Optical creation of a supercrystal with three-dimensional nanoscale periodicity.

Stimulation with ultrafast light pulses can realize and manipulate states of matter with emergent structural, electronic and magnetic phenomena. However, these non-equilibrium phases are often transient and the challenge is to stabilize them as persistent states. Here, we show that atomic-scale PbTiO3/SrTiO3 superlattices, counterpoising strain and polarization states in alternate layers, are converted by sub-picosecond optical pulses to a supercrystal phase. This phase persists indefinitely under ambient conditions, has not been created via equilibrium routes, and can be erased by heating. X-ray scattering and microscopy show this unusual phase consists of a coherent three-dimensional structure with polar, strain and charge-ordering periodicities of up to 30 nm. By adjusting only dielectric properties, the phase-field model describes this emergent phase as a photo-induced charge-stabilized supercrystal formed from a two-phase equilibrium state. Our results demonstrate opportunities for light-activated pathways to thermally inaccessible and emergent metastable states.

Pump-probe spectrometer for measuring x-ray induced strain.

A hard x-ray pump-probe spectrometer using a multi-crystal Bragg reflector is demonstrated at a third generation synchrotron source. This device derives both broadband pump and monochromatic probe pulses directly from a single intense, broadband x-ray pulse centered at 8.767 keV. We present a proof-of-concept experiment which directly measures x-ray induced crystalline lattice strain.

X-ray photonic microsystems for the manipulation of synchrotron light.

Photonic microsystems played an essential role in the development of integrated photonic devices, thanks to their unique spatiotemporal control and spectral shaping capabilities. Similar capabilities to markedly control and manipulate X-ray radiation are highly desirable but practically impossible due to the massive size of the silicon single-crystal optics currently used. Here we show that micromechanical systems can be used as X-ray optics to create and preserve the spatial, temporal and spectral correlation of the X-rays. We demonstrate that, as X-ray reflective optics they can maintain the wavefront properties with nearly 100% reflectivity, and as a dynamic diffractive optics they can generate nanosecond time windows with over 100-kHz repetition rates. Since X-ray photonic microsystems can be easily incorporated into lab-based and next-generation synchrotron X-ray sources, they bring unprecedented design flexibility for future dynamic and miniature X-ray optics for focusing, wavefront manipulation, multicolour dispersion, and pulse slicing.

Bunch mode specific rate corrections for PILATUS3 detectors.

PILATUS X-ray detectors are in operation at many synchrotron beamlines around the world. This article reports on the characterization of the new PILATUS3 detector generation at high count rates. As for all counting detectors, the measured intensities have to be corrected for the dead-time of the counting mechanism at high photon fluxes. The large number of different bunch modes at these synchrotrons as well as the wide range of detector settings presents a challenge for providing accurate corrections. To avoid the intricate measurement of the count rate behaviour for every bunch mode, a Monte Carlo simulation of the counting mechanism has been implemented, which is able to predict the corrections for arbitrary bunch modes and a wide range of detector settings. This article compares the simulated results with experimental data acquired at different synchrotrons. It is found that the usage of bunch mode specific corrections based on this simulation improves the accuracy of the measured intensities by up to 40% for high photon rates and highly structured bunch modes. For less structured bunch modes, the instant retrigger technology of PILATUS3 detectors substantially reduces the dependency of the rate correction on the bunch mode. The acquired data also demonstrate that the instant retrigger technology allows for data acquisition up to 15 million photons per second per pixel.

Transient crystalline superlattice generated by a photoacoustic transducer.

Designing an efficient and simple method for modulating the intensity of x-ray radiation on a picosecond time-scale has the potential to produce ultrafast pulses of hard x-rays. In this work, we generate a tunable transient superlattice, in an otherwise perfect crystal, by photoexciting a metal film on a crystalline substrate. The resulting transient strain has amplitudes approaching 1%, wavevectors greater than [Formula: see text], and lifetimes approaching 1 ns. This method has the potential to generate isolated picosecond x-ray bursts with scattering efficiencies in excess of 10%.

Picosecond time-resolved laser pump/X-ray probe experiments using a gated single-photon-counting area detector.

The recent developments in X-ray detectors have opened new possibilities in the area of time-resolved pump/probe X-ray experiments; this article presents the novel use of a PILATUS detector to achieve X-ray pulse duration limited time-resolution at the Advanced Photon Source (APS), USA. The capability of the gated PILATUS detector to selectively detect the signal from a given X-ray pulse in 24 bunch mode at the APS storage ring is demonstrated. A test experiment performed on polycrystalline organic thin films of alpha-perylene illustrates the possibility of reaching an X-ray pulse duration limited time-resolution of 60 ps using the gated PILATUS detector. This is the first demonstration of X-ray pulse duration limited data recorded using an area detector without the use of a mechanical chopper array at the beamline.

Empirical dead-time corrections for synchrotron sources.

An experimental comparison of models for performing dead-time corrections of photon-counting detectors at synchrotron sources is presented. The performance of several detectors in the three operating modes of the Advanced Photon Source is systematically compared, with particular emphasis on asymmetric fill patterns. Several simple and well known correction formulas are evaluated. The results demonstrate the critical importance of detector speed and synchrotron fill pattern in selecting the proper dead-time correction.

Sculpting semiconductor heteroepitaxial islands: from dots to rods.

In the Ge on Si model heteroepitaxial system, metal patterns on the silicon surface provide unprecedented control over the morphology of highly ordered Ge islands. Island shape including nanorods and truncated pyramids is set by the metal species and substrate orientation. Analysis of island faceting elucidates the prominent role of the metal in promoting growth of preferred facet orientations while investigations of island composition and structure reveal the importance of Si-Ge intermixing in island evolution. These effects reflect a remarkable combination of metal-mediated growth phenomena that may be exploited to tailor the functionality of island arrays in heteroepitaxial systems.