@unpublished{CavalleriSidersTothetal., author = {Cavalleri, Andrea and Siders, Craig and Toth, Csaba and Squier, Jeff A. and Barty, C. P. J. and Wilson, K. R. and Sokolowski-Tinten, Klaus and von der Linde, Dietrich and Kammler, Martin and Horn- von Hoegen, Michael}, title = {Measurement of harmonic and anharmonic semi-conductor-lattice dynamics with ultrafast x-ray diffraction}, abstract = {Many fundamental processes in solids, such as heat transport and phase transitions involve atomic movement on ultrafast time-scales, but cannot be directly measured with visible light. Using ultrafast x-ray diffraction, atomic motion can be measured on its natural time-scale. Photo-excitation of bulk and layered semiconductors was achieved with 800-nm wavelength femtosecond laser pulses. Optical excitation triggers a chain of relaxation processes, causing rapid lattice heating, generation and propagation of stress/strain waves into the bulk and eventual anharmonic decay of coherent acoustic phonons into the thermal bath of the solid. While the first steps of carrier relaxation, excitation and decay of Raman-active optical phonons have been in the past characterized optically at surfaces, the bulk acoustic dynamics at longer times has not. We measure length scales of lattice excitation, thereby detecting ultrafast heat diffusion via fast electrons, coherent acoustic pulse propagation into the bulk or across buried interfaces and anharmonic damping of non-equilibrium acoustic phonons. The measurement is performed with sensitivity on lattice spacing of 10 femtometers (i.e., 3 nuclear diameters).}, language = {en} } @unpublished{SidersCavalleriTothetal., author = {Siders, Craig and Cavalleri, Andrea and Toth, Csaba and Squier Jeff A., and Barty, C. P. J. and Wilson, K. R. and Sokolowski-Tinten, Klaus and von der Linde, Dietrich and Kammler, Martin and Horn- von Hoegen, Michael}, title = {Ultrafast Nonthermal Melting of Femtosecond-laser-irradiated Germanium Measured by Ultrafast X-ray Diffraction}, abstract = {Many fundamental processes in nature, such as chemical reactions and phase transitions involve rearrangement of the constituent atoms. Such changes cannot be directly measured with visible light and occur transiently on time-scales comparable with the natural oscillation periods of atoms (femtoseconds to picoseconds). We present experiments on Ge-111 films irradiated with 100-fs 800-nm light pulses and probed by a time-delayed sub-ps x-ray pulse at 8 keV. After excitation of a dense electron-hole plasma within the 160-nm film, the ultrafast pathway of lattice disordering is measured as a function laser fluence. For close-to-threshold irradiation, inhomogeneous thermal melting, occurring via surface nucleation of the liquid phase and growth into the bulk determines the dynamics of the solid-to-liquid phase transition. For excitation at about twice the melting threshold, a nonthermal pathway, starting from a highly excited cold solid and relaxing into a hot liquid causes ultrafast melting. At long time delays, nearly perfect recrystallization of a (111) crystal is observed.}, language = {en} } @inproceedings{KammlerHornvonHoegenVossetal., author = {Kammler, Martin and Horn- von Hoegen, Michael and Voss, N. and Tringides, Michael C. and Menzel, Andreas and Conrad, E. H.}, title = {Surface Dynamics of Stepped Si(001) Studied by Temporal Leed Spectroscopy}, series = {Collective Diffusion on Surfaces: Correlation Effects and Adatom Interactions (NATO Science Series II: Mathematics, Physics and Chemistry}, volume = {29}, booktitle = {Collective Diffusion on Surfaces: Correlation Effects and Adatom Interactions (NATO Science Series II: Mathematics, Physics and Chemistry}, publisher = {Springer}, doi = {10.1007/978-94-010-0816-7_3}, pages = {23 -- 32}, abstract = {We present the first demonstration of Temporal LEED Spectroscopy's ability to measure surface dynamics as shown by a study of step dynamics on vicinal Si(001). While we measure activation energies consistent with other work, the observed microscopic mechanism driving the fluctuations is inconsistent with previous claims. We exclude evaporation/condensation of atoms from the steps as the rate limiting kinetics in the temperature range of this experiment. Possible reasons for these differences are discussed.}, language = {en} } @article{MenzelConradTringidesetal., author = {Menzel, Andreas and Conrad, E. H. and Tringides, Michael C. and Kammler, Martin and Horn- von Hoegen, Michael}, title = {Finite collection time effects in autocovariance function measurements}, series = {Journal of Applied Physics}, volume = {93}, journal = {Journal of Applied Physics}, number = {4}, publisher = {AIP Publishing}, doi = {10.1063/1.1537466}, pages = {2229 -- 2235}, abstract = {In this paper we discuss how finite data sets influence experimental measurements of the autocovariance function. Autocovariance estimators are biased, meaning that the expectation value for any measured autocovariance function is not identical to the actual autocovariance function. In this work we show that the measured autocovariance function for a finite length time series must become negative for some lag times. We derive analytic corrections to these finite time errors for different types of correlated random sequences. Our results explain the apparent anticorrelated noise observed in experimental observations.}, language = {en} } @article{KammlerHornvonHoegenVossetal., author = {Kammler, Martin and Horn- von Hoegen, Michael and Voss, N. and Tringides, Michael C. and Menzel, Andreas and Conrad, E. H.}, title = {Si(001) step dynamics: A temporal low-energy electron diffraction study}, series = {Physical Review B}, volume = {65}, journal = {Physical Review B}, number = {7}, publisher = {APS}, doi = {10.1103/PhysRevB.65.075312}, abstract = {We present equilibrium measurements of the dynamics of steps on Si(001) using temporal electron-diffraction spectroscopy. Activation energies and the rate limiting kinetics are identified for 950K<~T<~1130K. Unlike previous studies at higher temperatures, we can exclude evaporation and condensation of atoms or dimers from the step edges as the rate limiting process in this temperature regime. The possible reason for this difference is discussed in terms of a crossover from different rate-limiting kinetics.}, language = {en} } @article{SokolowskiTintenBlomeBlumsetal., author = {Sokolowski-Tinten, Klaus and Blome, Christian and Blums, Juris and Dietrich, Clemens and Tarsevitch, Alexander and Horn-von Hoegen, Michael and von der Linde, Dietrich and Cavalleri, Andrea and Kammler, Martin and Uschmann, Ingo and Foerster, Eckhart}, title = {Femtosecond X-ray Diffraction Study of Large Amplitude Coherent Optical Phonons in Laser-Excited Bismuth}, series = {Conference on Lasers and Electro-Optics, 1-6 June 2003, Baltimore, Maryland}, journal = {Conference on Lasers and Electro-Optics, 1-6 June 2003, Baltimore, Maryland}, publisher = {Optical Society of America}, abstract = {Femtosecond time-resolved X-ray diffraction was used to directly study optical phonons in laser-excited Bismuth. A periodic modulation of the diffraction efficiency reveals initially coherent lattice distortions with atomic displacements of nearly 10\% of the nearest- neighbor-distance.}, language = {en} } @article{LuNicoulShymanovichetal., author = {Lu, Wei and Nicoul, Matthieu and Shymanovich, Uladzimir and Tarsevitch, Alexander and Kammler, Martin and Horn-von Hoegen, Michael and von der Linde, Dietrich and Sokolowski-Tinten, Klaus}, title = {Extreme Phonon Softening in Laser-excited Bismuth - Towards an Inverse Peierls-transition}, series = {MRS Online Proceedings Library}, volume = {1230}, journal = {MRS Online Proceedings Library}, publisher = {Springer}, doi = {10.1557/PROC-1230-MM03-05}, abstract = {Large amplitude coherent optical phonons have been investigated in laser-excited Bismuth by means of femtosecond time-resolved X-ray diffraction. For absorbed laser fluences above 2 mJ/cm2, the experimental data reveal an extreme softening of the excited A1g-mode down to frequencies of about 1 THz, only 1/3 of the unperturbed A1g-frequency. At even stronger excitation the measured diffraction signals no longer exhibit an oscillatory behavior presenting strong indication that upon intense laser-excitation the Peierls-distortion, which defines the equilibrium structure of Bismuth, can be transiently reversed.}, language = {en} } @inproceedings{SidersCavalleriTothetal., author = {Siders, C. W. and Cavalleri, Andrea and T{\´o}th, Csaba and Wilson, K. R. and Squier, Jeff A. and Barty, C. P. J. and Kammler, Martin and Sokolowski-Tinten, Klaus and Horn-von Hoegen, Michael and von der Linde, D.}, title = {Femtosecond X-ray diffraction of short-pulse irradiated semiconductors}, series = {Summaries of Papers Presented at the Lasers and Electro-Optics. CLEO '02. Technical Diges, 24-24 May 2002, Long Beach, CA, USA}, booktitle = {Summaries of Papers Presented at the Lasers and Electro-Optics. CLEO '02. Technical Diges, 24-24 May 2002, Long Beach, CA, USA}, publisher = {IEEE}, doi = {10.1109/CLEO.2002.1033997}, pages = {297 -- 298}, abstract = {Summary form only given, as follow. Ultrafast optical-pump, X-ray diffraction probe experiments are providing new ways to study transient processes including the direct observation of the atomic motion by which many solid-state processes and chemical and biochemical reactions take place. Current table-top-terawatt femtosecond laser systems provide an attractive source of few-hundred femtosecond duration bursts of angstrom-scale X-ray radiation with fluxes comparable to standard rotating anode sources. Their compact size enables time resolved structural dynamics to be studied in the small laboratory with temporal resolution better than typical molecular vibrational periods. Ultrafast structural dynamics in crystalline samples are readily studied with such systems and experiments to be discussed in this talk include ultrafast non-thermal solid-to-liquid transition in thin single-crystal Ge-111 films grown on Si-111 substrates; ultrafast non-thermal solid-to-solid transitions in bulk vanadium dioxide from a low temperature insulating phase to a high temperature metallic phase; and harmonic and anharmonic coherent acoustic dynamics in layered Ge-111/Si-111 and bulk GaAs-111 samples. Future improvements in high-average power short-pulse lasers will enable the study of a wider class of materials such as amorphous solids or liquid-phase dynamics of simple molecules, while proposed 4th generation light sources based upon single-pass X-ray free-electron lasers will permit singleshot structural determination of complex biomolecules.}, language = {en} } @article{SokolowskiTintenBlomeBlumsetal., author = {Sokolowski-Tinten, Klaus and Blome, Christian and Blums, Juris and Cavalleri, Andrea and Dietrich, Clemens and Tarasevitch, Alexander and Uschmann, Ingo and F{\"o}rster, Eckhard and Kammler, Martin and Horn-von Hoegen, Michael and von der Linde, Dietrich}, title = {Femtosecond X-ray measurement of coherent lattice vibrations near the Lindemann stability limit}, series = {Nature}, volume = {422}, journal = {Nature}, number = {6929}, publisher = {Springer}, doi = {10.1038/nature01490}, pages = {287 -- 289}, abstract = {The study of phase-transition dynamics in solids beyond a time-averaged kinetic description requires direct measurement of the changes in the atomic configuration along the physical pathways leading to the new phase. The timescale of interest is in the range 10(-14) to 10(-12) s. Until recently, only optical techniques were capable of providing adequate time resolution, albeit with indirect sensitivity to structural arrangement. Ultrafast laser-induced changes of long-range order have recently been directly established for some materials using time-resolved X-ray diffraction. However, the measurement of the atomic displacements within the unit cell, as well as their relationship with the stability limit of a structural phase, has to date remained obscure. Here we report time-resolved X-ray diffraction measurements of the coherent atomic displacement of the lattice atoms in photoexcited bismuth close to a phase transition. Excitation of large-amplitude coherent optical phonons gives rise to a periodic modulation of the X-ray diffraction efficiency. Stronger excitation corresponding to atomic displacements exceeding 10 per cent of the nearest-neighbour distance-near the Lindemann limit-leads to a subsequent loss of long-range order, which is most probably due to melting of the material.}, language = {en} } @article{SokolowskiTintenHornvonHoegenvonderLindeetal., author = {Sokolowski-Tinten, Klaus and Horn-von Hoegen, Michael and von der Linde, D. and Cavalleri, Andrea and Siders, C. W. and Brown, F. L. H. and Leitner, D. M. and T{\´o}th, Csaba and Squier, Jeff A. and Barty, C. P. J. and Wilson, K. R. and Kammler, Martin}, title = {Transient lattice dynamics in fs-laser-excited semiconductors probed by ultrafast X-ray diffraction}, series = {Journal de Physique IV}, volume = {11}, journal = {Journal de Physique IV}, number = {Pr2}, publisher = {EDP}, doi = {10.1051/jp4:2001290}, pages = {473 -- 477}, abstract = {A study of lattice dynamics in fs-laser-excited crystalline bulk Ge and Ge/Si-heterostructures, using time-resolved x-ray diffraction, was presented. Fast energy transport deep into the bulk of the material, coherent acoustic phonon dynamics, lattice anharmonicity, and vibrational transport across a buried interfaces were observed. Graphs showing time-dependent shifts of the centroid of the measured rocking curves in the Ge-overlayer and in the Si-substrate for different fluences, were presented.}, language = {en} } @article{SokolowskiTintenCavalleriSidersetal., author = {Sokolowski-Tinten, Klaus and Cavalleri, Andrea and Siders, C. W. and Brown, F. L. H. and Leitner, D. M. and T{\´o}th, Csaba and Kammler, Martin and Horn-von Hoegen, Michael and von der Linde, D. and Squier, Jeff A. and Barty, C. P. J. and Wilson, K. R.}, title = {Time-resolved x-ray diffraction study of ultrafast acoustic phonon dynamics in Ge/Si-heterostructures}, series = {Chemical Physics}, volume = {66}, journal = {Chemical Physics}, publisher = {Springer}, doi = {10.1007/978-3-642-56546-5_81}, pages = {281 -- 283}, abstract = {Using time-resolved x-ray diffraction the ultafast strain dynamics in fs-laserexcited Ge/Si-heterostructures has been studied. A fluence dependent, anharmonic damping of the impulsively generated acoustic phonons and vibrational transport across the buried Ge/Si-interface are observed.}, language = {en} } @inproceedings{SokolowskiTintenBlomeDietrichetal., author = {Sokolowski-Tinten, Klaus and Blome, Christian and Dietrich, Clemens and Blums, Juris and Horn-von Hoegen, Michael and von der Linde, D. and Cavalleri, Andrea and Squier, Jeff A. and Kammler, Martin}, title = {Structural dynamics in laser-excited solids investigated with femtosecond x-ray diffraction}, series = {2002 Summaries of Papers Presented at the Quantum Electronics and Laser Science Conference, 19-24 May 2002, Long Beach, CA, USA}, booktitle = {2002 Summaries of Papers Presented at the Quantum Electronics and Laser Science Conference, 19-24 May 2002, Long Beach, CA, USA}, publisher = {IEEE}, doi = {10.1109/QELS.2002.1031182}, pages = {115 -- 116}, abstract = {Summary form only given. Ultrashort x-ray pulses offer a unique combination of atomic-scale spatial and temporal resolution, which permits direct measurements of structural transients on an ultrafast time scale. Using time-resolved X-ray diffraction with femtosecond, multi-keV X-ray pulses we have studied transient lattice dynamics in optically excited semiconductors.}, language = {en} }