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Photoionization by an eXtreme UltraViolet (XUV) attosecond pulse train (APT) in the presence of an infrared pulse (RABBITT method) conveys information about the atomic photoionization delay. By taking the difference of the spectral delays between pairs of rare gases (Ar,He), (Kr,He) and (Ne,He) it is possible to eliminate in each case the larger group delay ('attochirp') associated with the APT itself and obtain the Ar, Kr and Ne Wigner delays referenced to model calculations of the He delay. In this work we measure how the delays vary as a function of XUV photon energy but we cannot determine the absolute delay difference between atoms due to lack of precise knowledge of the initial conditions. The extracted delays are compared with several theoretical predictions and the results are consistent within 30 as over the energy range from 10 to 50 eV. An 'effective' Wigner delay over all emission angles is found to be more consistent with our angle-integrated measurement near the Cooper minimum in Ar. We observe a few irregular features in the delay that may be signatures of resonances., AuthorCount:7

Here we present the first angle-resolved, non-resonant (normal) Auger spectra for impulsively aligned nitrogen molecules. We have measured the angular pattern of Auger electron emission following K -shell photoionization by 1.1 keV photons from the Linac Coherent Light Source (LCLS). Using strong-field-induced molecular alignment to make molecular frame measurements is equally effective for both repulsive and quasi-bound final states. The capability to resolve Auger emission angular distributions in the molecular frame of reference provides a new tool for spectral assignments in congested Auger electron spectra that takes advantage of the symmetries of the final diction states. Based on our experimental results and theoretical predictions, we propose the assignment of the spectral features in the Auger electron spectrum.

Explosions of large Xe clusters (< N > similar to 11 000) irradiated by femtosecond pulses of 850 eV x-ray photons focused to an intensity of up to 1017 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.

The Linac Coherent Light Source free electron laser is a source of high brightness x rays, 2×1011 photons in a ∼5 fs pulse, that can be focused to produce double core vacancies through rapid sequential ionization. This enables double core vacancy Auger electron spectroscopy, an entirely new way to study femtosecond chemical dynamics with Auger electrons that probe the local valence structure of molecules near a specific atomic core. Using 1.1 keV photons for sequential x-ray ionization of impulsively aligned molecular nitrogen, we observed a rich single-site double core vacancy Auger electron spectrum near 413 eV, in good agreement with ab initio calculations, and we measured the corresponding Auger electron angle dependence in the molecular frame.

The first time-resolved x-ray/optical pump-probe experiments at the SLAC Linac Coherent Light Source (LCLS) used a combination of feedback methods and post-analysis binning techniques to synchronize an ultrafast optical laser to the linac-based x-ray laser. Transient molecular nitrogen alignment revival features were resolved in time-dependent x-ray-induced fragmentation spectra. These alignment features were used to find the temporal overlap of the pump and probe pulses. The strong-field dissociation of x-ray generated quasi-bound molecular dications was used to establish the residual timing jitter. This analysis shows that the relative arrival time of the Ti:Sapphire laser and the x-ray pulses had a distribution with a standard deviation of approximately 120 fs. The largest contribution to the jitter noise spectrum was the locking of the laser oscillator to the reference RF of the accelerator, which suggests that simple technical improvements could reduce the jitter to better than 50 fs.

Photo-double ionization (PDI) of xenon by the Ti: Sapphire laser fundamental frequency combined to its 19th and 25th harmonics has been studied by means of a momentum imaging spectrometer. The measurement of the two emitted photoelectrons' momenta and their energy and angular correlations gives insight into the various mechanisms leading to PDI. Although the conditions for non-sequential direct photo-double ionization are fulfilled in the experiment, it is found that the two-step processes dominate.