Towards ultrafast dynamics with split-pulse X-ray photon correlation spectroscopy at free electron laser sources.

One of the important challenges in condensed matter science is to understand ultrafast, atomic-scale fluctuations that dictate dynamic processes in equilibrium and non-equilibrium materials. Here, we report an important step towards reaching that goal by using a state-of-the-art perfect crystal based split-and-delay system, capable of splitting individual X-ray pulses and introducing femtosecond to nanosecond time delays. We show the results of an ultrafast hard X-ray photon correlation spectroscopy experiment at LCLS where split X-ray pulses were used to measure the dynamics of gold nanoparticles suspended in hexane. We show how reliable speckle contrast values can be extracted even from very low intensity free electron laser (FEL) speckle patterns by applying maximum likelihood fitting, thus demonstrating the potential of a split-and-delay approach for dynamics measurements at FEL sources. This will enable the characterization of equilibrium and, importantly also reversible non-equilibrium processes in atomically disordered materials.

The Extreme Conditions Beamline P02.2 and the Extreme Conditions Science Infrastructure at PETRA III.

A detailed description is presented of the Extreme Conditions Beamline P02.2 for micro X-ray diffraction studies of matter at simultaneous high pressure and high/low temperatures at PETRA III, in Hamburg, Germany. This includes performance of the X-ray optics and instrumental resolution as well as an overview of the different sample environments available for high-pressure studies in the diamond anvil cell. Particularly emphasized are the high-brilliance and high-energy X-ray diffraction capabilities of the beamline in conjunction with the use of fast area detectors to conduct time-resolved compression studies in the millisecond time regime. Finally, the current capability of the Extreme Conditions Science Infrastructure to support high-pressure research at the Extreme Conditions Beamline and other PETRA III beamlines is described.

Resonant scattering and diffraction beamline P09 at PETRA III.

The resonant scattering and diffraction beamline P09 at PETRA III is designed for X-ray experiments requiring small beams, energy tunability, variable polarization and high photon flux. It is highly flexible in terms of beam size and offers full higher harmonic suppression. A state-of-the-art double phase-retarder set-up provides variable linear or circular polarization. A high-precision Psi-diffractometer and a heavy-load diffractometer in horizontal Psi-geometry allow the accommodation of a wide variety of sample environments. A 14 T cryo-magnet is available for scattering experiments in magnetic fields.

The high-resolution diffraction beamline P08 at PETRA III.

The new third-generation synchrotron radiation source PETRA III located at the Deutsches Elektronen-Synchrotron DESY in Hamburg, Germany, has been operational since the second half of 2009. PETRA III is designed to deliver hard X-ray beams with very high brilliance. As one of the first beamlines of PETRA III the high-resolution diffraction beamline P08 is fully operational. P08 is specialized in X-ray scattering and diffraction experiments on solids and liquids where extreme high resolution in reciprocal space is required. The resolving power results in the high-quality PETRA III beam and unique optical elements such as a large-offset monochromator and beryllium lens changers. A high-precision six-circle diffractometer for solid samples and a specially designed liquid diffractometer are installed in the experimental hutch. Regular users have been accepted since summer 2010.

Observation of structural anisotropy and the onset of liquidlike motion during the nonthermal melting of InSb.

The melting dynamics of laser excited InSb have been studied with femtosecond x-ray diffraction. These measurements observe the delayed onset of diffusive atomic motion, signaling the appearance of liquidlike dynamics. They also demonstrate that the root-mean-squared displacement in the [111] direction increases faster than in the [110] direction after the first 500 fs. This structural anisotropy indicates that the initially generated fluid differs significantly from the equilibrium liquid.

Clocking femtosecond X rays.

Linear-accelerator-based sources will revolutionize ultrafast x-ray science due to their unprecedented brightness and short pulse duration. However, time-resolved studies at the resolution of the x-ray pulse duration are hampered by the inability to precisely synchronize an external laser to the accelerator. At the Sub-Picosecond Pulse Source at the Stanford Linear-Accelerator Center we solved this problem by measuring the arrival time of each high energy electron bunch with electro-optic sampling. This measurement indirectly determined the arrival time of each x-ray pulse relative to an external pump laser pulse with a time resolution of better than 60 fs rms.

Atomic-scale visualization of inertial dynamics.

The motion of atoms on interatomic potential energy surfaces is fundamental to the dynamics of liquids and solids. An accelerator-based source of femtosecond x-ray pulses allowed us to follow directly atomic displacements on an optically modified energy landscape, leading eventually to the transition from crystalline solid to disordered liquid. We show that, to first order in time, the dynamics are inertial, and we place constraints on the shape and curvature of the transition-state potential energy surface. Our measurements point toward analogies between this nonequilibrium phase transition and the short-time dynamics intrinsic to equilibrium liquids.

Beam-position monitors in the X-ray undulator beamline at PETRA.

At the 12 GeV storage ring PETRA, the first synchrotron radiation beamline uses a 4 m-long undulator. The beamline, with a length of 130 m between source and sample, delivers hard X-ray photons usable up to 300 keV. The photon beam has a total power of 7 kW. Combined with the high brilliance, the powerful beam is very critical for all beamline components. Copper, located at a distance of 26 m, hit by the full undulator beam, melts within 20 ms. Different monitors are described for stable, safe and reliable operation of beam and experiments.

Adaptive indirectly cooled monochromator crystals at HASYLAB.

The high-heat-load monochromator, based on the HASYLAB (Hamburger Synchrotronstrahlungslabor) 'Torii' design, has been used successfully for 2 years at the BW2 wiggler beamline. The bowing of the reflecting surface induced by the heat load and water pressure is compensated mechanically. This is achieved by mounting the specially shaped crystal in a bending mechanism and by heat transfer from the directly water-cooled crystal. We present the latest step in the development of this design. The piezoceramic-driven actuators are replaced by actuators based on the thermal expansion of copper rods. The direct water cooling of the crystal is replaced by a safer indirect water-cooling scheme. Characterization results of the crystal are presented. The Si(111) rocking-curve width at 9.5 keV was measured to be 8.3 arcsec under 500 W heat load.

Measurements of emittance and absolute spectral flux of the PETRA undulator at DESY Hamburg.

The first synchrotron radiation beamline using a 4 m-long undulator at the 12 GeV storage ring PETRA delivers hard X-ray photons usable up to 300 keV. The photon intensity is measured on an absolute scale in the energy range between 16 and 60 keV and compared with calculated intensities. The experimental set-up described is also used to measure the horizontal and vertical emittance of the source.

Adaptive Silicon Monochromators for High-Power Insertion Devices. Tests at CHESS, ESRF and HASYLAB.

X-ray wigglers which produce tens of kilowatts of photon power within the white beam will soon become available at third-generation sources of synchrotron radiation. Insertion devices that produce several kilowatts already exist and we have used those at CHESS, ESRF and HASYLAB to test adaptive 111 silicon water-jet-cooled monochromators at up to 2 kW total incident beam power. This development from earlier work at the Brookhaven National Synchrotron Light Source (NSLS) uses the pressure in the water coolant to provide active compensation of the strain field in the thermal footprint, nulling its effect to within residual variations in Bragg angle of only a few arc s. The design is robust, vacuum compatible and uses no moving mechanical parts.