of closed-shell metal clusters. In contrast, the lifetime of the Ag 8 resonance is estimated to be of the order of nanoseconds, which is inconsistent with the plasmon picture and typical for molecular transitions.PACS. 36.40.Mr Spectroscopy of clusters -67.40.Yv Impurities and other defects in 4 He

Gas-phase C60 photoionization and photofragmentation experiments were performed using a sub-50 fs Ti Sapphire laser system and reflectron time-of-flight (RETOF) mass spectrometer. The dependence of the C60+ and C602+ signals on the laser intensity for the fundamental (795 nm) and second harmonic (ca. 400 nm) has been determined. For low laser intensities, before the onset of fragmentation, single ionization is a direct multiphoton process. Double ionization is a sequential process in which C602+ originates from already singly ionized fullerenes. At laser intensities beyond the onset of C602+ there is considerable metastable fragmentation indicating a strong coupling of electronic excitation energy into vibrational degrees of freedom that appears to be in competition with multiple ionization.

Explosions of large Xe clusters ( ~ 11,000) irradiated by femtosecond pulses of 850 eV x-ray photons focused to an intensity of up to 10(17) W/cm(2) from the Linac Coherent Light Source were investigated experimentally. Measurements of ion charge-state distributions and energy spectra exhibit strong evidence for the formation of a Xe nanoplasma in the intense x-ray pulse. This x-ray produced Xe nanoplasma is accompanied by a three-body recombination and hydrodynamic expansion. These experimental results appear to be consistent with a model in which a spherically exploding nanoplasma is formed inside the Xe cluster and where the plasma temperature is determined by photoionization heating.