@phdthesis{Schick2013, author = {Schick, Daniel}, title = {Ultrafast lattice dynamics in photoexcited nanostructures : femtosecond X-ray diffraction with optimized evaluation schemes}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus-68827}, school = {Universit{\"a}t Potsdam}, year = {2013}, abstract = {Within the course of this thesis, I have investigated the complex interplay between electron and lattice dynamics in nanostructures of perovskite oxides. Femtosecond hard X-ray pulses were utilized to probe the evolution of atomic rearrangement directly, which is driven by ultrafast optical excitation of electrons. The physics of complex materials with a large number of degrees of freedom can be interpreted once the exact fingerprint of ultrafast lattice dynamics in time-resolved X-ray diffraction experiments for a simple model system is well known. The motion of atoms in a crystal can be probed directly and in real-time by femtosecond pulses of hard X-ray radiation in a pump-probe scheme. In order to provide such ultrashort X-ray pulses, I have built up a laser-driven plasma X-ray source. The setup was extended by a stable goniometer, a two-dimensional X-ray detector and a cryogen-free cryostat. The data acquisition routines of the diffractometer for these ultrafast X-ray diffraction experiments were further improved in terms of signal-to-noise ratio and angular resolution. The implementation of a high-speed reciprocal-space mapping technique allowed for a two-dimensional structural analysis with femtosecond temporal resolution. I have studied the ultrafast lattice dynamics, namely the excitation and propagation of coherent phonons, in photoexcited thin films and superlattice structures of the metallic perovskite SrRuO3. Due to the quasi-instantaneous coupling of the lattice to the optically excited electrons in this material a spatially and temporally well-defined thermal stress profile is generated in SrRuO3. This enables understanding the effect of the resulting coherent lattice dynamics in time-resolved X-ray diffraction data in great detail, e.g. the appearance of a transient Bragg peak splitting in both thin films and superlattice structures of SrRuO3. In addition, a comprehensive simulation toolbox to calculate the ultrafast lattice dynamics and the resulting X-ray diffraction response in photoexcited one-dimensional crystalline structures was developed in this thesis work. With the powerful experimental and theoretical framework at hand, I have studied the excitation and propagation of coherent phonons in more complex material systems. In particular, I have revealed strongly localized charge carriers after above-bandgap femtosecond photoexcitation of the prototypical multiferroic BiFeO3, which are the origin of a quasi-instantaneous and spatially inhomogeneous stress that drives coherent phonons in a thin film of the multiferroic. In a structurally imperfect thin film of the ferroelectric Pb(Zr0.2Ti0.8)O3, the ultrafast reciprocal-space mapping technique was applied to follow a purely strain-induced change of mosaicity on a picosecond time scale. These results point to a strong coupling of in- and out-of-plane atomic motion exclusively mediated by structural defects.}, language = {en} } @article{SchickBojahrHerzogetal.2013, author = {Schick, Daniel and Bojahr, Andre and Herzog, Marc and Gaal, P. and Vrejoiu, I. and Bargheer, Matias}, title = {Following Strain-Induced Mosaicity Changes of Ferroelectric Thin Films by Ultrafast Reciprocal Space Mapping}, series = {Physical review letters}, volume = {110}, journal = {Physical review letters}, number = {9}, publisher = {American Physical Society}, address = {College Park}, issn = {0031-9007}, doi = {10.1103/PhysRevLett.110.095502}, pages = {5}, year = {2013}, abstract = {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.}, language = {en} } @article{BojahrHerzogMitzscherlingetal.2013, author = {Bojahr, Andre and Herzog, Marc and Mitzscherling, Steffen and Maerten, Lena and Schick, Daniel and Goldshteyn, J. and Leitenberger, Wolfram and Shayduk, R. and Gaal, P. and Bargheer, Matias}, title = {Brillouin scattering of visible and hard X-ray photons from optically synthesized phonon wavepackets}, series = {Optics express : the international electronic journal of optics}, volume = {21}, journal = {Optics express : the international electronic journal of optics}, number = {18}, publisher = {Optical Society of America}, address = {Washington}, issn = {1094-4087}, doi = {10.1364/OE.21.021188}, pages = {21188 -- 21197}, year = {2013}, abstract = {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.}, language = {en} } @article{SchickShaydukBojahretal.2013, author = {Schick, Daniel and Shayduk, Roman and Bojahr, Andre and Herzog, Marc and von Korff Schmising, Clemens and Gaal, Peter and Bargheer, Matias}, title = {Ultrafast reciprocal-space mapping with a convergent beam}, series = {JOURNAL OF APPLIED CRYSTALLOGRAPHY}, volume = {46}, journal = {JOURNAL OF APPLIED CRYSTALLOGRAPHY}, number = {10}, publisher = {WILEY-BLACKWELL}, address = {HOBOKEN}, issn = {0021-8898}, doi = {10.1107/S0021889813020013}, pages = {1372 -- 1377}, year = {2013}, abstract = {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.}, language = {en} } @article{ShaydukHerzogBojahretal.2013, author = {Shayduk, Roman and Herzog, Marc and Bojahr, Andre and Schick, Daniel and Gaal, Peter and Leitenberger, Wolfram and Navirian, Hengameh and Sander, Mathias and Goldshteyn, Jevgenij and Vrejoiu, Ionela and Bargheer, Matias}, title = {Direct time-domain sampling of subterahertz coherent acoustic phonon spectra in SrTiO3 using ultrafast x-ray diffraction}, series = {Physical review : B, Condensed matter and materials physics}, volume = {87}, journal = {Physical review : B, Condensed matter and materials physics}, number = {18}, publisher = {American Physical Society}, address = {College Park}, issn = {1098-0121}, doi = {10.1103/PhysRevB.87.184301}, pages = {7}, year = {2013}, abstract = {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.}, language = {en} } @article{HerzogSchickGaaletal.2012, author = {Herzog, Marc and Schick, Daniel and Gaal, P. and Shayduk, Roman and von Korff Schmising, Clemens and Bargheer, Matias}, title = {Analysis of ultrafast X-ray diffraction data in a linear-chain model of the lattice dynamics}, series = {Applied physics : A, Materials science \& processing}, volume = {106}, journal = {Applied physics : A, Materials science \& processing}, number = {3}, publisher = {Springer}, address = {New York}, issn = {0947-8396}, doi = {10.1007/s00339-011-6719-z}, pages = {489 -- 499}, year = {2012}, abstract = {We present ultrafast X-ray diffraction (UXRD) experiments which sensitively probe impulsively excited acoustic phonons propagating in a SrRuO3/SrTiO3 superlattice and further into the substrate. These findings are discussed together with previous UXRD results (Herzog et al. in Appl. Phys. Lett. 96, 161906, 2010; Woerner et al. in Appl. Phys. A 96, 83, 2009; v. Korff Schmising in Phys. Rev. B 78, 060404(R), 2008 and in Appl. Phys. B 88, 1, 2007) using a normal-mode analysis of a linear-chain model of masses and springs, thus identifying them as linear-response phenomena. We point out the direct correspondence of calculated observables with X-ray signals. In this framework the complex lattice motion turns out to result from an interference of vibrational eigenmodes of the coupled system of nanolayers and substrate. UXRD in principle selectively measures the lattice motion occurring with a specific wavevector, however, each Bragg reflection only measures the amplitude of a delocalized phonon mode in a spatially localized region, determined by the nanocomposition of the sample or the extinction depth of X-rays. This leads to a decay of experimental signals although the excited modes survive.}, language = {en} } @article{SchickBojahrHerzogetal.2012, author = {Schick, Daniel and Bojahr, Andre and Herzog, Marc and von Korff Schmising, Clemens and Shayduk, Roman and Leitenberger, Wolfram and Gaa, P. and Bargheer, Matias}, title = {Normalization schemes for ultrafast x-ray diffraction using a table-top laser-driven plasma source}, series = {Review of scientific instruments : a monthly journal devoted to scientific instruments, apparatus, and techniques}, volume = {83}, journal = {Review of scientific instruments : a monthly journal devoted to scientific instruments, apparatus, and techniques}, number = {2}, publisher = {American Institute of Physics}, address = {Melville}, issn = {0034-6748}, doi = {10.1063/1.3681254}, pages = {7}, year = {2012}, abstract = {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.}, language = {en} } @article{NavirianSchickGaaletal.2014, author = {Navirian, Hengameh A. and Schick, Daniel and Gaal, Peter and Leitenberger, Wolfram and Shayduk, Roman and Bargheer, Matias}, title = {Thermoelastic study of nanolayered structures using time-resolved X-ray diffraction at high repetition rate}, series = {Applied physics letters}, volume = {104}, journal = {Applied physics letters}, number = {2}, publisher = {American Institute of Physics}, address = {Melville}, issn = {0003-6951}, doi = {10.1063/1.4861873}, pages = {4}, year = {2014}, abstract = {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.}, language = {en} } @article{SchickHerzogBojahretal.2014, author = {Schick, Daniel and Herzog, Marc and Bojahr, Andre and Leitenberger, Wolfram and Hertwig, Andreas and Shayduk, Roman and Bargheer, Matias}, title = {Ultrafast lattice response of photoexcited thin films studied by X-ray diffraction}, series = {Structural dynamics}, volume = {1}, journal = {Structural dynamics}, number = {6}, publisher = {American Institute of Physics}, address = {Melville}, issn = {2329-7778}, doi = {10.1063/1.4901228}, pages = {13}, year = {2014}, abstract = {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.}, language = {en} } @article{SchickBojahrHerzogetal.2014, author = {Schick, Daniel and Bojahr, Andre and Herzog, Marc and Shayduk, Roman and von Korff Schmising, Clemens and Bargheer, Matias}, title = {Udkm1Dsim-A simulation toolkit for 1D ultrafast dynamics in condensed matter}, series = {Computer physics communications : an international journal devoted to computational physics and computer programs in physics}, volume = {185}, journal = {Computer physics communications : an international journal devoted to computational physics and computer programs in physics}, number = {2}, publisher = {Elsevier}, address = {Amsterdam}, issn = {0010-4655}, doi = {10.1016/j.cpc.2013.10.009}, pages = {651 -- 660}, year = {2014}, abstract = {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.}, language = {en} } @article{GaalSchickHerzogetal.2012, author = {Gaal, P. and Schick, Daniel and Herzog, Marc and Bojahr, Andre and Shayduk, Roman and Goldshteyn, J. and Navirian, Hengameh A. and Leitenberger, Wolfram and Vrejoiu, Ionela and Khakhulin, D. and Wulff, M. and Bargheer, Matias}, title = {Time-domain sampling of x-ray pulses using an ultrafast sample response}, series = {Applied physics letters}, volume = {101}, journal = {Applied physics letters}, number = {24}, publisher = {American Institute of Physics}, address = {Melville}, issn = {0003-6951}, doi = {10.1063/1.4769828}, pages = {4}, year = {2012}, abstract = {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.}, language = {en} } @article{MihocSchickLuetgensetal.2012, author = {Mihoc, Carmen and Schick, Daniel and L{\"u}tgens, Matthias and Lathe, Christian and Burkel, Eberhard}, title = {Formation of Al67Cu23Fe10 quasicrystals by microwave heating}, series = {International journal of materials research : Zeitschrift f{\"u}r Metallkunde}, volume = {103}, journal = {International journal of materials research : Zeitschrift f{\"u}r Metallkunde}, number = {11}, publisher = {Hanser}, address = {M{\"u}nchen}, issn = {1862-5282}, doi = {10.3139/146.110786}, pages = {1340 -- 1344}, year = {2012}, abstract = {The present work was carried out to compare the formation of single icosahedral phase during conventional heating and microwave processing. Al67Cu23Fe10 alloy powder was synthesized from high purity (99.9\%) powder elements by mechanical alloying. Differential scanning calorimetry combined with in-situ synchrotron energy dispersive X-ray diffraction was used to identify the main solid state reactions and the phase evolution of the powders. Inductive microwave processing in the magnetic field anti-node was performed to obtain the quasicrystalline phase in only a few seconds. Due to the rapid cooling of the sample it was possible to stabilize the icosahedral phase against its competing quasicrystalline approximants. Laboratory X-ray diffraction analysis was used to characterise the atomic structure of the specimen and scanning electron microscopy was used to characterise the microstructure after the microwave processing.}, language = {en} } @article{SchickHerzogWenetal.2014, author = {Schick, Daniel and Herzog, Marc and Wen, Haidan and Chen, Pice and Adamo, Carolina and Gaal, Peter and Schlom, Darrell G. and Evans, Paul G. and Li, Yuelin and Bargheer, Matias}, title = {Localized excited charge carriers generate ultrafast inhomogeneous strain in the multiferroic BiFeO3}, series = {Physical review letters}, volume = {112}, journal = {Physical review letters}, number = {9}, publisher = {American Physical Society}, address = {College Park}, issn = {0031-9007}, doi = {10.1103/PhysRevLett.112.097602}, pages = {6}, year = {2014}, abstract = {We apply ultrafast x-ray diffraction with femtosecond temporal resolution to monitor the lattice dynamics in a thin film of multiferroic BiFeO3 after above-band-gap photoexcitation. The sound-velocity limited evolution of the observed lattice strains indicates a quasi-instantaneous photoinduced stress which decays on a nanosecond time scale. This stress exhibits an inhomogeneous spatial profile evidenced by the broadening of the Bragg peak. These new data require substantial modification of existing models of photogenerated stresses in BiFeO3: the relevant excited charge carriers must remain localized to be consistent with the data.}, language = {en} } @article{GaalSchickHerzogetal.2014, author = {Gaal, Peter and Schick, Daniel and Herzog, Marc and Bojahr, Andre and Shayduk, Roman and Goldshteyn, Jevgeni and Leitenberger, Wolfram and Vrejoiu, Ionela and Khakhulin, Dmitry and Wulff, Michael and Bargheer, Matias}, title = {Ultrafast switching of hard X-rays}, series = {Journal of synchrotron radiation}, volume = {21}, journal = {Journal of synchrotron radiation}, publisher = {Wiley-Blackwell}, address = {Hoboken}, issn = {0909-0495}, doi = {10.1107/S1600577513031949}, pages = {380 -- 385}, year = {2014}, abstract = {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.}, language = {en} } @article{HerzogSchickLeitenbergeretal.2012, author = {Herzog, Marc and Schick, Daniel and Leitenberger, Wolfram and Shayduk, Roman and van der Veen, Renske M. and Milne, Christopher J. and Johnson, Steven Lee and Vrejoiu, Ionela and Bargheer, Matias}, title = {Tailoring interference and nonlinear manipulation of femtosecond x-rays}, series = {New journal of physics : the open-access journal for physics}, volume = {14}, journal = {New journal of physics : the open-access journal for physics}, number = {1}, publisher = {IOP Publ. Ltd.}, address = {Bristol}, issn = {1367-2630}, doi = {10.1088/1367-2630/14/1/013004}, pages = {9}, year = {2012}, abstract = {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.}, language = {en} } @article{BojahrHerzogSchicketal.2012, author = {Bojahr, Andre and Herzog, Marc and Schick, Daniel and Vrejoiu, Ionela and Bargheer, Matias}, title = {Calibrated real-time detection of nonlinearly propagating strain waves}, series = {Physical review : B, Condensed matter and materials physics}, volume = {86}, journal = {Physical review : B, Condensed matter and materials physics}, number = {14}, publisher = {American Physical Society}, address = {College Park}, issn = {1098-0121}, doi = {10.1103/PhysRevB.86.144306}, pages = {5}, year = {2012}, abstract = {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.}, language = {en} } @article{GoldshteynBojahrGaaletal.2014, author = {Goldshteyn, Jevgeni and Bojahr, Andre and Gaal, Peter and Schick, Daniel and Bargheer, Matias}, title = {Selective preparation and detection of phonon polariton wavepackets by stimulated Raman scattering}, series = {Physica status solidi : Physica status solidi}, volume = {251}, journal = {Physica status solidi : Physica status solidi}, number = {4}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {0370-1972}, doi = {10.1002/pssb.201350114}, pages = {821 -- 828}, year = {2014}, abstract = {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.}, language = {en} } @article{BojahrSchickMaertenetal.2012, author = {Bojahr, Andre and Schick, Daniel and M{\"a}rten, Lena and Herzog, Marc and Vrejoiu, Ionela and von Korff Schmising, Clemens and Milne, Chris and Johnson, Steven Lee and Bargheer, Matias}, title = {Comparing the oscillation phase in optical pump-probe spectra to ultrafast x-ray diffraction in the metal-dielectric SrRuO3/SrTiO3 superlattice}, series = {Physical review : B, Condensed matter and materials physics}, volume = {85}, journal = {Physical review : B, Condensed matter and materials physics}, number = {22}, publisher = {American Physical Society}, address = {College Park}, issn = {1098-0121}, doi = {10.1103/PhysRevB.85.224302}, pages = {6}, year = {2012}, abstract = {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.}, language = {en} } @article{SchickLeGuyaderPontiusetal.2016, author = {Schick, Daniel and Le Guyader, Loic and Pontius, Niko and Radu, Ilie and Kachel, Torsten and Mitzner, Rolf and Zeschke, Thomas and Schuessler-Langeheine, Christian and F{\"o}hlisch, Alexander and Holldack, Karsten}, title = {Analysis of the halo background in femtosecond slicing experiments}, series = {Journal of synchrotron radiation}, volume = {23}, journal = {Journal of synchrotron radiation}, publisher = {International Union of Crystallography}, address = {Chester}, issn = {1600-5775}, doi = {10.1107/S160057751600401X}, pages = {700 -- 711}, year = {2016}, abstract = {The slicing facility FemtoSpeX at BESSY II offers unique opportunities to study photo-induced dynamics on femtosecond time scales by means of X-ray magnetic circular dichroism, resonant and non-resonant X-ray diffraction, and X-ray absorption spectroscopy experiments in the soft X-ray regime. Besides femtosecond X-ray pulses, slicing sources inherently also produce a so-called `halo' background with a different time structure, polarization and pointing. Here a detailed experimental characterization of the halo radiation is presented, and a method is demonstrated for its correct and unambiguous removal from femtosecond time-resolved data using a special laser triggering scheme as well as analytical models. Examples are given for time-resolved measurements with corresponding halo correction, and errors of the relevant physical quantities caused by either neglecting or by applying a simplified model to describe this background are estimated.}, language = {en} } @article{ThielemannKuehnSchickPontiusetal.2017, author = {Thielemann-K{\"u}hn, Nele and Schick, Daniel and Pontius, Niko and Trabant, Christoph and Mitzner, Rolf and Holldack, Karsten and Zabel, Hartmut and F{\"o}hlisch, Alexander and Schuessler-Langeheine, Christian}, title = {Ultrafast and Energy-Efficient Quenching of Spin Order: Antiferromagnetism Beats Ferromagnetism}, series = {Physical review letters}, volume = {119}, journal = {Physical review letters}, publisher = {American Physical Society}, address = {College Park}, issn = {0031-9007}, doi = {10.1103/PhysRevLett.119.197202}, pages = {6}, year = {2017}, abstract = {By comparing femtosecond laser pulse induced ferro- and antiferromagnetic dynamics in one and the same material-metallic dysprosium-we show both to behave fundamentally different. Antiferromagnetic order is considerably faster and much more efficiently reduced by optical excitation than its ferromagnetic counterpart. We assign the fast and extremely efficient process in the antiferromagnet to an interatomic transfer of angular momentum within the spin system. Our findings imply that this angular momentum transfer channel is effective in other magnetic metals with nonparallel spin alignment. They also point out a possible route towards energy-efficient spin manipulation for magnetic devices.}, language = {en} } @article{SchickEckertPontiusetal.2016, author = {Schick, Daniel and Eckert, Sebastian and Pontius, Niko and Mitzner, Rolf and F{\"o}hlisch, Alexander and Holldack, Karsten and Sorgenfrei, Florian}, title = {Versatile soft X-ray-optical cross-correlator for ultrafast applications}, series = {Structural dynamics}, volume = {3}, journal = {Structural dynamics}, publisher = {American Institute of Physics}, address = {Melville}, issn = {2329-7778}, doi = {10.1063/1.4964296}, pages = {054304-1 -- 054304-8}, year = {2016}, abstract = {We present an X-ray-optical cross-correlator for the soft (> 150 eV) up to the hard X-ray regime based on a molybdenum-silicon superlattice. The cross-correlation is done by probing intensity and position changes of superlattice Bragg peaks caused by photoexcitation of coherent phonons. This approach is applicable for a wide range of X-ray photon energies as well as for a broad range of excitation wavelengths and requires no external fields or changes of temperature. Moreover, the cross-correlator can be employed on a 10 ps or 100 fs time scale featuring up to 50\% total X-ray reflectivity and transient signal changes of more than 20\%. (C) 2016 Author(s).}, language = {en} } @misc{FondellEckertJayetal.2017, author = {Fondell, Mattis and Eckert, Sebastian and Jay, Raphael Martin and Weniger, Christian and Quevedo, Wilson and Niskanen, Johannes and Kennedy, Brian and Sorgenfrei, Florian and Schick, Daniel and Giangrisostomi, Erika and Ovsyannikov, Ruslan and Adamczyk, Katrin and Huse, Nils and Wernet, Philippe and Mitzner, Rolf and F{\"o}hlisch, Alexander}, title = {Time-resolved soft X-ray absorption spectroscopy in transmission mode on liquids at MHz repetition rates}, series = {Postprints der Universit{\"a}t Potsdam Mathematisch-Naturwissenschaftliche Reihe}, journal = {Postprints der Universit{\"a}t Potsdam Mathematisch-Naturwissenschaftliche Reihe}, number = {780}, issn = {1866-8372}, doi = {10.25932/publishup-43752}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-437529}, pages = {12}, year = {2017}, abstract = {We present a setup combining a liquid flatjet sample delivery and a MHz laser system for time-resolved soft X-ray absorption measurements of liquid samples at the high brilliance undulator beamline UE52-SGM at Bessy II yielding unprecedented statistics in this spectral range. We demonstrate that the efficient detection of transient absorption changes in transmission mode enables the identification of photoexcited species in dilute samples. With iron(II)-trisbipyridine in aqueous solution as a benchmark system, we present absorption measurements at various edges in the soft X-ray regime. In combination with the wavelength tunability of the laser system, the set-up opens up opportunities to study the photochemistry of many systems at low concentrations, relevant to materials sciences, chemistry, and biology.}, language = {en} } @article{FondellEckertJayetal.2017, author = {Fondell, Mattis and Eckert, Sebastian and Jay, Raphael Martin and Weniger, Christian and Quevedo, Wilson and Niskanen, Johannes and Kennedy, Brian and Sorgenfrei, Florian and Schick, Daniel and Giangrisostomi, Erika and Ovsyannikov, Ruslan and Adamczyk, Katrin and Huse, Nils and Wernet, Philippe and Mitzner, Rolf and F{\"o}hlisch, Alexander}, title = {Time-resolved soft X-ray absorption spectroscopy in transmission mode on liquids at MHz repetition rates}, series = {Structural dynamics}, volume = {4}, journal = {Structural dynamics}, publisher = {American Institute of Physics}, address = {Melville}, issn = {2329-7778}, doi = {10.1063/1.4993755}, pages = {11}, year = {2017}, abstract = {We present a setup combining a liquid flatjet sample delivery and a MHz laser system for time-resolved soft X-ray absorption measurements of liquid samples at the high brilliance undulator beamline UE52-SGM at Bessy II yielding unprecedented statistics in this spectral range. We demonstrate that the efficient detection of transient absorption changes in transmission mode enables the identification of photoexcited species in dilute samples. With iron(II)-trisbipyridine in aqueous solution as a benchmark system, we present absorption measurements at various edges in the soft X-ray regime. In combination with the wavelength tunability of the laser system, the set-up opens up opportunities to study the photochemistry of many systems at low concentrations, relevant to materials sciences, chemistry, and biology. (C) 2017 Author(s).}, language = {en} } @misc{SchickEckertPontiusetal.2016, author = {Schick, Daniel and Eckert, Sebastian and Pontius, Niko and Mitzner, Rolf and F{\"o}hlisch, Alexander and Holldack, Karsten and Sorgenfrei, Florian}, title = {Versatile soft X-ray-optical cross-correlator for ultrafast applications}, series = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe}, journal = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe}, number = {1331}, issn = {1866-8372}, doi = {10.25932/publishup-43696}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-436962}, pages = {054304-1 -- 054304-8}, year = {2016}, abstract = {We present an X-ray-optical cross-correlator for the soft (> 150 eV) up to the hard X-ray regime based on a molybdenum-silicon superlattice. The cross-correlation is done by probing intensity and position changes of superlattice Bragg peaks caused by photoexcitation of coherent phonons. This approach is applicable for a wide range of X-ray photon energies as well as for a broad range of excitation wavelengths and requires no external fields or changes of temperature. Moreover, the cross-correlator can be employed on a 10 ps or 100 fs time scale featuring up to 50\% total X-ray reflectivity and transient signal changes of more than 20\%. (C) 2016 Author(s).}, language = {en} } @article{ShaydukHallmannRodriguezFernandezetal.2022, author = {Shayduk, Roman and Hallmann, J{\"o}rg and Rodriguez-Fernandez, Angel and Scholz, Markus and Lu, Wei and B{\"o}senberg, Ulrike and M{\"o}ller, Johannes and Zozulya, Alexey and Jiang, Man and Wegner, Ulrike and Secareanu, Radu-Costin and Palmer, Guido and Emons, Moritz and Lederer, Max and Volkov, Sergey and Lindfors-Vrejoiu, Ionela and Schick, Daniel and Herzog, Marc and Bargheer, Matias and Madsen, Anders}, title = {Femtosecond x-ray diffraction study of multi-THz coherent phonons in SrTiO3}, series = {Applied physics letters}, volume = {120}, journal = {Applied physics letters}, number = {20}, publisher = {AIP Publishing}, address = {Melville}, issn = {0003-6951}, doi = {10.1063/5.0083256}, pages = {5}, year = {2022}, abstract = {We report generation of ultra-broadband longitudinal acoustic coherent phonon wavepackets in SrTiO3 (STO) with frequency components extending throughout the first Brillouin zone. The wavepackets are efficiently generated in STO using femtosecond infrared laser excitation of an atomically flat 1.6 nm-thick epitaxial SrRuO3 film. We use femtosecond x-ray diffraction at the European X-Ray Free Electron Laser Facility to study the dispersion and damping of phonon wavepackets. The experimentally determined damping constants for multi-THz frequency phonons compare favorably to the extrapolation of a simple ultrasound damping model over several orders of magnitude.}, language = {en} }