Graphite resistive heated diamond anvil cell for simultaneous high-pressure and high-temperature diffraction experiments.

High-pressure and high-temperature experiments using a resistively heated diamond anvil cell have the advantage of heating samples homogeneously with precise temperature control. Here, we present the design and performance of a graphite resistive heated diamond anvil cell (GRHDAC) setup for powder and single-crystal x-ray diffraction experiments developed at the Extreme Conditions Beamline (P02.2) at PETRA III, Hamburg, Germany. In the GRHDAC, temperatures up to 2000 K can be generated at high pressures by placing it in a water-cooled vacuum chamber. Temperature estimates from thermocouple measurements are within +/-35 K at the sample position up to 800 K and within +90 K between 800 and 1400 K when using a standard seat combination of cBN and WC. Isothermal compression at high temperatures can be achieved by employing a remote membrane control system. The advantage of the GRHDAC is demonstrated through the study of geophysical processes in the Earth's crust and upper mantle region.

Orientation order of a nonpolar molecular fluid compressed into a nanosmall space.

The ordering structures of non-polar carbon tetrachloride liquid compressed to nano-scales between parallel substrates is studied in this work. The theoretical considerations show that the potential well formed by the confined parallel substrates induces orientational ordering of non-polar molecules. Through molecular dynamic (MD) simulations, the relations between various ordered structures of a non-polar liquid (carbon tetrachloride) and the confined gap size are demonstrated. The density distribution shows that the confinement does affect the ordering modes and induces an orientational ordering of molecules at the solid-liquid interface under extreme confinement conditions. This molecular orientation suggested from the theoretical model and MD simulation is directly supported by the experimental studies for the first time. The X-ray reflectivity data reveal a strong layering effect with splitting of the density profile in C and Cl-rich sublayers. The investigation shows that the liquid structure factor in confinement has a characteristic length similar to the short-range ordering in bulk, but the confined structure is strongly influenced by the surface potential and the interface properties. This introduces preferred molecular orientation and ordering which are not favorable in the bulk phase. As the orientational ordering is closely related to crystallization, our results provide a new perspective to control the crystallization in nano-confined space by compression.

Laser heating system at the Extreme Conditions Beamline, P02.2, PETRA III.

A laser heating system for samples confined in diamond anvil cells paired with in situ X-ray diffraction measurements at the Extreme Conditions Beamline of PETRA III is presented. The system features two independent laser configurations (on-axis and off-axis of the X-ray path) allowing for a broad range of experiments using different designs of diamond anvil cells. The power of the continuous laser source can be modulated for use in various pulsed laser heating or flash heating applications. An example of such an application is illustrated here on the melting curve of iron at megabar pressures. The optical path of the spectroradiometry measurements is simulated with ray-tracing methods in order to assess the level of present aberrations in the system and the results are compared with other systems, that are using simpler lens optics. Based on the ray-tracing the choice of the first achromatic lens and other aspects for accurate temperature measurements are evaluated.

Single-crystal diffractometer coupled with double-sided laser heating system at the Extreme Conditions Beamline P02.2 at PETRAIII.

Combination of in situ laser heating with single-crystal X-ray diffraction (scXRD) in diamond anvil cells (DACs) provides a tool to study crystal structures and/or chemistry of materials at simultaneous high pressures and high temperatures. Here, we describe the first dedicated single-crystal X-ray diffractometer coupled with double-sided laser heating (dsLH) system. The scXRD/dsLH setup was developed for the P02.2 Extreme Conditions Beamline at PETRA III and became available for general users in 2017. It enables the collection of reliable scXRD data at simultaneous high pressure and high temperature. We demonstrate the performance of the setup on example of studies of iron and chromium nitrides.

Experimental Observation of Crystal-Liquid Coexistence in Slit-Confined Nonpolar Fluids.

Films of carbon tetrachloride (CCl4) confined in slit geometry between two flat diamond substrates down to a few tens of Angstroms are studied by combining X-ray reflectivity with in-plane and out-of-plane X-ray scattering. The confined films form a heterogeneous structure with coexisting regions of liquid and crystalline phases. The liquid phase shows short-range ordering normal to the surfaces of the substrates. The experiments directly show the ability of the confinement to induce crystal objects, which is a long-discussed issue in the literature. The surface structure and morphology of the substrates may influence the actual realization of the crystalline phase in confinement.

A new setup for high resolution fast X-ray reflectivity data acquisition.

A new method for fast x-ray reflectivity data acquisition is presented. The method is based on a fast rotating, slightly tilted sample reflecting to a stationary mounted position sensitive detector and it allows for measurements of reflectivity curves in a quarter of a second. The resolution in q-space mainly depends on the beam properties and the pixel size of the detector. Maximum qz-value of 1 Å-1 can be achieved. The time-temperature depending structure changes of poly(N-isopropylacrylamide) thin films were investigated in situ by applying the fast-reflectivity setup. The results are presented in this paper as illustration of the method and proof of principle.

Development of a hard X-ray delay line for X-ray photon correlation spectroscopy and jitter-free pump-probe experiments at X-ray free-electron laser sources.

A hard X-ray delay line capable of splitting and delaying single X-ray pulses has been developed with the aim of performing X-ray photon correlation spectroscopy (XPCS) and X-ray pump-probe experiments at hard X-ray free-electron laser sources. The performance of the device was tested with 8.39 keV synchrotron radiation. Time delays up to 2.95 ns have been demonstrated. The feasibility of the device for performing XPCS studies was tested by recording static speckle patterns. The achieved speckle contrast of 56% indicates the possibility of performing ultra-fast XPCS studies with the delay line.

Performance of a picosecond x-ray delay line unit at 8.39 keV.

A prototype device capable of splitting an x-ray pulse into two adjustable fractions, delaying one of them with the aim to perform x-ray photon correlation spectroscopy and pump-probe type studies, was designed, manufactured, and tested. The device utilizes eight perfect silicon crystals in vertical 90 degrees scattering geometry. Its performance has been verified with 8.39 keV synchrotron radiation. The measured throughput of the device with a Si(333) premonochromator at 8.39 keV under ambient conditions is 0.6%. Time delays up to 2.62 ns have been achieved, detected with a time resolution of 16.7 ps.