A modular table-top setup for ultrafast x-ray diffraction.

We present a table-top setup for femtosecond time-resolved x-ray diffraction based on a Cu Kα (8.05 keV) laser driven plasma x-ray source. Due to its modular design, it provides high accessibility to its individual components (e.g., x-ray optics and sample environment). The Kα-yield of the source is optimized using a pre-pulse scheme. A magnifying multilayer x-ray mirror with Montel-Helios geometry is used to collect the emitted radiation, resulting in a quasi-collimated flux of more than 105 Cu Kα photons/pulse impinging on the sample under investigation at a repetition rate of 10 Hz. A gas ionization chamber detector is placed right after the x-ray mirror and used for the normalization of the diffraction signals, enabling the measurement of relative signal changes of less than 1% even at the given low repetition rate. Time-resolved diffraction experiments on laser-excited epitaxial Bi films serve as an example to demonstrate the capabilities of the setup. The setup can also be used for Debye-Scherrer type measurements on poly-crystalline samples.

Time-resolved diffraction with an optimized short pulse laser plasma X-ray source.

We present a setup for time-resolved X-ray diffraction based on a short pulse, laser-driven plasma X-ray source. The employed modular design provides high flexibility to adapt the setup to the specific requirements (e.g., X-ray optics and sample environment) of particular applications. The configuration discussed here has been optimized toward high angular/momentum resolution and uses K α -radiation (4.51 keV) from a Ti wire-target in combination with a toroidally bent crystal for collection, monochromatization, and focusing of the emitted radiation. 2 × 10 5 Ti-K α1 photons per pulse with 10 - 4 relative bandwidth are delivered to the sample at a repetition rate of 10 Hz. This allows for the high dynamic range (104) measurements of transient changes in the rocking curves of materials as for example induced by laser-triggered strain waves.

Optimized Kalpha x-ray flashes from femtosecond-laser-irradiated foils.

We investigate the generation of ultrashort Kalpha pulses from plasmas produced by intense femtosecond p-polarized laser pulses on Copper and Titanium targets. Particular attention is given to the interplay between the angle of incidence of the laser beam on the target and a controlled prepulse. It is observed experimentally that the Kalpha yield can be optimized for correspondingly different prepulse and plasma scale-length conditions. For steep electron-density gradients, maximum yields can be achieved at larger angles. For somewhat expanded plasmas expected in the case of laser pulses with a relatively poor contrast, the Kalpha yield can be enhanced by using a near-normal-incidence geometry. For a certain scale-length range (between 0.1 and 1 times a laser wavelength) the optimized yield is scale-length independent. Physically this situation arises because of the strong dependence of collisionless absorption mechanisms-in particular resonance absorption-on the angle of incidence and the plasma scale length, giving scope to optimize absorption and hence the Kalpha yield. This qualitative description is supported by calculations based on the classical resonance absorption mechanism and by particle-in-cell simulations. Finally, the latter simulations also show that even for initially steep gradients, a rapid profile expansion occurs at oblique angles in which ions are pulled back toward the laser by hot electrons circulating at the front of the target. The corresponding enhancement in Kalpha yield under these conditions seen in the present experiment represents strong evidence for this suprathermal shelf formation effect.

Toward ultrafast time-resolved Debye-Scherrer x-ray diffraction using a laser-plasma source.

An elliptical glass capillary has been used to focus ultrashort Cu K alpha x-ray pulses emitted from a femtosecond laser-produced plasma. Due to its high magnification (7x), the optic transforms the divergent x-ray emission of the plasma into a quasicollimated x-ray beam with a divergence of only 0.18 degrees. As an application we demonstrate the possibility to perform Debye-Scherrer diffraction experiments with the simultaneous detection of several diffraction orders. This will allow one to extend time-resolved x-ray diffraction with femtosecond laser-plasma x-ray sources to a much wider range of materials, which are not easily available as single crystals.

X-ray diffuse scattering measurements of nucleation dynamics at femtosecond resolution.

Femtosecond time-resolved small and wide angle x-ray diffuse scattering techniques are applied to investigate the ultrafast nucleation processes that occur during the ablation process in semiconducting materials. Following intense optical excitation, a transient liquid state of high compressibility characterized by large-amplitude density fluctuations is observed and the buildup of these fluctuations is measured in real time. Small-angle scattering measurements reveal snapshots of the spontaneous nucleation of nanoscale voids within a metastable liquid and support theoretical predictions of the ablation process.

Ultrafast bond softening in bismuth: mapping a solid's interatomic potential with X-rays.

Intense femtosecond laser excitation can produce transient states of matter that would otherwise be inaccessible to laboratory investigation. At high excitation densities, the interatomic forces that bind solids and determine many of their properties can be substantially altered. Here, we present the detailed mapping of the carrier density-dependent interatomic potential of bismuth approaching a solid-solid phase transition. Our experiments combine stroboscopic techniques that use a high-brightness linear electron accelerator-based x-ray source with pulse-by-pulse timing reconstruction for femtosecond resolution, allowing quantitative characterization of the interatomic potential energy surface of the highly excited solid.