@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{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{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{EnquistNavirianNueskeetal.2010, author = {Enquist, Henrik and Navirian, Hengameh and Nueske, Ralf and von Korff Schmising, Clemens and Jurgilaitis, Andrius and Herzog, Marc and Bargheer, Matias and Sondhauss, Peter and Larsson, Joergen}, title = {Subpicosecond hard x-ray streak camera using single-photon counting}, issn = {0146-9592}, doi = {10.1364/OL.35.003219}, year = {2010}, abstract = {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.}, 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{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} } @phdthesis{Herzog2012, author = {Herzog, Marc}, title = {Structural dynamics of photoexcited nanolayered perovskites studied by ultrafast x-ray diffraction}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus-62632}, school = {Universit{\"a}t Potsdam}, year = {2012}, abstract = {This publication-based thesis represents a contribution to the active research field of ultrafast structural dynamics in laser-excited nanostructures. The investigation of such dynamics is mandatory for the understanding of the various physical processes on microscopic scales in complex materials which have great potentials for advances in many technological applications. I theoretically and experimentally examine the coherent, incoherent and anharmonic lattice dynamics of epitaxial metal-insulator heterostructures on timescales ranging from femtoseconds up to nanoseconds. To infer information on the transient dynamics in the photoexcited crystal lattices experimental techniques using ultrashort optical and x-ray pulses are employed. The experimental setups include table-top sources as well as large-scale facilities such as synchrotron sources. At the core of my work lies the development of a linear-chain model to simulate and analyze the photoexcited atomic-scale dynamics. The calculated strain fields are then used to simulate the optical and x-ray response of the considered thin films and multilayers in order to relate the experimental signatures to particular structural processes. This way one obtains insight into the rich lattice dynamics exhibiting coherent transport of vibrational energy from local excitations via delocalized phonon modes of the samples. The complex deformations in tailored multilayers are identified to give rise to highly nonlinear x-ray diffraction responses due to transient interference effects. The understanding of such effects and the ability to precisely calculate those are exploited for the design of novel ultrafast x-ray optics. In particular, I present several Phonon Bragg Switch concepts to efficiently generate ultrashort x-ray pulses for time-resolved structural investigations. By extension of the numerical models to include incoherent phonon propagation and anharmonic lattice potentials I present a new view on the fundamental research topics of nanoscale thermal transport and anharmonic phonon-phonon interactions such as nonlinear sound propagation and phonon damping. The former issue is exemplified by the time-resolved heat conduction from thin SrRuO3 films into a SrTiO3 substrate which exhibits an unexpectedly slow heat conductivity. Furthermore, I discuss various experiments which can be well reproduced by the versatile numerical models and thus evidence strong lattice anharmonicities in the perovskite oxide SrTiO3. The thesis also presents several advances of experimental techniques such as time-resolved phonon spectroscopy with optical and x-ray photons as well as concepts for the implementation of x-ray diffraction setups at standard synchrotron beamlines with largely improved time-resolution for investigations of ultrafast structural processes. This work forms the basis for ongoing research topics in complex oxide materials including electronic correlations and phase transitions related to the elastic, magnetic and polarization degrees of freedom.}, language = {en} } @article{HerzogBojahrGoldshteynetal.2012, author = {Herzog, Marc and Bojahr, Andre and Goldshteyn, J. and Leitenberger, Wolfram and Vrejoiu, I. and Khakhulin, D. and Wulff, M. and Shayduk, Roman and Gaal, P. and Bargheer, Matias}, title = {Detecting optically synthesized quasi-monochromatic sub-terahertz phonon wavepackets by ultrafast x-ray diffraction}, series = {Applied physics letters}, volume = {100}, journal = {Applied physics letters}, number = {9}, publisher = {American Institute of Physics}, address = {Melville}, issn = {0003-6951}, doi = {10.1063/1.3688492}, pages = {4}, year = {2012}, abstract = {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.}, language = {en} } @article{HerzogLeitenbergerShayduketal.2010, author = {Herzog, Marc and Leitenberger, Wolfram and Shayduk, Roman and van der Veen, Renske Marjan and Milne, Chris J. and Johnson, Steven Lee and Vrejoiu, Ionela and Alexe, Marin and Hesse, Dietrich and Bargheer, Matias}, title = {Ultrafast manipulation of hard x-rays by efficient Bragg switches}, issn = {0003-6951}, doi = {10.1063/1.3402773}, year = {2010}, abstract = {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.}, 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} }