Compact hard x-ray split-delay system based on variable-gap channel-cut crystals.

We present the concept and a prototypical implementation of a compact x-ray split-delay system that is capable of performing continuous on-the-fly delay scans over a range of ∼10 ps with sub-100 nanoradian pointing stability. The system consists of four channel-cut silicon crystals, two of which have gradually varying gap sizes from intentional 5 deg asymmetric cuts. The delay adjustment is realized by linear motions of these two monolithic varying-gap channel cuts, where the x-ray beam experiences pairs of anti-parallel reflections, and thus becomes less sensitive in output beam pointing to motion imperfections of the translation stages. The beam splitting is accomplished by polished crystal edges. A high degree of mutual coherence between the two branches at the focus is observed by analyzing small-angle coherent x-ray scattering patterns. We envision a wide range of applications including single-shot x-ray pulse temporal diagnostics, studies of high-intensity x-ray-matter interactions, as well as measurement of dynamics in disordered material systems using split-pulse x-ray photon correlation spectroscopy.

Characterization of the X-ray coherence properties of an undulator beamline at the Advanced Photon Source.

In anticipation of the increased use of coherent X-ray methods and the need to upgrade beamlines to match improved source quality, here the coherence properties of the X-rays delivered by beamline 12ID-D at the Advanced Photon Source have been characterized. The measured X-ray divergence, beam size, brightness and coherent flux at energies up to 26 keV are compared with the calculated values from the undulator source, and the effects of beamline optics such as a mirror, monochromator and compound refractive lenses are evaluated. Diffraction patterns from slits as a function of slit width are analyzed using wave propagation theory to obtain the beam divergence and thus coherence length. Imaging of the source using a compound refractive lens was found to be the most accurate method for determining the vertical divergence. While the brightness and coherent flux obtained without a monochromator (`pink beam') agree well with those calculated for the source, those measured with the monochromator were a factor of three to six lower than the source, primarily because of vertical divergence introduced by the monochromator. The methods described herein should be widely applicable for measuring the X-ray coherence properties of synchrotron beamlines.

Utilizing broadband X-rays in a Bragg coherent X-ray diffraction imaging experiment.

A method is presented to simplify Bragg coherent X-ray diffraction imaging studies of complex heterogeneous crystalline materials with a two-stage screening/imaging process that utilizes polychromatic and monochromatic coherent X-rays and is compatible with in situ sample environments. Coherent white-beam diffraction is used to identify an individual crystal particle or grain that displays desired properties within a larger population. A three-dimensional reciprocal-space map suitable for diffraction imaging is then measured for the Bragg peak of interest using a monochromatic beam energy scan that requires no sample motion, thus simplifying in situ chamber design. This approach was demonstrated with Au nanoparticles and will enable, for example, individual grains in a polycrystalline material of specific orientation to be selected, then imaged in three dimensions while under load.

Strain imaging of nanoscale semiconductor heterostructures with x-ray Bragg projection ptychography.

We report the imaging of nanoscale distributions of lattice strain and rotation in complementary components of lithographically engineered epitaxial thin film semiconductor heterostructures using synchrotron x-ray Bragg projection ptychography (BPP). We introduce a new analysis method that enables lattice rotation and out-of-plane strain to be determined independently from a single BPP phase reconstruction, and we apply it to two laterally adjacent, multiaxially stressed materials in a prototype channel device. These results quantitatively agree with mechanical modeling and demonstrate the ability of BPP to map out-of-plane lattice dilatation, a parameter critical to the performance of electronic materials.

Ultrafast photovoltaic response in ferroelectric nanolayers.

We show that light drives large-amplitude structural changes in thin films of the prototypical ferroelectric PbTiO3 via direct coupling to its intrinsic photovoltaic response. Using time-resolved x-ray scattering to visualize atomic displacements on femtosecond time scales, photoinduced changes in the unit-cell tetragonality are observed. These are driven by the motion of photogenerated free charges within the ferroelectric and can be simply explained by a model including both shift and screening currents, associated with the displacement of electrons first antiparallel to and then parallel to the ferroelectric polarization direction.

Framework for three-dimensional coherent diffraction imaging by focused beam x-ray Bragg ptychography.

We present the framework for convergent beam Bragg ptychography, and, using simulations, we demonstrate that nanocrystals can be ptychographically reconstructed from highly convergent x-ray Bragg diffraction. The ptychographic iterative engine is extended to three dimensions and shown to successfully reconstruct a simulated nanocrystal using overlapping raster scans with a defocused curved beam, the diameter of which matches the crystal size. This object reconstruction strategy can serve as the basis for coherent diffraction imaging experiments at coherent scanning nanoprobe x-ray sources.

Polarization switching without domain formation at the intrinsic coercive field in ultrathin ferroelectric PbTiO3.

Polarization switching in ferroelectrics has been thought to occur only through the nucleation and growth of new domains. Here we use in situ synchrotron x-ray scattering to monitor switching controlled by applied chemical potential. In sufficiently thin PbTiO3 films, nucleation is suppressed and switching occurs by a continuous mechanism, i.e., by uniform decrease and inversion of the polarization without domain formation. The observed lattice parameter shows that the electric field in the film during switching reaches the theoretical intrinsic coercive field.

Double-pulse speckle contrast correlations with near Fourier transform limited free-electron laser light using hard X-ray split-and-delay.

The ability to deliver two coherent X-ray pulses with precise time-delays ranging from a few femtoseconds to nanoseconds enables critical capabilities of probing ultra-fast phenomena in condensed matter systems at X-ray free electron laser (FEL) sources. Recent progress made in the hard X-ray split-and-delay optics developments now brings a very promising prospect for resolving atomic-scale motions that were not accessible by previous time-resolved techniques. Here, we report on characterizing the spatial and temporal coherence properties of the hard X-ray FEL beam after propagating through split-and-delay optics. Speckle contrast analysis of small-angle scattering measurements from nanoparticles reveals well-preserved transverse coherence of the beam. Measuring intensity fluctuations from successive X-ray pulses also reveals that only single or double temporal modes remain in the transmitted beam, corresponding to nearly Fourier transform limited pulses.

An instrument for in situ coherent x-ray studies of metal-organic vapor phase epitaxy of III-nitrides.

We describe an instrument that exploits the ongoing revolution in synchrotron sources, optics, and detectors to enable in situ studies of metal-organic vapor phase epitaxy (MOVPE) growth of III-nitride materials using coherent x-ray methods. The system includes high-resolution positioning of the sample and detector including full rotations, an x-ray transparent chamber wall for incident and diffracted beam access over a wide angular range, and minimal thermal sample motion, giving the sub-micron positional stability and reproducibility needed for coherent x-ray studies. The instrument enables surface x-ray photon correlation spectroscopy, microbeam diffraction, and coherent diffraction imaging of atomic-scale surface and film structure and dynamics during growth, to provide fundamental understanding of MOVPE processes.

Atomic layer engineering of perovskite oxides for chemically sharp heterointerfaces.

Atomic layer engineering enables fabrication of a chemically sharp oxide heterointerface. The interface formation and strain evolution during the initial growth of LaAlO(3) /SrTiO(3) heterostructures by pulsed laser deposition are investigated in search of a means for controlling the atomic-sharpness of the interface. This study shows that inserting a monolayer of LaAlO(3) grown at high oxygen pressure dramatically enhances interface abruptness.

Ferroelectricity in ultrathin perovskite films.

Understanding the suppression of ferroelectricity in perovskite thin films is a fundamental issue that has remained unresolved for decades. We report a synchrotron x-ray study of lead titanate as a function of temperature and film thickness for films as thin as a single unit cell. At room temperature, the ferroelectric phase is stable for thicknesses down to 3 unit cells (1.2 nanometers). Our results imply that no thickness limit is imposed on practical devices by an intrinsic ferroelectric size effect.