TY - JOUR A1 - Shayduk, Roman A1 - Herzog, Marc A1 - Bojahr, Andre A1 - Schick, Daniel A1 - Gaal, Peter A1 - Leitenberger, Wolfram A1 - Navirian, Hengameh A1 - Sander, Mathias A1 - Goldshteyn, Jevgenij A1 - Vrejoiu, Ionela A1 - Bargheer, Matias T1 - Direct time-domain sampling of subterahertz coherent acoustic phonon spectra in SrTiO3 using ultrafast x-ray diffraction JF - Physical review : B, Condensed matter and materials physics N2 - 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. Y1 - 2013 U6 - https://doi.org/10.1103/PhysRevB.87.184301 SN - 1098-0121 VL - 87 IS - 18 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Schick, Daniel A1 - Shayduk, Roman A1 - Bojahr, Andre A1 - Herzog, Marc A1 - von Korff Schmising, Clemens A1 - Gaal, Peter A1 - Bargheer, Matias T1 - Ultrafast reciprocal-space mapping with a convergent beam JF - JOURNAL OF APPLIED CRYSTALLOGRAPHY N2 - 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. Y1 - 2013 U6 - https://doi.org/10.1107/S0021889813020013 SN - 0021-8898 VL - 46 IS - 10 SP - 1372 EP - 1377 PB - WILEY-BLACKWELL CY - HOBOKEN ER - TY - JOUR A1 - Schick, Daniel A1 - Herzog, Marc A1 - Bojahr, Andre A1 - Leitenberger, Wolfram A1 - Hertwig, Andreas A1 - Shayduk, Roman A1 - Bargheer, Matias T1 - Ultrafast lattice response of photoexcited thin films studied by X-ray diffraction JF - Structural dynamics N2 - 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. Y1 - 2014 U6 - https://doi.org/10.1063/1.4901228 SN - 2329-7778 VL - 1 IS - 6 PB - American Institute of Physics CY - Melville ER - TY - JOUR A1 - Schick, Daniel A1 - Bojahr, Andre A1 - Herzog, Marc A1 - von Korff Schmising, Clemens A1 - Shayduk, Roman A1 - Leitenberger, Wolfram A1 - Gaa, P. A1 - Bargheer, Matias T1 - Normalization schemes for ultrafast x-ray diffraction using a table-top laser-driven plasma source JF - Review of scientific instruments : a monthly journal devoted to scientific instruments, apparatus, and techniques N2 - We present an experimental setup of a laser-driven x-ray plasma source for femtosecond x-ray diffraction. Different normalization schemes accounting for x-ray source intensity fluctuations are discussed in detail. We apply these schemes to measure the temporal evolution of Bragg peak intensities of perovskite superlattices after ultrafast laser excitation. Y1 - 2012 U6 - https://doi.org/10.1063/1.3681254 SN - 0034-6748 VL - 83 IS - 2 PB - American Institute of Physics CY - Melville ER - TY - JOUR A1 - Schick, Daniel A1 - Bojahr, Andre A1 - Herzog, Marc A1 - Shayduk, Roman A1 - von Korff Schmising, Clemens A1 - Bargheer, Matias T1 - Udkm1Dsim-A simulation toolkit for 1D ultrafast dynamics in condensed matter JF - Computer physics communications : an international journal devoted to computational physics and computer programs in physics N2 - The UDKM1DSIM toolbox is a collection of MATLAB (MathWorks Inc.) classes and routines to simulate the structural dynamics and the according X-ray diffraction response in one-dimensional crystalline sample structures upon an arbitrary time-dependent external stimulus, e.g. an ultrashort laser pulse. The toolbox provides the capabilities to define arbitrary layered structures on the atomic level including a rich database of corresponding element-specific physical properties. The excitation of ultrafast dynamics is represented by an N-temperature model which is commonly applied for ultrafast optical excitations. Structural dynamics due to thermal stress are calculated by a linear-chain model of masses and springs. The resulting X-ray diffraction response is computed by dynamical X-ray theory. The UDKM1DSIM toolbox is highly modular and allows for introducing user-defined results at any step in the simulation procedure. Program summary Program title: udkm1Dsim Catalogue identifier: AERH_v1_0 Program summary URL: http://cpc.cs.qub.ac.uk/summaries/AERH_v1_0.html Licensing provisions: BSD No. of lines in distributed program, including test data, etc.: 130221 No. of bytes in distributed program, including test data, etc.: 2746036 Distribution format: tar.gz Programming language: Matlab (MathWorks Inc.). Computer: PC/Workstation. Operating system: Running Matlab installation required (tested on MS Win XP -7, Ubuntu Linux 11.04-13.04). Has the code been vectorized or parallelized?: Parallelization for dynamical XRD computations. Number of processors used: 1-12 for Matlab Parallel Computing Toolbox; 1 - infinity for Matlab Distributed Computing Toolbox External routines: Optional: Matlab Parallel Computing Toolbox, Matlab Distributed Computing Toolbox Required (included in the package): mtimesx Fast Matrix Multiply for Matlab by James Tursa, xml io tools by Jaroslaw Tuszynski, textprogressbar by Paul Proteus Nature of problem: Simulate the lattice dynamics of 1D crystalline sample structures due to an ultrafast excitation including thermal transport and compute the corresponding transient X-ray diffraction pattern. Solution method: Restrictions: The program is restricted to 1D sample structures and is further limited to longitudinal acoustic phonon modes and symmetrical X-ray diffraction geometries. Unusual features: The program is highly modular and allows the inclusion of user-defined inputs at any time of the simulation procedure. Running time: The running time is highly dependent on the number of unit cells in the sample structure and other simulation parameters such as time span or angular grid for X-ray diffraction computations. However, the example files are computed in approx. 1-5 min each on a 8 Core Processor with 16 GB RAM available. KW - Ultrafast dynamics KW - Heat diffusion KW - N-temperature model KW - Coherent phonons KW - Incoherent phonons KW - Thermoelasticity KW - Dynamical X-ray theory Y1 - 2014 U6 - https://doi.org/10.1016/j.cpc.2013.10.009 SN - 0010-4655 SN - 1879-2944 VL - 185 IS - 2 SP - 651 EP - 660 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Schick, Daniel A1 - Bojahr, Andre A1 - Herzog, Marc A1 - Gaal, P. A1 - Vrejoiu, I. A1 - Bargheer, Matias T1 - Following Strain-Induced Mosaicity Changes of Ferroelectric Thin Films by Ultrafast Reciprocal Space Mapping JF - Physical review letters N2 - 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. Y1 - 2013 U6 - https://doi.org/10.1103/PhysRevLett.110.095502 SN - 0031-9007 SN - 1079-7114 VL - 110 IS - 9 PB - American Physical Society CY - College Park ER - TY - GEN A1 - Pavlenko, Elena S. A1 - Sander, Mathias A1 - Mitzscherling, Steffen A1 - Pudell, Jan-Etienne A1 - Zamponi, Flavio A1 - Rössle, Matthias A1 - Bojahr, Andre A1 - Bargheer, Matias T1 - Azobenzene – functionalized polyelectrolyte nanolayers as ultrafast optoacoustic transducers N2 - We introduce azobenzene-functionalized polyelectrolyte multilayers as efficient, inexpensive optoacoustic transducers for hyper-sound strain waves in the GHz range. By picosecond transient reflectivity measurements we study the creation of nanoscale strain waves, their reflection from interfaces, damping by scattering from nanoparticles and propagation in soft and hard adjacent materials like polymer layers, quartz and mica. The amplitude of the generated strain ε ∼ 5 × 10−4 is calibrated by ultrafast X-ray diffraction. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 297 Y1 - 2016 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-101996 VL - 8 SP - 13297 EP - 13302 ER - TY - JOUR A1 - Pavlenko, Elena S. A1 - Sander, Mathias A1 - Mitzscherling, S. A1 - Pudell, Jan-Etienne A1 - Zamponi, Flavio A1 - Roessle, M. A1 - Bojahr, Andre A1 - Bargheer, Matias T1 - Azobenzene - functionalized polyelectrolyte nanolayers as ultrafast optoacoustic transducers JF - Nanoscale N2 - We introduce azobenzene-functionalized polyelectrolyte multilayers as efficient, inexpensive optoacoustic transducers for hyper-sound strain waves in the GHz range. By picosecond transient reflectivity measurements we study the creation of nanoscale strain waves, their reflection from interfaces, damping by scattering from nanoparticles and propagation in soft and hard adjacent materials like polymer layers, quartz and mica. The amplitude of the generated strain epsilon similar to 5 x 10(-4) is calibrated by ultrafast X-ray diffraction. Y1 - 2016 U6 - https://doi.org/10.1039/c6nr01448h SN - 2040-3364 SN - 2040-3372 VL - 8 SP - 13297 EP - 13302 PB - Royal Society of Chemistry CY - Cambridge ER - TY - JOUR A1 - Maerten, Lena A1 - Bojahr, Andre A1 - Gohlke, Mathias A1 - Rössle, Matthias A1 - Bargheer, Matias T1 - Coupling of GHz Phonons to Ferroelastic Domain Walls in SrTiO3 JF - Physical review letters N2 - We study the linear and nonlinear acoustic response of SrTiO3 across its ferroelastic transition at T-a = 105 K by time domain Brillouin scattering. Above T-a we observe that for a strain amplitude of similar to 0.18% the sound velocity for compressive strain exceeds the tensile strain velocity by 3%. Below T-a we find a giant slowing down of the sound velocity by 12% and attribute this to the coupling of GHz phonons to ferroelastic twin domain walls. We propose a new mechanism for this coupling on the ultrafast time scale, providing an important new test ground for theories used to simulate atomic motion in domain forming crystals. Y1 - 2015 U6 - https://doi.org/10.1103/PhysRevLett.114.047401 SN - 0031-9007 SN - 1079-7114 VL - 114 IS - 4 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Herzog, Marc A1 - Bojahr, Andre A1 - Goldshteyn, J. A1 - Leitenberger, Wolfram A1 - Vrejoiu, I. A1 - Khakhulin, D. A1 - Wulff, M. A1 - Shayduk, Roman A1 - Gaal, P. A1 - Bargheer, Matias T1 - Detecting optically synthesized quasi-monochromatic sub-terahertz phonon wavepackets by ultrafast x-ray diffraction JF - Applied physics letters N2 - 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. KW - acoustic waves KW - epitaxial layers KW - phonon dispersion relations KW - terahertz waves KW - thin film devices KW - X-ray diffraction Y1 - 2012 U6 - https://doi.org/10.1063/1.3688492 SN - 0003-6951 VL - 100 IS - 9 PB - American Institute of Physics CY - Melville ER - TY - JOUR A1 - Goldshteyn, Jevgeni A1 - Bojahr, Andre A1 - Gaal, Peter A1 - Schick, Daniel A1 - Bargheer, Matias T1 - Selective preparation and detection of phonon polariton wavepackets by stimulated Raman scattering JF - Physica status solidi : Physica status solidi N2 - Wavevector-selective impulsive excitation of phonon-polaritons by a spectrally broad femtosecond transient grating produces wavepackets propagating in opposite directions. The photons in spectrally narrow probe pulses are scattered from these elementary excitations in lithium niobate (LiNbO3). Both elastically and inelastically scattered photons are simultaneously detected in a spectrometer. The Stokes- and anti-Stokes shifted probe pulses uniquely determine the propagation direction of the detected polariton wavepacket components and correspond to creation or annihilation of phonon-polaritons. Our experiments with spectrally broad pump and spectrally narrow probe pulses allows dissecting the four-wave-mixing process into two sequential stimulated Raman scattering events. Y1 - 2014 U6 - https://doi.org/10.1002/pssb.201350114 SN - 0370-1972 SN - 1521-3951 VL - 251 IS - 4 SP - 821 EP - 828 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Gaal, Peter A1 - Schick, Daniel A1 - Herzog, Marc A1 - Bojahr, Andre A1 - Shayduk, Roman A1 - Goldshteyn, Jevgeni A1 - Leitenberger, Wolfram A1 - Vrejoiu, Ionela A1 - Khakhulin, Dmitry A1 - Wulff, Michael A1 - Bargheer, Matias T1 - Ultrafast switching of hard X-rays JF - Journal of synchrotron radiation N2 - 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. KW - ultrafast X-ray diffraction KW - thin film KW - coherent phonons KW - X-ray switching KW - pulse shortening KW - optical pump X-ray probe KW - time-resolved Y1 - 2014 U6 - https://doi.org/10.1107/S1600577513031949 SN - 0909-0495 SN - 1600-5775 VL - 21 SP - 380 EP - 385 PB - Wiley-Blackwell CY - Hoboken ER - TY - JOUR A1 - Gaal, P. A1 - Schick, Daniel A1 - Herzog, Marc A1 - Bojahr, Andre A1 - Shayduk, Roman A1 - Goldshteyn, J. A1 - Navirian, Hengameh A. A1 - Leitenberger, Wolfram A1 - Vrejoiu, Ionela A1 - Khakhulin, D. A1 - Wulff, M. A1 - Bargheer, Matias T1 - Time-domain sampling of x-ray pulses using an ultrafast sample response JF - Applied physics letters N2 - 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. Y1 - 2012 U6 - https://doi.org/10.1063/1.4769828 SN - 0003-6951 VL - 101 IS - 24 PB - American Institute of Physics CY - Melville ER - TY - JOUR A1 - Bojahr, Andre A1 - Schick, Daniel A1 - Märten, Lena A1 - Herzog, Marc A1 - Vrejoiu, Ionela A1 - von Korff Schmising, Clemens A1 - Milne, Chris A1 - Johnson, Steven Lee A1 - Bargheer, Matias T1 - Comparing the oscillation phase in optical pump-probe spectra to ultrafast x-ray diffraction in the metal-dielectric SrRuO3/SrTiO3 superlattice JF - Physical review : B, Condensed matter and materials physics N2 - We measured the ultrafast optical response of metal-dielectric superlattices by broadband all-optical pump-probe spectroscopy. The observed phase of the superlattice mode depends on the probe wavelength, making assignments of the excitation mechanism difficult. Ultrafast x-ray diffraction data reveal the true oscillation phase of the lattice which changes as a function of the excitation fluence. This result is confirmed by the fluence dependence of optical transients. We set up a linear chain model of the lattice dynamics and successfully simulated the broadband optical reflection by unit-cell resolved calculation of the strain-dependent dielectric functions of the constituting materials. Y1 - 2012 U6 - https://doi.org/10.1103/PhysRevB.85.224302 SN - 1098-0121 VL - 85 IS - 22 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Bojahr, Andre A1 - Herzog, Marc A1 - Schick, Daniel A1 - Vrejoiu, Ionela A1 - Bargheer, Matias T1 - Calibrated real-time detection of nonlinearly propagating strain waves JF - Physical review : B, Condensed matter and materials physics N2 - Epitaxially grown metallic oxide transducers support the generation of ultrashort strain pulses in SrTiO3 (STO) with high amplitudes up to 0.5%. The strain amplitudes are calibrated by real-time measurements of the lattice deformation using ultrafast x-ray diffraction. We determine the speed at which the strain fronts propagate by broadband picosecond ultrasonics and conclude that, above a strain level of approx. 0.2%, the compressive and tensile strain components travel at considerably different sound velocities, indicating nonlinear wave behavior. Simulations based on an anharmonic linear-chain model are in excellent accord with the experimental findings and show how the spectrum of coherent phonon modes changes with time. Y1 - 2012 U6 - https://doi.org/10.1103/PhysRevB.86.144306 SN - 1098-0121 VL - 86 IS - 14 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Bojahr, Andre A1 - Herzog, Marc A1 - Mitzscherling, Steffen A1 - Maerten, Lena A1 - Schick, Daniel A1 - Goldshteyn, J. A1 - Leitenberger, Wolfram A1 - Shayduk, R. A1 - Gaal, P. A1 - Bargheer, Matias T1 - Brillouin scattering of visible and hard X-ray photons from optically synthesized phonon wavepackets JF - Optics express : the international electronic journal of optics N2 - 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. Y1 - 2013 U6 - https://doi.org/10.1364/OE.21.021188 SN - 1094-4087 VL - 21 IS - 18 SP - 21188 EP - 21197 PB - Optical Society of America CY - Washington ER - TY - JOUR A1 - Bojahr, Andre A1 - Gohlke, Matthias A1 - Leitenberger, Wolfram A1 - Pudell, Jan-Etienne A1 - Reinhardt, Matthias A1 - von Reppert, Alexander A1 - Rössle, Matthias A1 - Sander, Mathias A1 - Gaal, Peter A1 - Bargheer, Matias T1 - Second Harmonic Generation of Nanoscale Phonon Wave Packets JF - Physical review letters N2 - 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. Y1 - 2015 U6 - https://doi.org/10.1103/PhysRevLett.115.195502 SN - 0031-9007 SN - 1079-7114 VL - 115 IS - 19 PB - American Physical Society CY - College Park ER - TY - THES A1 - Bojahr, Andre T1 - Hypersound interaction studied by time-resolved inelastic light and x-ray scattering T1 - Wechselwirkende Hyperschallwellen untersucht mittels zeitaufgelöster inelastischer Licht- und Röntgenstreuung N2 - This publications-based thesis summarizes my contribution to the scientific field of ultrafast structural dynamics. It consists of 16 publications, about the generation, detection and coupling of coherent gigahertz longitudinal acoustic phonons, also called hypersonic waves. To generate such high frequency phonons, femtosecond near infrared laser pulses were used to heat nanostructures composed of perovskite oxides on an ultrashort timescale. As a consequence the heated regions of such a nanostructure expand and a high frequency acoustic phonon pulse is generated. To detect such coherent acoustic sound pulses I use ultrafast variants of optical Brillouin and x-ray scattering. Here an incident optical or x-ray photon is scattered by the excited sound wave in the sample. The scattered light intensity measures the occupation of the phonon modes. The central part of this work is the investigation of coherent high amplitude phonon wave packets which can behave nonlinearly, quite similar to shallow water waves which show a steepening of wave fronts or solitons well known as tsunamis. Due to the high amplitude of the acoustic wave packets in the solid, the acoustic properties can change significantly in the vicinity of the sound pulse. This may lead to a shape change of the pulse. I have observed by time-resolved Brillouin scattering, that a single cycle hypersound pulse shows a wavefront steepening. I excited hypersound pulses with strain amplitudes until 1% which I have calibrated by ultrafast x-ray diffraction (UXRD). On the basis of this first experiment we developed the idea of the nonlinear mixing of narrowband phonon wave packets which we call "nonlinear phononics" in analogy with the nonlinear optics, which summarizes a kaleidoscope of surprising optical phenomena showing up at very high electric fields. Such phenomena are for instance Second Harmonic Generation, four-wave-mixing or solitons. But in case of excited coherent phonons the wave packets have usually very broad spectra which make it nearly impossible to look at elementary scattering processes between phonons with certain momentum and energy. For that purpose I tested different techniques to excite narrowband phonon wave packets which mainly consist of phonons with a certain momentum and frequency. To this end epitaxially grown metal films on a dielectric substrate were excited with a train of laser pulses. These excitation pulses drive the metal film to oscillate with the frequency given by their inverse temporal displacement and send a hypersonic wave of this frequency into the substrate. The monochromaticity of these wave packets was proven by ultrafast optical Brillouin and x-ray scattering. Using the excitation of such narrowband phonon wave packets I was able to observe the Second Harmonic Generation (SHG) of coherent phonons as a first example of nonlinear wave mixing of nanometric phonon wave packets. N2 - Diese publikationsbasierte Dissertation fasst meinen Beitrag zum Forschungsgebiet der ultraschnellen Strukturdynamik zusammen. Diese Arbeit besteht aus 16 Publikationen aus den Bereichen der Erzeugung, Detektion und Kopplung von kohärenten Gigahertz longitudinal-akustischen Phononen, auch Hyperschallwellen genannt. Um solch hochfrequente Phononen zu erzeugen, werden Femtosekunden nahinfrarot Laserpulse benutzt, um Nanostrukturen auf einer ultraschnellen Zeitskala zu erhitzen. Die aufgeheizten Regionen der Nanostruktur dehnen sich aufgrund der hohen Temperatur aus und ein hochfrequenter Schallpuls wird generiert. Um solche akustischen Pulse zu detektieren benutze ich ultraschnelle Varianten der Brillouin- und Röntgenstreuung. Dabei wird ein einfallendes optisches oder Röntgenphoton an der erzeugten Schallwelle gestreut. Die gemessene Streuintensität ist hierbei ein Maß für die Besetzung einzelner Phononenzustände. Der zentrale Teil dieser Arbeit ist die Untersuchung von kohärenten Phonon-Wellenpaketen mit sehr hoher Amplitude. Diese Wellenpakete können sich nichtlinear verhalten, sehr ähnlich zu Flachwasserwellen bei denen nichtlineare Effekte in Form eines Aufsteilens der Wellenfronten oder der Existenz von Solitonen, bekannt als Tsunamis, äußern. Durch die hohe Amplitude der akustischen Wellenpakete können sich die akustischen Eigenschaften des Festkörpers in der Umgebung des Schallpulses signifikant ändern, welches sich dann in einer Formänderung des Schallpulses widerspiegelt. Ich konnte mittels zeitaufgelöster Brillouinstreuung das Aufsteilen der Wellenfronten eines Hyperschallpulses bestehend aus einem einzigen Oszillationszyklus beobachten. Hierbei wurden Hyperschallwellen mit einer Dehnungsamplitude von bis zu 1% angeregt, wobei ich diesen Wert mittels ultraschneller Röntgenbeugung kalibrieren konnte. Mit diesem ersten Experiment als Basis entwickelten wir die Idee der nichtlinearen Wellenmischung von schmalbandigen Phonon-Wellenpaketen unter dem Titel "nichtlineare Phononik" in Analogie zur nichtlinearen Optik, welche sich aus einer Reihe von verblüffenden optischen Phänomenen bei sehr hohen elektrischen Feldstärken zusammensetzt. Solche Phänomene sind z. B. die optische Frequenzverdopplung, das Vier-Wellen-Mischen oder Solitone. Nur sind im Falle von kohärenten Phononen die erzeugten Spektren sehr breitbandig, was die Untersuchung von spezifischen Phononen mit festem Impuls und definierter Frequenz fast unmöglich macht. Aus diesem Grund testete ich verschiedene Methoden um schmalbandige Phonon-Wellenpakete anzuregen, welche im Wesentlichen aus Phononen bestimmten Impulses und definierter Frequenz bestehen. Dafür wurden schließ lich epitaktisch auf ein dielektrisches Substrat aufgewachsene Metallfilme mit einen Laserpulszug angeregt. Hier sorgen die Lichtpulse für eine periodische Oszillation des Metalfilms, wobei die Anregefrequenz durch den inversen zeitlichen Abstand der Lichtpulse gegeben ist. Diese periodische Oszillation sendet dann ein Hyperschallwellenpaket eben dieser Frequenz ins Substrat. Die Monochromie dieser Wellenpakete konnte dabei mittels ultraschneller Brillouin- und Röntgenstreuung bestätigt werden. Durch die Benutzung dieser schmalbandigen Phonon-Wellenpakete war es mir möglich, die Frequenzverdopplung (SHG) von kohärenten Phononen zu beobachten, was ein erstes Beispiel für die nichtlineare Wellenmischung von nanometrischen Phonon-Wellenpaketen ist. KW - hypersound KW - nonlinear acoustics KW - ultrafast KW - Brillouin scattering KW - x-ray diffraction KW - self-steepening KW - second-harmonic generation KW - Phononen KW - Wechselwirkung KW - Anharmonizität KW - nichtlineare Wellenmischung KW - zweite Harmonische KW - Phononenstreuung KW - nichlineare Phononik Y1 - 2016 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-93860 ER -