Evidence of Extreme Ultraviolet Superfluorescence in Xenon.

We present a comprehensive experimental and theoretical study on superfluorescence in the extreme ultraviolet wavelength regime. Focusing a free-electron laser pulse in a cell filled with Xe gas, the medium is quasi-instantaneously population inverted by 4d-shell ionization on the giant resonance followed by Auger decay. On the timescale of ∼10 ps to ∼100 ps (depending on parameters) a macroscopic polarization builds up in the medium, resulting in superfluorescent emission of several Xe lines in the forward direction. As the number of emitters in the system is increased by either raising the pressure or the pump-pulse energy, the emission yield grows exponentially over four orders of magnitude and reaches saturation. With increasing yield, we observe line broadening, a manifestation of superfluorescence in the spectral domain. Our novel theoretical approach, based on a full quantum treatment of the atomic system and the irradiated field, shows quantitative agreement with the experiment and supports our interpretation.

High-harmonic probing of electronic coherence in dynamically aligned molecules.

We introduce and demonstrate a new approach to measuring coherent electron wave packets using high-harmonic spectroscopy. By preparing a molecule in a coherent superposition of electronic states, we show that electronic coherence opens previously unobserved high-harmonic-generation channels that connect distinct but coherently related electronic states. Performing the measurements in dynamically aligned nitric oxide molecules we observe the complex temporal evolution of the electronic coherence under coupling to nuclear motion. Choosing a weakly allowed transition to prepare the wave packet, we demonstrate an unprecedented sensitivity that arises from optical interference between coherent and incoherent pathways. This mechanism converts a 0.1% excitation fraction into a ∼20% signal modulation.

Resonant Kα spectroscopy of solid-density aluminum plasmas.

The x-ray intensities made available by x-ray free electron lasers (FEL) open up new x-ray matter interaction channels not accessible with previous sources. We report here on the resonant generation of Kα emission, that is to say the production of copious Kα radiation by tuning the x-ray FEL pulse to photon energies below that of the K edge of a solid aluminum sample. The sequential absorption of multiple photons in the same atom during the 80 fs pulse, with photons creating L-shell holes and then one resonantly exciting a K-shell electron into one of these holes, opens up a channel for the Kα production, as well as the absorption of further photons. We demonstrate rich spectra of such channels, and investigate the emission produced by tuning the FEL energy to the K-L transitions of those highly charged ions that have transition energies below the K edge of the cold material. The spectra are sensitive to x-ray intensity dependent opacity effects, with ions containing L-shell holes readily reabsorbing the Kα radiation.

Unveiling and driving hidden resonances with high-fluence, high-intensity x-ray pulses.

We show that high fluence, high-intensity x-ray pulses from the world's first hard x-ray free-electron laser produce nonlinear phenomena that differ dramatically from the linear x-ray-matter interaction processes that are encountered at synchrotron x-ray sources. We use intense x-ray pulses of sub-10-fs duration to first reveal and subsequently drive the 1s↔2p resonance in singly ionized neon. This photon-driven cycling of an inner-shell electron modifies the Auger decay process, as evidenced by line shape modification. Our work demonstrates the propensity of high-fluence, femtosecond x-ray pulses to alter the target within a single pulse, i.e., to unveil hidden resonances, by cracking open inner shells energetically inaccessible via single-photon absorption, and to consequently trigger damaging electron cascades at unexpectedly low photon energies.

Nonlinear atomic response to intense ultrashort x rays.

The nonlinear absorption mechanisms of neon atoms to intense, femtosecond kilovolt x rays are investigated. The production of Ne(9+) is observed at x-ray frequencies below the Ne(8+), 1s(2) absorption edge and demonstrates a clear quadratic dependence on fluence. Theoretical analysis shows that the production is a combination of the two-photon ionization of Ne(8+) ground state and a high-order sequential process involving single-photon production and ionization of transient excited states on a time scale faster than the Auger decay. We find that the nonlinear direct two-photon ionization cross section is orders of magnitude higher than expected from previous calculations.

Design and measurement of a Cu L-edge x-ray filter for free electron laser pumped x-ray laser experiments.

An inner-shell photoionized x-ray laser pumped by the Linac Coherent Light Source (LCLS) free electron laser has been proposed recently. The measurement of the on-axis 849 eV Ne Kα laser and protection of the x-ray spectrometer from damage require attenuation of the 1 keV LCLS beam. An Al/Cu foil combination is well suited, serving as a low energy bandpass filter below the Cu L-edge at 933 eV. A high resolution grating spectrometer is used to measure the transmission of a candidate filter with an intense laser-produced x-ray backlighter developed at the Lawrence Livermore National Laboratory Jupiter Laser Facility Janus. The methodology and discussion of the observed fine structure above the Cu L-edge will be presented.

Femtosecond electronic response of atoms to ultra-intense X-rays.

An era of exploring the interactions of high-intensity, hard X-rays with matter has begun with the start-up of a hard-X-ray free-electron laser, the Linac Coherent Light Source (LCLS). Understanding how electrons in matter respond to ultra-intense X-ray radiation is essential for all applications. Here we reveal the nature of the electronic response in a free atom to unprecedented high-intensity, short-wavelength, high-fluence radiation (respectively 10(18) W cm(-2), 1.5-0.6 nm, approximately 10(5) X-ray photons per A(2)). At this fluence, the neon target inevitably changes during the course of a single femtosecond-duration X-ray pulse-by sequentially ejecting electrons-to produce fully-stripped neon through absorption of six photons. Rapid photoejection of inner-shell electrons produces 'hollow' atoms and an intensity-induced X-ray transparency. Such transparency, due to the presence of inner-shell vacancies, can be induced in all atomic, molecular and condensed matter systems at high intensity. Quantitative comparison with theory allows us to extract LCLS fluence and pulse duration. Our successful modelling of X-ray/atom interactions using a straightforward rate equation approach augurs favourably for extension to complex systems.