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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.
We investigate coherent phonon propagation in a thin film of ferroelectric PbZr0.2Ti0.8O3 (PZT) by ultrafast x-ray diffraction experiments, which are analyzed as time-resolved reciprocal space mapping in order to observe the in-and out-of-plane structural dynamics, simultaneously. The mosaic structure of the PZT leads to a coupling of the excited out-of-plane expansion to in-plane lattice dynamics on a picosecond time scale, which is not observed for out-of-plane compression.
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.
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.
A diffractometer setup is presented, based on a laser-driven plasma X-ray source for reciprocal-space mapping with femtosecond temporal resolution. In order to map out the reciprocal space, an X-ray optic with a convergent beam is used with an X-ray area detector to detect symmetrically and asymmetrically diffracted X-ray photons simultaneously. The setup is particularly suited for measuring thin films or imperfect bulk samples with broad rocking curves. For quasi-perfect crystalline samples with insignificant in-plane Bragg peak broadening, the measured reciprocal-space maps can be corrected for the known resolution function of the diffractometer in order to achieve high-resolution rocking curves with improved data quality. In this case, the resolution of the diffractometer is not limited by the convergence of the incoming X-ray beam but is solely determined by its energy bandwidth.
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.
We have developed and characterized a hard x-ray accumulating streak camera that achieves subpicosecond time resolution by using single-photon counting. A high repetition rate of 2 kHz was achieved by use of a readout camera with built-in image processing capabilities. The effects of sweep jitter were removed by using a UV timing reference. The use of single-photon counting allows the camera to reach a high quantum efficiency by not limiting the divergence of the photoelectrons.
Laser-driven plasma sources of femtosecond hard X-ray pulses have found widespread application in ultrafast X- ray diffraction. The recent development of plasma sources working at kilohertz repetition rates has allowed for diffraction experiments with strongly improved sensitivity, now revealing subtle fully reversible changes of the geometry of crystal lattices. We provide a brief review of this development and present a novel plasma source with an optimized mechanical and optical design, providing a high flux of several 10(10) photons/s at the Cu-K alpha energy of 8.04 keV and a pulse duration of a parts per thousand currency sign300 fs. First experiments, including the generation of Debye-Scherrer diffraction patterns from Si powder, demonstrate the high performance of this source.
Femtosecond x-ray diffraction provides direct insight into the ultrafast reversible lattice dynamics of materials with a perovskite structure. Superlattice (SL) structures consisting of a sequence of nanometer-thick layer pairs allow for optically inducing a tailored stress profile that drives the lattice motions and for limiting the influence of strain propagation on the observed dynamics. We demonstrate this concept in a series of diffraction experiments with femtosecond time resolution, giving detailed information on the ultrafast lattice dynamics of ferroelectric and ferromagnetic superlattices. Anharmonically coupled lattice motions in a SrRuO3/PbZr0.2Ti0.8O3 (SRO/ PZT) SL lead to a switch-off of the electric polarizations on a time scale of the order of 1 ps. Ultrafast magnetostriction of photoexcited SRO layers is demonstrated in a SRO/SrTiO3 (STO) SL.
In der Nanotechnologie und der molekularen Biologie werden immer kleinere Strukturelemente, wie beispielsweise einzelne Atomlagen oder Molekülgruppen, manipuliert, um bestimmte Funktionen zu erzielen. Veränderungen in solchen Systemen laufen auf atomarer Längen- und Zeitskala ab. Für das physikalische Verständnis dieser ultraschnellen Prozesse ist ein anschauliches Bild wichtig. Dank ihrer hohen Struktur- und Zeitauflösung liefert die Femtosekunden-Röntgenbeugung Bildsequenzen atomarer Bewegung von Molekülen und Festkörpern und ermöglicht somit Rückschlüsse über die komplexe Wechselwirkung zwischen Elektronen- und Kernbewegungen. Die aktuellen und zukünftigen Möglichkeiten, Atomen bei ihren Bewegungen zuzusehen, diskutiert der Referent an aktuellen Beispielen.