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Institute
We implemented an experimental scheme for ultrafast x-ray diffraction at storage rings based on a laser-driven Bragg-switch that shortens the x-ray pulses emitted from an undulator. The increased time-resolution is demonstrated by observing changes of intensity, position and width of the diffraction peaks of a La(0.7)Sr(0.3)MnO(3)/SrTiO(3) superlattice sample after optical excitation, i.e., by quantitatively measuring the propagation of an expansion wave through the sample. These experimental transients with timescales of 35 to 60 ps evidence a reduction of the x-ray pulse duration by a factor of two.
Simultaneous dynamic characterization of charge and structural motion during ferroelectric switching
(2017)
Monitoring structural changes in ferroelectric thin films during electric field induced polarization switching is important for a full microscopic understanding of the coupled motion of charges, atoms, and domainwalls in ferroelectric nanostructures. We combine standard ferroelectric test sequences of switching and nonswitching electrical pulses with time-resolved x-ray diffraction to investigate the structural response of a nanoscale Pb(Zr0.2Ti0.8)O-3 ferroelectric oxide capacitor upon charging, discharging, and polarization reversal. We observe that a nonlinear piezoelectric response of the ferroelectric layer develops on a much longer time scale than the RC time constant of the device. The complex atomic motion during the ferroelectric polarization reversal starts with a contraction of the lattice, whereas the expansive piezoelectric response sets in after considerable charge flow due to the applied voltage pulses on the electrodes of the capacitor. Our simultaneous measurements on a working device elucidate and visualize the complex interplay of charge flow and structural motion and challenges theoretical modeling.
Synchrotron based combined in situ x-ray diffractometry and reflectometry is used to investigate the role of vacancies for the relaxation of residual stress in thin metallic Pt films. From the experimentally determined relative changes of the lattice parameter a and of the film thickness L the modification of vacancy concentration and residual strain was derived as a function of annealing time at 130 degrees C. The results indicate that relaxation of strain resulting from compressive stress is accompanied by the creation of vacancies at the free film surface. This proves experimentally the postulated dominant role of vacancies for stress relaxation in thin metal films close to room temperature.
A new approach to achieve sub-pixel spatial resolution in a pnCCD detector with 75 x 75 mu m(2) pixel size is proposed for X-ray applications in single photon counting mode. The approach considers the energy dependence of the charge cloud created by a single photon and its split probabilities between neighboring pixels of the detector based on a rectangular model for the charge cloud density. For cases where the charge of this cloud becomes distributed over three or four pixels the center position of photon impact can be reconstructed with a precision better than 2 mu m. The predicted charge cloud sizes are tested at selected X-ray fluorescence lines emitting energies between 6.4 keV and 17.4 keV and forming charge clouds with size (rms) varying between 8 mu m and 10 mu m respectively. The 2 mu m enhanced spatial resolution of the pnCCD is verified by means of an x-ray transmission experiment throughout an optical grating.
We present a setup for ultrafast x-ray diffraction (UXRD) based at the storage ring BESSY II, in particular, a pump laser that excites the sample using 250 fs laser-pulses at repetition rates ranging from 208 kHz to 1.25 MHz. We discuss issues connected to the high heat-load and spatio-temporal alignment strategies in the context of a UXRD experiment at high repetition rates. The spatial overlap between laser pump and x-ray probe pulse is obtained with 10 mu m precision and transient lattice changes can be recorded with an accuracy of delta a/a(0) = 10(-6). We also compare time-resolved x-ray diffraction signals from a laser excited LSMO/STO superlattice with phonon dynamics simulations. From the analysis we determine the x-ray pulse duration to 120 ps in standard operation mode and below 10 ps in low-alpha mode.
We present ultrafast x-ray diffraction (UXRD) experiments on different photoexcited oxide superlattices. All data are successfully simulated by dynamical x-ray diffraction calculations based on a microscopic model, that accounts for the linear response of phonons to the excitation laser pulse. Some Bragg reflections display a highly nonlinear strain dependence. The origin of linear and two distinct nonlinear response phenomena is discussed in a conceptually simpler model using the interference of envelope functions that describe the diffraction efficiency of the average constituent nanolayers. The combination of both models facilitates rapid and accurate simulations of UXRD experiments.
Temperature dependent energy-dispersive X-ray diffraction and magnetic study of Fe/Al interface
(2007)
In situ temperature dependent energy-dispersive structural and magnetic study of electron beam evaporated Fe/Al multilayer sample (MLS) has been investigated. The structural studies show the formation of an intermixed FeAl transition layer of a few nanometers thick at the interface during deposition, which on annealing at 300 degrees C transforms to B2FeAl intermetallic phase. Magnetization decreases with increase in temperature and drops to minimum above 300 degrees C due to increase in anti-ferromagnetic interlayer coupling and formation of nonmagnetic FeAl phase at the interface. The Curie temperature (T-c) is found to be 288 degrees C and is much less than that of bulk bcc Fe.
We investigate the thermoelastic response of a nanolayered sample composed of a metallic SrRuO3 electrode sandwiched between a ferroelectric Pb(Zr0.2Ti0.8)O-3 film with negative thermal expansion and a SrTiO3 substrate. SrRuO3 is rapidly heated by fs-laser pulses with 208 kHz repetition rate. Diffraction of X-ray pulses derived from a synchrotron measures the transient out-of-plane lattice constant c of all three materials simultaneously from 120 ps to 5 mu s with a relative accuracy up to Delta c/c = 10(-6). The in-plane propagation of sound is essential for understanding the delayed out-of-plane compression of Pb(Zr0.2Ti0.8)O-3.
We employ the ultrafast response of a 15.4 nm thin SrRuO3 layer grown epitaxially on a SrTiO3 substrate to perform time-domain sampling of an x-ray pulse emitted from a synchrotron storage ring. Excitation of the sample with an ultrashort laser pulse triggers coherent expansion and compression waves in the thin layer, which turn the diffraction efficiency on and off at a fixed Bragg angle during 5 ps. This is significantly shorter than the duration of the synchrotron x-ray pulse of 100 ps. Cross-correlation measurements of the ultrafast sample response and the synchrotron x-ray pulse allow to reconstruct the x-ray pulse shape.
The electric field-dependence of structural dynamics in a tetragonal ferroelectric lead zirconate titanate thin film is investigated under subcoercive and above-coercive fields using time-resolved X-ray diffraction. The domain nucleation and growth are monitored in real time during the application of an external field to the prepoled thin film capacitor. We propose the observed broadening of the in-plane peak width of the symmetric 002 Bragg reflection as an indicator of the domain disorder and discuss the processes that change the measured peak intensity. Subcoercive field switching results in remnant disordered domain configurations. Published under license by AIP Publishing.
We employ ultrafast X-ray diffraction to compare the lattice dynamics of laser-excited continuous and granular FePt films on MgO (100) substrates. Contrary to recent results on free-standing granular films, we observe in both cases a pronounced and long-lasting out-of-plane expansion. We attribute this discrepancy to the in-plane expansion, which is suppressed by symmetry in continuous films. Granular films on substrates are less constrained and already show a reduced out-of-plane contraction. Via the Poisson effect, out-of-plane contractions drive in-plane expansion and vice versa. Consistently, the granular film exhibits a short-lived out-of-plane contraction driven by ultrafast demagnetization which is followed by a reduced and delayed expansion. From the acoustic reflections of the observed strain waves at the film-substrate interface, we extract a 13% reduction of the elastic constants in thin 10 nm FePt films compared to bulk-like samples. (C) 2018 Author(s).
Using ultrafast X-ray diffraction, we study the coherent picosecond lattice dynamics of photoexcited thin films in the two limiting cases, where the photoinduced stress profile decays on a length scale larger and smaller than the film thickness. We solve a unifying analytical model of the strain propagation for acoustic impedance-matched opaque films on a semi-infinite transparent substrate, showing that the lattice dynamics essentially depend on two parameters: One for the spatial profile and one for the amplitude of the strain. We illustrate the results by comparison with high-quality ultrafast X-ray diffraction data of SrRuO3 films on SrTiO3 substrates. (C) 2014 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution 3.0 Unported License.
We experimentally demonstrate efficient switching of the hard x-ray Bragg reflectivity of a SrRuO3 /SrTiO3 superlattice by optical excitation of large-amplitude coherent acoustic superlattice phonons. The rocking curve changes drastically on a 1 ps timescale. The (0 0 116) reflection is almost extinguished (Delta R/R-0=-0.91), while the (0 0 118) reflection increases by more than an order of magnitude (Delta R/R-0=24.1). The change of the x-ray structure factor depends nonlinearly on the phonon amplitude, allowing manipulation of the x-ray response on a timescale considerably shorter than the phonon period. Numerical simulations for a superlattice with slightly changed geometry and realistic parameters predict a switching-contrast ratio Delta R/R-0 of 700 with high reflectivity.
A new concept for shortening hard X-ray pulses emitted from a third-generation synchrotron source down to few picoseconds is presented. The device, called the PicoSwitch, exploits the dynamics of coherent acoustic phonons in a photo-excited thin film. A characterization of the structure demonstrates switching times of <= 5 ps and a peak reflectivity of similar to 10(-3). The device is tested in a real synchrotron-based pump-probe experiment and reveals features of coherent phonon propagation in a second thin film sample, thus demonstrating the potential to significantly improve the temporal resolution at existing synchrotron facilities.
We investigate the heat transport through a rare earth multilayer system composed of yttrium (Y), dysprosium (Dy), and niobium (Nb) by ultrafast x-ray diffraction. This is an example of a complex heat flow problem on the nanoscale, where several different quasiparticles carry the heat and conserve a nonequilibrium for more than 10 ns. The Bragg peak positions of each layer represent layer-specific thermometers that measure the energy flow through the sample after excitation of the Y top layer with fs-laser pulses. In an experiment-based analytic solution to the nonequilibrium heat transport problem, we derive the individual contributions of the spins and the coupled electron-lattice system to the heat conduction. The full characterization of the spatiotemporal energy flow at different starting temperatures reveals that the spin excitations of antiferromagnetic Dy speed up the heat transport into the Dy layer at low temperatures, whereas the heat transport through this layer and further into the Y and Nb layers underneath is slowed down. The experimental findings are compared to the solution of the heat equation using macroscopic temperature-dependent material parameters without separation of spin and phonon contributions to the heat. We explain why the simulated energy density matches our experiment-based derivation of the heat transport, although the simulated thermoelastic strain in this simulation is not even in qualitative agreement.