@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{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{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{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{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{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} } @misc{SarhanKoopmanSchuetzetal.2018, author = {Sarhan, Radwan Mohamed and Koopman, Wouter-Willem Adriaan and Schuetz, Roman and Schmid, Thomas and Liebig, Ferenc and Koetz, Joachim and Bargheer, Matias}, title = {The importance of plasmonic heating for the plasmondriven photodimerization of 4-nitrothiophenol}, series = {Postprints der Universit{\"a}t Potsdam Mathematisch-Naturwissenschaftliche Reihe}, journal = {Postprints der Universit{\"a}t Potsdam Mathematisch-Naturwissenschaftliche Reihe}, number = {698}, issn = {1866-8372}, doi = {10.25932/publishup-42719}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-427197}, pages = {8}, year = {2018}, abstract = {Metal nanoparticles form potent nanoreactors, driven by the optical generation of energetic electrons and nanoscale heat. The relative influence of these two factors on nanoscale chemistry is strongly debated. This article discusses the temperature dependence of the dimerization of 4-nitrothiophenol (4-NTP) into 4,4′-dimercaptoazobenzene (DMAB) adsorbed on gold nanoflowers by Surface-Enhanced Raman Scattering (SERS). Raman thermometry shows a significant optical heating of the particles. The ratio of the Stokes and the anti-Stokes Raman signal moreover demonstrates that the molecular temperature during the reaction rises beyond the average crystal lattice temperature of the plasmonic particles. The product bands have an even higher temperature than reactant bands, which suggests that the reaction proceeds preferentially at thermal hot spots. In addition, kinetic measurements of the reaction during external heating of the reaction environment yield a considerable rise of the reaction rate with temperature. Despite this significant heating effects, a comparison of SERS spectra recorded after heating the sample by an external heater to spectra recorded after prolonged illumination shows that the reaction is strictly photo-driven. While in both cases the temperature increase is comparable, the dimerization occurs only in the presence of light. Intensity dependent measurements at fixed temperatures confirm this finding.}, language = {en} } @article{NavirianShaydukLeitenbergeretal.2012, author = {Navirian, H. and Shayduk, R. and Leitenberger, Wolfram and Goldshteyn, J. and Gaal, P. and Bargheer, Matias}, title = {Synchrotron-based ultrafast x-ray diffraction at high repetition rates}, 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 = {6}, publisher = {American Institute of Physics}, address = {Melville}, issn = {0034-6748}, doi = {10.1063/1.4727872}, pages = {7}, year = {2012}, abstract = {We present a setup for ultrafast x-ray diffraction (UXRD) based at the storage ring BESSY II, in particular, a pump laser that excites the sample using 250 fs laser-pulses at repetition rates ranging from 208 kHz to 1.25 MHz. We discuss issues connected to the high heat-load and spatio-temporal alignment strategies in the context of a UXRD experiment at high repetition rates. The spatial overlap between laser pump and x-ray probe pulse is obtained with 10 mu m precision and transient lattice changes can be recorded with an accuracy of delta a/a(0) = 10(-6). We also compare time-resolved x-ray diffraction signals from a laser excited LSMO/STO superlattice with phonon dynamics simulations. From the analysis we determine the x-ray pulse duration to 120 ps in standard operation mode and below 10 ps in low-alpha mode.}, 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{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} }