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- ultrafast X-ray diffraction (2)
- Detector modelling and simulations II (electric fields, charge transport, multiplication and induction, pulse formation, electron emission, etc) (1)
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Ca3NbGa3Si2O14 (CNGS), a five-component crystal of lanthanum-gallium silicate group, was grown by the Czochralski method. The parameters of the elementary unit cell of the crystal were measured by powder diffraction. The independent piezoelectric strain coefficients d(11) and d(14) were determined by the triple-axis X-ray diffraction in the Bragg and Laue geometries. Excitation and propagation of surface acoustic waves (SAW) were studied by high-resolution X-ray diffraction at BESSY II synchrotron radiation source. The velocity of SAW propagation and power flow angles in the Y-, X-and yxl/+36 degrees-cuts of the CNGS crystal were determined from the analysis of the diffraction spectra. The CNGS crystal was found practically isotropic by its acoustic properties.
Phonons are often regarded as delocalized quasiparticles with certain energy and momentum. The anharmonic interaction of phonons determines macroscopic properties of the solid, such as thermal expansion or thermal conductivity, and a detailed understanding becomes increasingly important for functional nanostructures. Although phonon-phonon scattering processes depicted in simple wave-vector diagrams are the basis of theories describing these macroscopic phenomena, experiments directly accessing these coupling channels are scarce. We synthesize monochromatic acoustic phonon wave packets with only a few cycles to introduce nonlinear phononics as the acoustic counterpart to nonlinear optics. Control of the wave vector, bandwidth, and consequently spatial extent of the phonon wave packets allows us to observe nonlinear phonon interaction, in particular, second harmonic generation, in real time by wave-vector-sensitive Brillouin scattering with x-rays and optical photons.
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.
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.
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.
Brillouin scattering of visible and hard X-ray photons from optically synthesized phonon wavepackets
(2013)
We monitor how destructive interference of undesired phonon frequency components shapes a quasi-monochromatic hypersound wavepacket spectrum during its local real-time preparation by a nanometric transducer and follow the subsequent decay by nonlinear coupling. We prove each frequency component of an optical supercontinuum probe to be sensitive to one particular phonon wavevector in bulk material and cross-check this by ultrafast x-ray diffraction experiments with direct access to the lattice dynamics. Establishing reliable experimental techniques with direct access to the transient spectrum of the excitation is crucial for the interpretation in strongly nonlinear regimes, such as soliton formation.
In this work we study the response of a pnCCD by means of X-ray spectroscopy in the energy range between 6 key and 20 key and by Laue diffraction techniques. The analyses include measurements of characteristic detector parameters like energy resolution, count rate capability and effects of different gain settings. The limit of a single photon counting operation in white beam X-ray diffraction experiments is discussed with regard to the occurrence of pile-up events, for which the energy information about individual photons is lost. In case of monochromatic illumination the pnCCD can be used as a fast conventional CCD with a charge handling capacity (CHC) of about 300,000 electrons per pixel. If the CHC is exceeded, any surplus charge will spill to neighboring pixels perpendicular to the transfer direction due to electrostatic repulsion. The possibilities of increasing the number of storable electrons are investigated for different voltage settings by exposing a single pixel with X-rays generated by a microfocus X-ray source. The pixel binning mode is tested as an alternative approach that enables a pnCCD operation with significantly shorter readout times.
We synthesize sub-THz longitudinal quasimonochromatic acoustic phonons in a SrTiO3 single crystal using a SrRuO3/SrTiO3 superlattice as an optical-acoustic transducer. The generated acoustic phonon spectrum is determined using ultrafast x-ray diffraction. The analysis of the generated phonon spectrum in the time domain reveals a k-vector dependent phonon lifetime. It is observed that even at sub-THz frequencies the phonon lifetime agrees with the 1/omega(2) power law known from Akhiezer's model for hyper sound attenuation. The observed shift of the synthesized spectrum to the higher q is discussed in the framework of nonlinear effects appearing due to the high amplitude of the synthesized phonons.
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 excite an epitaxial SrRuO3 thin film transducer by a pulse train of ultrashort laser pulses, launching coherent sound waves into the underlying SrTiO3 substrate. Synchrotron-based x-ray diffraction (XRD) data exhibiting separated sidebands to the substrate peak evidence the excitation of a quasi-monochromatic phonon wavepacket with sub-THz central frequency. The frequency and bandwidth of this sound pulse can be controlled by the optical pulse train. We compare the experimental data to combined lattice dynamics and dynamical XRD simulations to verify the coherent phonon dynamics. In addition, we observe a lifetime of 130 ps of such sub-THz phonons in accordance with the theory.