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ABSTRACT: In recent years, X-ray radiography has been used to probe the internal structure of dense sprays with microsecond time resolution and a spatial resolution of 15 µm even in high-pressure environments. Recently, the 7BM beamline at the Advanced Photon Source (APS) has been commissioned to focus on the needs of X-ray spray radiography measurements. The spatial resolution and X-ray intensity at this beamline represent a significant improvement over previous time-resolved X-ray radiography measurements at the APS.
Journal of Synchrotron Radiation 07/2012; 19(Pt 4):654-7. · 2.73 Impact Factor
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ABSTRACT: Complex-oxide superlattices (SLs) with atomic-scale periodicity have dynamical properties that are distinct from thin films of uniform composition. The origins of these properties are closely related to the dynamics of polarization domains and to field-driven changes in the symmetries resulting from interfacial coupling between different components. These dynamics are apparent at timescales from a few nanoseconds to several milliseconds in experiments probing the piezoelectricity of a ferroelectric/dielectric BaTiO 3 (BTO)/CaTiO 3 (CTO) SL using time-resolved x-ray microdiffraction. At the 100 ns timescale, the piezoelectric distortion is approximately ten times smaller than in the millisecond regime. This reduced piezoelectricity at short timescales is not observed in previously studied PbTiO 3 /SrTiO 3 SLs or compositionally uniform ferroelectrics such as tetragonal compositions of Pb(Zr, Ti)O 3 . The unusual behavior of the BTO/CTO SL can be linked to the switching of a nanodomain state into a uniform polarization state or to a field-induced crystallographic symmetry transition. A comparison of the results 5 These authors have contributed equally to this work. 2 with the characteristic timescales of these two dynamical phenomena in other complex oxides with different compositions suggests that the phase transition is a more likely possibility.
New Journal of Physics 01/2012; 14:13034-12. · 4.18 Impact Factor
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ABSTRACT: Combined measurements of X-ray absorption and fluorescence have been performed in jets of pure and diluted argon gas to demonstrate the feasibility of using X-ray fluorescence to study turbulent mixing. Measurements show a strong correspondence between the absorption and fluorescence measurements for high argon concentration. For lower argon concentration, fluorescence provides a much more robust measurement than absorption. The measurements agree well with the accepted behavior of turbulent jets.
Journal of Synchrotron Radiation 09/2011; 18(Pt 5):811-5. · 2.73 Impact Factor
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ABSTRACT: The nanosecond response of a PbTiO(3)/SrTiO(3) ferroelectric/dielectric superlattice to applied electric fields is closely linked to the dynamics of striped domains of the remnant polarization. The intensity of domain satellite reflections observed with time-resolved x-ray microdiffraction decays in 5-100 ns depending on the magnitude of the electric field. The piezoelectric response of the superlattice within stripe domains is strongly suppressed due to electromechanical clamping between adjacent regions of opposite polarization. Regions of the superlattice that have been switched into a uniform polarization state by the applied electric field, however, exhibit piezoelectricity during the course of the switching process. We propose a switching model different from previous models of the switching of superlattices, based instead on a spatially heterogeneous transformation between striped and uniform polarization states.
Physical Review Letters 07/2011; 107(5):055501. · 7.37 Impact Factor
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Stephen T Kelly,
Jonathan C Trenkle,
Lucas J Koerner,
Sara C Barron,
Nöel Walker,
Philippe O Pouliquen,
Mark W Tate,
Sol M Gruner, Eric M Dufresne,
Timothy P Weihs,
Todd C Hufnagel
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ABSTRACT: A pair of techniques have been developed for performing time-resolved X-ray microdiffraction on irreversible phase transformations. In one technique capillary optics are used to focus a high-flux broad-spectrum X-ray beam to a 60 µm spot size and a fast pixel array detector is used to achieve temporal resolution of 55 µs. In the second technique the X-rays are focused with Kirkpatrick-Baez mirrors to achieve a spatial resolution better than 10 µm and a fast shutter is used to provide temporal resolution better than 20 µs while recording the diffraction pattern on a (relatively slow) X-ray CCD camera. Example data from experiments are presented where these techniques are used to study self-propagating high-temperature synthesis reactions in metal laminate foils.
Journal of Synchrotron Radiation 05/2011; 18(Pt 3):464-74. · 2.73 Impact Factor
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ABSTRACT: The origin of the functional properties of complex oxide superlattices can be resolved using time-resolved synchrotron x-ray diffraction into contributions from the component layers making up the repeating unit. The CaTiO3 layers of a CaTiO3/BaTiO3 superlattice have a piezoelectric response to an applied electric field, consistent with a large continuous polarization throughout the superlattice. The overall piezoelectric coefficient at large strains, 54 pm/V, agrees with first-principles predictions in which a tetragonal symmetry is imposed on the superlattice by the SrTiO3 substrate.
Physical Review Letters 05/2010; 104(20):207601. · 7.37 Impact Factor
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ABSTRACT: In recent years, x-ray radiography has been used to probe the internal structure of dense sprays. Quantita-tive measurements of spray mass distribution have been obtained on microsecond time scales and with spatial reso-lution of 15 µm even in high-pressure environments. These data have been difficult or impossible to obtain with conventional optical diagnostics. A limitation to these measurements is the need to perform them at a synchrotron light source. While several synchrotrons are available throughout the world, the experimental time at these facilities is competitively awarded and is often limited. Moreover, synchrotron beamlines are often not well instrumented to study sprays. This has limited the scope of previous spray radiography measurements. Recently, commissioning has begun of a new experimental station at the Advanced Photon Source largely dedicated to x-ray spray measurements. This facility provides significantly enhanced access to the x-ray beam in an environment tailored to spray measurements. The spatial resolution and x-ray intensity at this beamline also represent a significant improvement over previous x-ray radiography measurements at the APS. The capabilities of the beamline will be outlined in detail. Sample data from a diesel spray from a 110 µm single-hole nozzle will be used to demonstrate the capabilities of the new beamline for performing spray measurements. The prospects for additional measurements of sprays and spray systems will also be discussed.
04/2010;
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ABSTRACT: 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.
Journal of Synchrotron Radiation 06/2009; 16(Pt 3):358-67. · 2.73 Impact Factor
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ABSTRACT: Probing the piezoelectricity and ferroelectricity of thin film devices and nanostruc-tures quantitatively has proven to be challenging because the appropriate experimental tools have had a limited range of usefulness. We show here that the piezoelectric and ferroelectric properties of epitaxial thin films can be measured quantitatively using time-resolved synchrotron x-ray microdiffraction. Microdiffraction combines structural specificity with the appropriate spatial resolution and ability to probe structures with electrical contacts. Our measurements of piezoelectric coefficients and coercive elec-tric fields for Pb(Zr,Ti)O 3 capacitors using this approach are in excellent quantitative agreement with results obtained electrically and mechanically. The time and spatial resolution of microdiffraction probes are well-defined and decoupled from electrical and mechanical resonances of the ferroelectric capacitor.
Integrated Ferroelectrics 01/2009; 101:174-181. · 0.30 Impact Factor
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ABSTRACT: 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.
Physical Review Letters 02/2008; 100(2):027604. · 7.37 Impact Factor
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ABSTRACT: 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.
Review of Scientific Instruments 03/2007; 78(2):023105. · 1.37 Impact Factor
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ABSTRACT: 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.
Physical Review Letters 06/2006; 96(18):187601. · 7.37 Impact Factor
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ABSTRACT: As the polarization of a ferroelectric thin film reverses in response to an applied electric field, concomitant structural changes can be visualized using time-resolved x-ray mi-crodiffraction. We report the details of this visualization approach and discuss the struc-tural signature of polarization switching measured by time-resolved x-ray diffraction.
Integrated Ferroelectrics 01/2006; 85:165-173. · 0.30 Impact Factor
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ABSTRACT: 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.
Journal of Synchrotron Radiation 04/2005; 12(Pt 2):177-92. · 2.73 Impact Factor
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ABSTRACT: 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.
Physical Review Letters 03/2005; 94(5):055501. · 7.37 Impact Factor
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ABSTRACT: 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.
Nature Material 07/2004; 3(6):365-9. · 32.84 Impact Factor
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ABSTRACT: 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.
Nature Material 11/2002; 1(2):99-101. · 32.84 Impact Factor
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ABSTRACT: 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.
Physical Review E 07/2002; 65(6 Pt 1):061507. · 2.26 Impact Factor
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ABSTRACT: The initial stage of polarization switching in ferroelectric thin films depends on phenomena that occur at characteristic time scales of tens to hundreds of nanoseconds, including the nucleation polarization domains and the propagation of domain walls. These long intrinsic times allow short-duration electric fields with magnitudes far above the low-frequency coercive electric field to be applied across capacitor devices without inducing switching. Using time-resolved x-ray microdiffraction, we have found that a series of 50 ns duration electric field pulses switches the polarization of a 35-nm-thick ferroelectric PbZr, TiO 3 film only at electric fields greater than 1.5 MV/cm, a factor of three higher than the low-frequency coercive field. There is no switching in response to a large number of short pulses with amplitudes lower than 1.5 MV/cm, even when the total duration reaches several milliseconds. In comparison, a series of microsecond-duration pulses causes cumulative changes in the area of switched polarization and eventually switches the entire capacitor. The difference between long-and short-duration electric field pulses arises from effects linked to domain nucleation and charge transport in the ferroelectric film. A phase-field model shows that the shrinking of the switched domain in the interval between pulses is a less important effect. This opportunity to apply large fields for short times without inducing switching by domain-wall motion raises the possibility that future experiments could reach the intrinsic coercive field of ferroelectric layers and provides a way to study the properties of materials under high electric fields.
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