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When one performs a coherent small-angle X-ray scattering experiment, the incident beam must be spatially filtered by slits on a length scale smaller than the transverse coherence length of the source which is typically around 10 microm. The Fraunhofer diffraction pattern of the slit is one of the important sources of background in these experiments. New slits which minimize this parasitic background have been designed and tested. The slit configuration apodizes the beam by the use of partially transmitting inclined slit jaws. A model is presented which predicts that the high wavevector tails of the diffraction pattern fall as the inverse fourth power of the wavevector instead of the inverse second power that is observed for standard slits. Using cleaved GaAs single-crystal edges, Fraunhofer diffraction patterns from 3 and 5.5 keV X-rays were measured, in agreement with the theoretical model proposed. A novel phase-peak diffraction pattern associated with phase variations of the transmitted electric field was also observed. The model proposed adequately accounts for this phenomenon.

Nonlinear effects in the coupling of polarization with elastic strain have been predicted to occur in ferroelectric materials subjected to high electric fields. Such predictions are tested here for a PbZr0.2Ti0.8O3 ferroelectric thin film at electric fields in the range of several hundred MV/m and strains reaching up to 2.7%. The piezoelectric strain exceeds predictions based on constant piezoelectric coefficients at electric fields from approximately 200 to 400 MV/m, which is consistent with a nonlinear effect predicted to occur at corresponding piezoelectric distortions.

Time scales of long-range physical processes in solids are typically in the range of picoseconds to nanoseconds. These times are commensurate with the time resolution of structural probes based on modern synchrotron x-ray sources. Several processes of technological and scientific interest can be driven by applied electric fields, but synchronizing electrically driven phenomena with an x-ray probe poses a technical challenge. We describe the synchronization of a well-defined number of fast electrical pulses with the time structure of synchrotron x rays to probe the dynamics of thin films and nanostructures. This synchronization technique yields x-ray transient signals with 600 ps transitions in ferroelectric thin films, with a contribution of approximately 320 ps due to timing jitter in the synchronization.

We have developed a synchrotron-based, time-resolved x-ray microprobe to investigate optical strong-field processes at intermediate intensities (10(14) - 10(15) W/cm2). This quantum-state specific probe has enabled the direct observation of orbital alignment in the residual ion produced by strong-field ionization of krypton atoms via resonant, polarized x-ray absorption. We found strong alignment to persist for a period long compared to the spin-orbit coupling time scale (6.2 fs). The observed degree of alignment can be explained by models that incorporate spin-orbit coupling. The methodology is applicable to a wide range of problems.

Domain wall motion during polarization switching in ferroelectric thin films is fundamentally important and poses challenges for both experiments and modeling. We have visualized the switching of a Pb(Zr, Ti)O(3) capacitor using time-resolved x-ray microdiffraction. The structural signatures of switching include a reversal in the sign of the piezoelectric coefficient and a change in the intensity of x-ray reflections. The propagation of polarization domain walls is highly reproducible from cycle to cycle of the electric field. Domain wall velocities of 40 m s(-1) are consistent with the results of other methods, but are far less than saturation values expected at high electric fields.

Ultrafast X-ray experiments at synchrotron sources hold tremendous promise for measuring the atomistic dynamics of materials under a wide variety of transient conditions. In particular, the marriage of synchrotron radiation and ultrafast laser technology is opening up a new frontier of materials research. Structural changes initiated by femtosecond laser pulses can be tracked in real time using time-resolved X-ray diffraction on picosecond time scales or shorter. Here, research at the Advanced Photon Source is described, illustrating the opportunities for ultrafast diffraction with some recent work on the generation of impulsive strain, coherent phonon generation and supersonic diffusion of electron-hole plasmas. The flexibility of time-resolved Bragg and Laue diffraction geometries are both utilized to illuminate the strain generation and evolution process. Time-resolved X-ray science will become increasingly important with the construction of linac-based ultrafast X-ray sources.

The order-disorder phase transition in Cu3Au has been studied by x-ray intensity fluctuation spectroscopy. Following a quench from the high-temperature, disordered phase, the ordering kinetics is well described by a universal scaling form that can be measured by time-resolved (incoherent) x-ray scattering. By using coherent scattering, we have measured the fluctuations about this universal scaling form. In the late stages of the ordering process, these fluctuations give a two-time correlation function C(q,t1,t2) which has a scaling form with natural variables deltat=/t1-t2/ and t =(t1+t2) / 2. The scaling form crosses over from linear in t to t1/2. These present the first such results for a nonconserved system.

Ferroelectric oxides, such as Pb(Zr,Ti)O(3), are useful for electronic and photonic devices because of their ability to retain two stable polarization states, which can form the basis for memory and logic circuitry. Requirements for long-term operation of practical devices such as non-volatile RAM (random access memory) include consistent polarization switching over many (more than 10(12)) cycles of the applied electric field, which represents a major challenge. As switching is largely controlled by the motion and pinning of domain walls, it is necessary to develop suitable tools that can directly probe the ferroelectric domain structures in operating devices-thin-film structures with electrical contacts. A recently developed synchrotron X-ray microdiffraction technique complements existing microscopic probes, and allows us to visualize directly the evolution of polarization domains in ferroelectric devices, through metal or oxide electrodes, and with submicrometre spatial resolution. The images reveal two regimes of fatigue, depending on the magnitude of the electric field pulses driving the device: a low-field regime in which fatigue can be reversed with higher electric field pulses, and a regime at very high electric fields in which there is a non-reversible crystallographic relaxation of the epitaxial ferroelectric film.

We measure transient strain in ultrafast laser-excited Ge by time-resolved x-ray anomalous transmission. The development of the coherent strain pulse is dominated by rapid ambipolar diffusion. This pulse extends considerably longer than the laser penetration depth because the plasma initially propagates faster than the acoustic modes. X-ray diffraction simulations are in agreement with the observed dynamics.

Obtaining accurate structural information on epitaxial films and interfaces is nowhere more critical than in semiconductor passivation layers, where details of the atomic structure and bonding determine the nature of the interface electronic states. Various non-destructive methods have been used to investigate the structure of films and interfaces, but their interpretation is model-dependent, leading occasionally to wrong conclusions. We have developed a new X-ray method for the direct determination of epitaxial structures, coherent Bragg rod analysis (COBRA). The usefulness of our technique is demonstrated by mapping, with atomic precision, the structure of the interfacial region of a Gd2O3 film grown epitaxially on a (100) GaAs substrate. Our findings reveal interesting behaviour not previously suggested by existing structural methods, in particular a lock-in of the in-plane Gd atomic positions to those of the Ga/As atoms of the substrate. Moreover, we find that the bulk stacking of the Gd2O3 atomic layers is abandoned in favour of a new structure that is directly correlated with the stacking sequence of the substrate. These results have important implications for Gd2O3 as an effective passivation layer for GaAs (ref. 7). Our work shows that the COBRA technique, taking advantage of the brilliance of insertion device synchrotron X-ray sources, is widely applicable to epitaxial films and interfaces.

We report on a small-angle x-ray scattering study of the hexane-nitrobenzene binary fluid mixture near its critical point. The use of an ultrabright x-ray undulator synchrotron source enabled us to measure the temperature dependence of the static structure factor with unprecedented contrast, and the large coherent flux of this source provided a probe for the fluctuation dynamics via the x-ray photon correlation spectroscopy technique. We find that the intensity and correlation lengths diverge with the expected three-dimensional Ising critical exponents, and the dynamical correlation function decays exponentially with correlation times as small as 250 micros. In the range of wave vector studied here (1.2-2.6 x 10(-3) A(-1)) the concentration fluctuations relaxed diffusively with a diffusion constant consistent with that determined from visible light scattering measurements.

Synchrotrons produce continuous trains of closely spaced X-ray pulses. Application of such sources to the study of atomic-scale motion requires efficient modulation of these beams on timescales ranging from nanoseconds to femtoseconds. However, ultrafast X-ray modulators are not generally available. Here we report efficient subnanosecond coherent switching of synchrotron beams by using acoustic pulses in a crystal to modulate the anomalous low-loss transmission of X-ray pulses. The acoustic excitation transfers energy between two X-ray beams in a time shorter than the synchrotron pulse width of about 100 ps. Gigahertz modulation of the diffracted X-rays is also observed. We report different geometric arrangements, such as a switch based on the collision of two counter-propagating acoustic pulses: this doubles the X-ray modulation frequency, and also provides a means of observing a localized transient strain inside an opaque material. We expect that these techniques could be scaled to produce subpicosecond pulses, through laser-generated coherent optical phonon modulation of X-ray diffraction in crystals. Such ultrafast capabilities have been demonstrated thus far only in laser-generated X-ray sources, or through the use of X-ray streak cameras.