Sub-micrometer focusing setup for high-pressure crystallography at the Extreme Conditions beamline at PETRA†III.

Scientific tasks aimed at decoding and characterizing complex systems and processes at high pressures set new challenges for modern X-ray diffraction instrumentation in terms of X-ray flux, focal spot size and sample positioning. Presented here are new developments at the Extreme Conditions beamline (P02.2, PETRA III, DESY, Germany) that enable considerable improvements in data collection at very high pressures and small scattering volumes. In particular, the focusing of the X-ray beam to the sub-micrometer level is described, and control of the aberrations of the focusing compound refractive lenses is made possible with the implementation of a correcting phase plate. This device provides a significant enhancement of the signal-to-noise ratio by conditioning the beam shape profile at the focal spot. A new sample alignment system with a small sphere of confusion enables single-crystal data collection from grains of micrometer to sub-micrometer dimensions subjected to pressures as high as 200 GPa. The combination of the technical development of the optical path and the sample alignment system contributes to research and gives benefits on various levels, including rapid and accurate diffraction mapping of samples with sub-micrometer resolution at multimegabar pressures.

Ptychographic characterisation of polymer compound refractive lenses manufactured by additive technology.

The recent success in the development of high-precision printing techniques allows one to manufacture free-standing polymer structures of high quality. Two-photon polymerization lithography is a mask-less technique with down to 100 nm resolution that provides full geometric freedom. It has recently been applied to the nanofabrication of X-ray compound refractive lenses (CRLs). In this article we report on the characterization of two sets of CRLs of different design produced by two-photon polymerization-induced lithography.

Pump-probe X-ray holographic imaging of laser-induced cavitation bubbles with femtosecond FEL pulses.

Cavitation bubbles can be seeded from a plasma following optical breakdown, by focusing an intense laser in water. The fast dynamics are associated with extreme states of gas and liquid, especially in the nascent state. This offers a unique setting to probe water and water vapor far-from equilibrium. However, current optical techniques cannot quantify these early states due to contrast and resolution limitations. X-ray holography with single X-ray free-electron laser pulses has now enabled a quasi-instantaneous high resolution structural probe with contrast proportional to the electron density of the object. In this work, we demonstrate cone-beam holographic flash imaging of laser-induced cavitation bubbles in water with nanofocused X-ray free-electron laser pulses. We quantify the spatial and temporal pressure distribution of the shockwave surrounding the expanding cavitation bubble at time delays shortly after seeding and compare the results to numerical simulations.

Direct imaging of ultrafast lattice dynamics.

Under rapid high-temperature, high-pressure loading, lattices exhibit complex elastic-inelastic responses. The dynamics of these responses are challenging to measure experimentally because of high sample density and extremely small relevant spatial and temporal scales. Here, we use an x-ray free-electron laser providing simultaneous in situ direct imaging and x-ray diffraction to spatially resolve lattice dynamics of silicon under high-strain rate conditions. We present the first imaging of a new intermediate elastic feature modulating compression along the axis of applied stress, and we identify the structure, compression, and density behind each observed wave. The ultrafast probe x-rays enabled time-resolved characterization of the intermediate elastic feature, which is leveraged to constrain kinetic inhibition of the phase transformation between 2 and 4 ns. These results not only address long-standing questions about the response of silicon under extreme environments but also demonstrate the potential for ultrafast direct measurements to illuminate new lattice dynamics.