@article{MatternReppertZeuschneretal.2023, author = {Mattern, Maximilian and Reppert, Alexander von and Zeuschner, Steffen Peer and Herzog, Marc and Pudell, Jan-Etienne and Bargheer, Matias}, title = {Concepts and use cases for picosecond ultrasonics with x-rays}, series = {Photoacoustics}, volume = {31}, journal = {Photoacoustics}, publisher = {Elsevier}, address = {Amsterdam}, issn = {2213-5979}, doi = {10.1016/j.pacs.2023.100503}, pages = {22}, year = {2023}, abstract = {This review discusses picosecond ultrasonics experiments using ultrashort hard x-ray probe pulses to extract the transient strain response of laser-excited nanoscopic structures from Bragg-peak shifts. This method provides direct, layer-specific, and quantitative information on the picosecond strain response for structures down to few-nm thickness. We model the transient strain using the elastic wave equation and express the driving stress using Gruneisen parameters stating that the laser-induced stress is proportional to energy density changes in the microscopic subsystems of the solid, i.e., electrons, phonons and spins. The laser-driven strain response can thus serve as an ultrafast proxy for local energy-density and temperature changes, but we emphasize the importance of the nanoscale morphology for an accurate interpretation due to the Poisson effect. The presented experimental use cases encompass ultrathin and opaque metal-heterostructures, continuous and granular nanolayers as well as negative thermal expansion materials, that each pose a challenge to established all-optical techniques.}, language = {en} } @article{HerzogReppertPudelletal.2022, author = {Herzog, Marc and Reppert, Alexander von and Pudell, Jan-Etienne and Henkel, Carsten and Kronseder, Matthias and Back, Christian H. and Maznev, Alexei A. and Bargheer, Matias}, title = {Phonon-dominated energy transport in purely metallic heterostructures}, series = {Advanced functional materials}, volume = {32}, journal = {Advanced functional materials}, number = {41}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1616-301X}, doi = {10.1002/adfm.202206179}, pages = {8}, year = {2022}, abstract = {Ultrafast X-ray diffraction is used to quantify the transport of energy in laser-excited nanoscale gold-nickel (Au-Ni) bilayers. Electron transport and efficient electron-phonon coupling in Ni convert the laser-deposited energy in the conduction electrons within a few picoseconds into a strong non-equilibrium between hot Ni and cold Au phonons at the bilayer interface. Modeling of the subsequent equilibration dynamics within various two-temperature models confirms that for ultrathin Au films, the thermal transport is dominated by phonons instead of conduction electrons because of the weak electron-phonon coupling in Au.}, 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} } @article{MatternReppertZeuschneretal.2022, author = {Mattern, Maximilian and Reppert, Alexander von and Zeuschner, Steffen Peer and Pudell, Jan-Etienne and K{\"u}hne, F. and Diesing, Detlef and Herzog, Marc and Bargheer, Matias}, title = {Electronic energy transport in nanoscale Au/Fe hetero-structures in the perspective of ultrafast lattice dynamics}, series = {Applied physics letters}, volume = {120}, journal = {Applied physics letters}, number = {9}, publisher = {AIP Publishing}, address = {Melville}, issn = {0003-6951}, doi = {10.1063/5.0080378}, pages = {5}, year = {2022}, abstract = {We study the ultrafast electronic transport of energy in a photoexcited nanoscale Au/Fe hetero-structure by modeling the spatiotemporal profile of energy densities that drives transient strain, which we quantify by femtosecond x-ray diffraction. This flow of energy is relevant for intrinsic demagnetization and ultrafast spin transport. We measured lattice strain for different Fe layer thicknesses ranging from few atomic layers to several nanometers and modeled the spatiotemporal flow of energy densities. The combination of a high electron-phonon coupling coefficient and a large Sommerfeld constant in Fe is found to yield electronic transfer of nearly all energy from Au to Fe within the first hundreds of femtoseconds.}, language = {en} } @article{MorHerzogNoacketal.2018, author = {Mor, Selene and Herzog, Marc and Noack, Johannes and Katayama, Naoyuki and Nohara, Minoru and Takagi, Hide and Trunschke, Annette and Mizokawa, Takashi and Monney, Claude and St{\"a}hler, Julia}, title = {Inhibition of the photoinduced structural phase transition in the excitonic insulator Ta2NiSe5}, series = {Physical review : B, Condensed matter and materials physics}, volume = {97}, journal = {Physical review : B, Condensed matter and materials physics}, number = {11}, publisher = {American Physical Society}, address = {College Park}, issn = {2469-9950}, doi = {10.1103/PhysRevB.97.115154}, pages = {5}, year = {2018}, abstract = {Femtosecond time-resolved midinfrared reflectivity is used to investigate the electron and phonon dynamics occurring at the direct band gap of the excitonic insulator Ta2NiSe5 below the critical temperature of its structural phase transition. We find that the phonon dynamics show a strong coupling to the excitation of free carriers at the Gamma point of the Brillouin zone. The optical response saturates at a critical excitation fluence F-C = 0.30 +/- 0.08 mJ/cm(2) due to optical absorption saturation. This limits the optical excitation density in Ta2NiSe5 so that the system cannot be pumped sufficiently strongly to undergo the structural change to the high-temperature phase. We thereby demonstrate that Ta2NiSe5 exhibits a blocking mechanism when pumped in the near-infrared regime, preventing a nonthermal structural phase transition.}, language = {en} } @article{PudellMaznevHerzogetal.2018, author = {Pudell, Jan-Etienne and Maznev, A. A. and Herzog, Marc and Kronseder, M. and Back, Christian H. and Malinowski, Gregory and Reppert, Alexander von and Bargheer, Matias}, title = {Layer specific observation of slow thermal equilibration in ultrathin metallic nanostructures by femtosecond X-ray diffraction}, series = {Nature Communications}, volume = {9}, journal = {Nature Communications}, publisher = {Nature Publ. Group}, address = {London}, issn = {2041-1723}, doi = {10.1038/s41467-018-05693-5}, pages = {7}, year = {2018}, abstract = {Ultrafast heat transport in nanoscale metal multilayers is of great interest in the context of optically induced demagnetization, remagnetization and switching. If the penetration depth of light exceeds the bilayer thickness, layer-specific information is unavailable from optical probes. Femtosecond diffraction experiments provide unique experimental access to heat transport over single digit nanometer distances. Here, we investigate the structural response and the energy flow in the ultrathin double-layer system: gold on ferromagnetic nickel. Even though the excitation pulse is incident from the Au side, we observe a very rapid heating of the Ni lattice, whereas the Au lattice initially remains cold. The subsequent heat transfer from Ni to the Au lattice is found to be two orders of magnitude slower than predicted by the conventional heat equation and much slower than electron-phonon coupling times in Au. We present a simplified model calculation highlighting the relevant thermophysical quantities.}, language = {en} } @article{ReppertWilligPudelletal.2018, author = {Reppert, Alexander von and Willig, Lisa and Pudell, Jan-Etienne and Roessle, M. and Leitenberger, Wolfram and Herzog, Marc and Ganss, F. and Hellwig, O. and Bargheer, Matias}, title = {Ultrafast laser generated strain in granular and continuous FePt thin films}, series = {Applied physics letters}, volume = {113}, journal = {Applied physics letters}, number = {12}, publisher = {American Institute of Physics}, address = {Melville}, issn = {0003-6951}, doi = {10.1063/1.5050234}, pages = {5}, year = {2018}, abstract = {We employ ultrafast X-ray diffraction to compare the lattice dynamics of laser-excited continuous and granular FePt films on MgO (100) substrates. Contrary to recent results on free-standing granular films, we observe in both cases a pronounced and long-lasting out-of-plane expansion. We attribute this discrepancy to the in-plane expansion, which is suppressed by symmetry in continuous films. Granular films on substrates are less constrained and already show a reduced out-of-plane contraction. Via the Poisson effect, out-of-plane contractions drive in-plane expansion and vice versa. Consistently, the granular film exhibits a short-lived out-of-plane contraction driven by ultrafast demagnetization which is followed by a reduced and delayed expansion. From the acoustic reflections of the observed strain waves at the film-substrate interface, we extract a 13\% reduction of the elastic constants in thin 10 nm FePt films compared to bulk-like samples. (C) 2018 Author(s).}, language = {en} } @article{ZeuschnerMatternPudelletal.2021, author = {Zeuschner, Steffen Peer and Mattern, Maximilian and Pudell, Jan-Etienne and Reppert, Alexander von and R{\"o}ssle, Matthias and Leitenberger, Wolfram and Schwarzkopf, Jutta and Boschker, Jos and Herzog, Marc and Bargheer, Matias}, title = {Reciprocal space slicing}, series = {Structural dynamics}, volume = {8}, journal = {Structural dynamics}, number = {1}, publisher = {AIP Publishing LLC}, address = {Melville, NY}, issn = {2329-7778}, doi = {10.1063/4.0000040}, pages = {10}, year = {2021}, abstract = {An experimental technique that allows faster assessment of out-of-plane strain dynamics of thin film heterostructures via x-ray diffraction is presented. In contrast to conventional high-speed reciprocal space-mapping setups, our approach reduces the measurement time drastically due to a fixed measurement geometry with a position-sensitive detector. This means that neither the incident (ω) nor the exit (2θ) diffraction angle is scanned during the strain assessment via x-ray diffraction. Shifts of diffraction peaks on the fixed x-ray area detector originate from an out-of-plane strain within the sample. Quantitative strain assessment requires the determination of a factor relating the observed shift to the change in the reciprocal lattice vector. The factor depends only on the widths of the peak along certain directions in reciprocal space, the diffraction angle of the studied reflection, and the resolution of the instrumental setup. We provide a full theoretical explanation and exemplify the concept with picosecond strain dynamics of a thin layer of NbO2.}, language = {en} } @article{PudellReppertSchicketal.2019, author = {Pudell, Jan-Etienne and Reppert, Alexander von and Schick, D. and Zamponi, F. and R{\"o}ssle, Matthias and Herzog, Marc and Zabel, Hartmut and Bargheer, Matias}, title = {Ultrafast negative thermal expansion driven by spin disorder}, series = {Physical review : B, Condensed matter and materials physics}, volume = {99}, journal = {Physical review : B, Condensed matter and materials physics}, number = {9}, publisher = {American Physical Society}, address = {College Park}, issn = {2469-9950}, doi = {10.1103/PhysRevB.99.094304}, pages = {7}, year = {2019}, abstract = {We measure the transient strain profile in a nanoscale multilayer system composed of yttrium, holmium, and niobium after laser excitation using ultrafast x-ray diffraction. The strain propagation through each layer is determined by transient changes in the material-specific Bragg angles. We experimentally derive the exponentially decreasing stress profile driving the strain wave and show that it closely matches the optical penetration depth. Below the Neel temperature of Ho, the optical excitation triggers negative thermal expansion, which is induced by a quasi-instantaneous contractive stress and a second contractive stress contribution increasing on a 12-ps timescale. These two timescales were recently measured for the spin disordering in Ho [Rettig et al., Phys. Rev. Lett. 116, 257202 (2016)]. As a consequence, we observe an unconventional bipolar strain pulse with an inverted sign traveling through the heterostructure.}, language = {en} } @article{SarhanKoopmanPudelletal.2019, author = {Sarhan, Radwan Mohamed and Koopman, Wouter-Willem Adriaan and Pudell, Jan-Etienne and Stete, Felix and R{\"o}ssle, Matthias and Herzog, Marc and Schmitt, Clemens Nikolaus Zeno and Liebig, Ferenc and Koetz, Joachim and Bargheer, Matias}, title = {Scaling up nanoplasmon catalysis}, series = {The journal of physical chemistry : C, Nanomaterials and interfaces}, volume = {123}, journal = {The journal of physical chemistry : C, Nanomaterials and interfaces}, number = {14}, publisher = {American Chemical Society}, address = {Washington}, issn = {1932-7447}, doi = {10.1021/acs.jpcc.8b12574}, pages = {9352 -- 9357}, year = {2019}, abstract = {Nanoscale heating by optical excitation of plasmonic nanoparticles offers a new perspective of controlling chemical reactions, where heat is not spatially uniform as in conventional macroscopic heating but strong temperature gradients exist around microscopic hot spots. In nanoplasmonics, metal particles act as a nanosource of light, heat, and energetic electrons driven by resonant excitation of their localized surface plasmon resonance. As an example of the coupling reaction of 4-nitrothiophenol into 4,4′-dimercaptoazobenzene, we show that besides the nanoscopic heat distribution at hot spots, the microscopic distribution of heat dictated by the spot size of the light focus also plays a crucial role in the design of plasmonic nanoreactors. Small sizes of laser spots enable high intensities to drive plasmon-assisted catalysis. This facilitates the observation of such reactions by surface-enhanced Raman scattering, but it challenges attempts to scale nanoplasmonic chemistry up to large areas, where the excess heat must be dissipated by one-dimensional heat transport.}, language = {en} } @article{PudellSanderBaueretal.2019, author = {Pudell, Jan-Etienne and Sander, M. and Bauer, R. and Bargheer, Matias and Herzog, Marc and Ga{\´a}l, Peter}, title = {Full Spatiotemporal Control of Laser-Excited Periodic Surface Deformations}, series = {Physical review applied}, volume = {12}, journal = {Physical review applied}, number = {2}, publisher = {American Physical Society}, address = {College Park}, issn = {2331-7019}, doi = {10.1103/PhysRevApplied.12.024036}, pages = {11}, year = {2019}, abstract = {We demonstrate full control of acoustic and thermal periodic deformations at solid surfaces down to subnanosecond time scales and few-micrometer length scales via independent variation of the temporal and spatial phase of two optical transient grating (TG) excitations. For this purpose, we introduce an experimental setup that exerts control of the spatial phase of subsequent time-delayed TG excitations depending on their polarization state. Specific exemplary coherent control cases are discussed theoretically and corresponding experimental data are presented in which time-resolved x-ray reflectivity measures the spatiotemporal surface distortion of nanolayered heterostructures. Finally, we discuss examples where the application of our method may enable the control of functional material properties via tailored spatiotemporal strain fields.}, language = {en} } @article{SanderHerzogPudelletal.2017, author = {Sander, Mathias and Herzog, Marc and Pudell, Jan-Etienne and Bargheer, Matias and Weinkauf, N. and Pedersen, M. and Newby, G. and Sellmann, J. and Schwarzkopf, J. and Besse, V. and Temnov, V. V. and Gaal, P.}, title = {Spatiotemporal Coherent Control of Thermal Excitations in Solids}, series = {Physical review letters}, volume = {119}, journal = {Physical review letters}, publisher = {American Physical Society}, address = {College Park}, issn = {0031-9007}, doi = {10.1103/PhysRevLett.119.075901}, pages = {102 -- 110}, year = {2017}, abstract = {X-ray reflectivity measurements of femtosecond laser-induced transient gratings (TG) are applied to demonstrate the spatiotemporal coherent control of thermally induced surface deformations on ultrafast time scales. Using grazing incidence x-ray diffraction we unambiguously measure the amplitude of transient surface deformations with sub-angstrom resolution. Understanding the dynamics of femtosecond TG excitations in terms of superposition of acoustic and thermal gratings makes it possible to develop new ways of coherent control in x-ray diffraction experiments. Being the dominant source of TG signal, the long-living thermal grating with spatial period. can be canceled by a second, time-delayed TG excitation shifted by Lambda/2. The ultimate speed limits of such an ultrafast x-ray shutter are inferred from the detailed analysis of thermal and acoustic dynamics in TG experiments.}, language = {en} } @article{MorHerzogGolezetal.2017, author = {Mor, Selene and Herzog, Marc and Golez, Denis and Werner, Philipp and Eckstein, Martin and Katayama, Naoyuki and Nohara, Minoru and Takagi, Hide and Mizokawa, Takashi and Monney, Claude and Staehler, Julia}, title = {Ultrafast Electronic Band Gap Control in an Excitonic Insulator}, series = {Physical review letters}, volume = {119}, journal = {Physical review letters}, publisher = {American Physical Society}, address = {College Park}, issn = {0031-9007}, doi = {10.1103/PhysRevLett.119.086401}, pages = {11559 -- 11567}, year = {2017}, abstract = {We report on the nonequilibrium dynamics of the electronic structure of the layered semiconductor Ta2NiSe5 investigated by time-and angle-resolved photoelectron spectroscopy. We show that below the critical excitation density of F-C = 0.2 mJ cm(-2), the band gap narrows transiently, while it is enhanced above FC. Hartree-Fock calculations reveal that this effect can be explained by the presence of the low-temperature excitonic insulator phase of Ta2NiSe5, whose order parameter is connected to the gap size. This work demonstrates the ability to manipulate the band gap of Ta2NiSe5 with light on the femtosecond time scale.}, language = {en} } @article{SanderPudellHerzogetal.2017, author = {Sander, Mathias and Pudell, Jan-Etienne and Herzog, Marc and Bargheer, Matias and Bauer, R. and Besse, V. and Temnov, V. and Gaal, P.}, title = {Quantitative disentanglement of coherent and incoherent laser-induced surface deformations by time-resolved x-ray reflectivity}, series = {Applied physics letters}, volume = {111}, journal = {Applied physics letters}, publisher = {American Institute of Physics}, address = {Melville}, issn = {0003-6951}, doi = {10.1063/1.5004522}, pages = {4}, year = {2017}, abstract = {We present time-resolved x-ray reflectivity measurements on laser excited coherent and incoherent surface deformations of thin metallic films. Based on a kinematical diffraction model, we derive the surface amplitude from the diffracted x-ray intensity and resolve transient surface excursions with sub-angstrom spatial precision and 70 ps temporal resolution. The analysis allows for decomposition of the surface amplitude into multiple coherent acoustic modes and a substantial contribution from incoherent phonons which constitute the sample heating. Published by AIP Publishing.}, language = {en} } @article{ZeuschnerParpiievPezeriletal.2019, author = {Zeuschner, Steffen Peer and Parpiiev, Tymur and Pezeril, Thomas and Hillion, Arnaud and Dumesnil, Karine and Anane, Abdelmadjid and Pudell, Jan-Etienne and Willig, Lisa and R{\"o}ssle, Matthias and Herzog, Marc and Reppert, Alexander von and Bargheer, Matias}, title = {Tracking picosecond strain pulses in heterostructures that exhibit giant magnetostriction}, series = {Structural Dynamics}, volume = {6}, journal = {Structural Dynamics}, number = {2}, publisher = {AIP Publishing LLC}, address = {Melville, NY}, issn = {2329-7778}, doi = {10.1063/1.5084140}, pages = {9}, year = {2019}, abstract = {We combine ultrafast X-ray diffraction (UXRD) and time-resolved Magneto-Optical Kerr Effect (MOKE) measurements to monitor the strain pulses in laser-excited TbFe2/Nb heterostructures. Spatial separation of the Nb detection layer from the laser excitation region allows for a background-free characterization of the laser-generated strain pulses. We clearly observe symmetric bipolar strain pulses if the excited TbFe2 surface terminates the sample and a decomposition of the strain wavepacket into an asymmetric bipolar and a unipolar pulse, if a SiO2 glass capping layer covers the excited TbFe2 layer. The inverse magnetostriction of the temporally separated unipolar strain pulses in this sample leads to a MOKE signal that linearly depends on the strain pulse amplitude measured through UXRD. Linear chain model simulations accurately predict the timing and shape of UXRD and MOKE signals that are caused by the strain reflections from multiple interfaces in the heterostructure.}, 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.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{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{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{NavirianHerzogGoldshteynetal.2011, author = {Navirian, Hengameh A. and Herzog, Marc and Goldshteyn, J. and Leitenberger, Wolfram and Vrejoiu, Ionella and Khakhulin, D. and Wulff, M. and Shayduk, Roman and Gaal, P. and Bargheer, Matias}, title = {Shortening x-ray pulses for pump-probe experiments at synchrotrons}, series = {Journal of applied physics}, volume = {109}, journal = {Journal of applied physics}, number = {12}, publisher = {American Institute of Physics}, address = {Melville}, issn = {0021-8979}, doi = {10.1063/1.3601057}, pages = {3}, year = {2011}, abstract = {We implemented an experimental scheme for ultrafast x-ray diffraction at storage rings based on a laser-driven Bragg-switch that shortens the x-ray pulses emitted from an undulator. The increased time-resolution is demonstrated by observing changes of intensity, position and width of the diffraction peaks of a La(0.7)Sr(0.3)MnO(3)/SrTiO(3) superlattice sample after optical excitation, i.e., by quantitatively measuring the propagation of an expansion wave through the sample. These experimental transients with timescales of 35 to 60 ps evidence a reduction of the x-ray pulse duration by a factor of two.}, language = {en} } @article{ShaydukNavirianLeitenbergeretal.2011, author = {Shayduk, Roman and Navirian, Hengameh and Leitenberger, Wolfram and Goldshteyn, Jevgenij and Vrejoiu, Ionela and Weinelt, Martin and Gaal, Peter and Herzog, Marc and von Korff Schmising, Clemens and Bargheer, Matias}, title = {Nanoscale heat transport studied by high-resolution time-resolved x-ray diffraction}, series = {New journal of physics : the open-access journal for physics}, volume = {13}, journal = {New journal of physics : the open-access journal for physics}, number = {11}, publisher = {IOP Publ. Ltd.}, address = {Bristol}, issn = {1367-2630}, doi = {10.1088/1367-2630/13/9/093032}, pages = {11}, year = {2011}, abstract = {We report on synchrotron-based high-repetition rate ultrafast x-ray diffraction (UXRD) experiments monitoring the transport of heat from an epitaxial La(0.7)Sr(0.3)MnO(3)/SrTiO(3) superlattice (SL) into the substrate on timescales from 100 ps to 4 mu s. Transient thermal lattice expansion was determined with an accuracy of 10(-7), corresponding to a sensitivity to temperature changes down to 0.01 K. We follow the heat flow within the SL and into the substrate after the impulsive laser heating leads to a small temperature rise of Delta T = 6 K. The transient lattice temperature can be simulated very well using the bulk heat conductivities. This contradicts the interpretation of previous UXRD measurements, which predicted a long-lasting expansion of SrRuO(3) for more than 200 ps. The disagreement could be resolved by assuming that the heat conductivity changes in the first hundred picoseconds.}, 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{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{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{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{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{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{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{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{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{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{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{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} }