| 1. |
- Gaffney, K J, et al.
(författare)
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Observation of structural anisotropy and the onset of liquidlike motion during the nonthermal melting of InSb
- 2005
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Ingår i: Physical Review Letters. - : American Physical Society. - 0031-9007 .- 1079-7114. ; 95:12
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Tidskriftsartikel (refereegranskat)abstract
- The melting dynamics of laser excited InSb have been studied with femtosecond x-ray diffraction. These measurements observe the delayed onset of diffusive atomic motion, signaling the appearance of liquidlike dynamics. They also demonstrate that the root-mean-squared displacement in the [111] direction increases faster than in the [110] direction after the first 500 fs. This structural anisotropy indicates that the initially generated fluid differs significantly from the equilibrium liquid.
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| 2. |
- Cavalieri, A L, et al.
(författare)
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Clocking femtosecond X rays.
- 2005
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Ingår i: Phys Rev Lett. - 0031-9007. ; 94:11
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Tidskriftsartikel (refereegranskat)abstract
- Linear-accelerator-based sources will revolutionize ultrafast x-ray science due to their unprecedented brightness and short pulse duration. However, time-resolved studies at the resolution of the x-ray pulse duration are hampered by the inability to precisely synchronize an external laser to the accelerator. At the Sub-Picosecond Pulse Source at the Stanford Linear-Accelerator Center we solved this problem by measuring the arrival time of each high energy electron bunch with electro-optic sampling. This measurement indirectly determined the arrival time of each x-ray pulse relative to an external pump laser pulse with a time resolution of better than 60 fs rms.
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| 3. |
- Maldonado, Pablo, et al.
(författare)
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Tracking the ultrafast nonequilibrium energy flow between electronic and lattice degrees of freedom in crystalline nickel
- 2020
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Ingår i: Physical Review B. - : AMER PHYSICAL SOC. - 2469-9950 .- 2469-9969. ; 101:10
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Tidskriftsartikel (refereegranskat)abstract
- Femtosecond laser excitation of solid-state systems creates out-of-equilibrium hot electrons that cool down by transferring their energy to other degrees of freedom and ultimately to lattice vibrations of the solid. By combining ab initio calculations with ultrafast diffuse electron scattering, we gain a detailed understanding of the complex nonequilibrium energy transfer between electrons and phonons in laser-excited Ni metal. Our experimental results show that the wave-vector-resolved population dynamics of phonon modes is distinctly different throughout the Brillouin zone and are in remarkable agreement with our theoretical results. We find that zone-boundary phonon modes become occupied first. As soon as the energy in these modes becomes larger than the average electron energy, a backflow of energy from lattice to electronic degrees of freedom occurs. Subsequent excitation of lower-energy phonon modes drives the thermalization of the whole system on the picosecond time scale. We determine the evolving nonequilibrium phonon occupations, which we find to deviate markedly from thermal occupations.
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| 4. |
- Chalupsky, J., et al.
(författare)
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Characteristics of focused soft X-ray free-electron laser beam determined by ablation of organic molecular solids
- 2007
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Ingår i: Optics Express. - 1094-4087. ; 15:10, s. 6036-6043
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Tidskriftsartikel (refereegranskat)abstract
- A linear accelerator based source of coherent radiation, FLASH (Free-electron LASer in Hamburg) provides ultra-intense femtosecond radiation pulses at wavelengths from the extreme ultraviolet (XUV; lambda< 100nm) to the soft X-ray (SXR; lambda<30nm) spectral regions. 25-fs pulses of 32-nm FLASH radiation were used to determine the ablation parameters of PMMA - poly ( methyl methacrylate). Under these irradiation conditions the attenuation length and ablation threshold were found to be (56.9 +/- 7.5) nm and similar to 2 mJ center dot cm(-2), respectively. For a second wavelength of 21.7 nm, the PMMA ablation was utilized to image the transverse intensity distribution within the focused beam at mu m resolution by a method developed here.
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| 5. |
- Chen, F., et al.
(författare)
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Reply to "comment on 'Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO3 ' "
- 2018
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Ingår i: Physical Review B. - 2469-9950. ; 97:22
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Tidskriftsartikel (refereegranskat)abstract
- In this reply to S. Durbin's comment on our original paper "Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO3," we concur that his final equations 8 and 9 more accurately describe the change in diffracted intensity as a function of Ti displacement. We also provide an alternative derivation based on an ensemble average over unit cells. The conclusions of the paper are unaffected by this correction.
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| 6. |
- Chen, F., et al.
(författare)
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Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO3
- 2016
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Ingår i: Physical Review B. - 1098-0121. ; 94:18
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Tidskriftsartikel (refereegranskat)abstract
- The dynamical processes associated with electric field manipulation of the polarization in a ferroelectric remain largely unknown but fundamentally determine the speed and functionality of ferroelectric materials and devices. Here we apply subpicosecond duration, single-cycle terahertz pulses as an ultrafast electric field bias to prototypical BaTiO3 ferroelectric thin films with the atomic-scale response probed by femtosecond x-ray-scattering techniques. We show that electric fields applied perpendicular to the ferroelectric polarization drive large-amplitude displacements of the titanium atoms along the ferroelectric polarization axis, comparable to that of the built-in displacements associated with the intrinsic polarization and incoherent across unit cells. This effect is associated with a dynamic rotation of the ferroelectric polarization switching on and then off on picosecond time scales. These transient polarization modulations are followed by long-lived vibrational heating effects driven by resonant excitation of the ferroelectric soft mode, as reflected in changes in the c-axis tetragonality. The ultrafast structural characterization described here enables a direct comparison with first-principles-based molecular-dynamics simulations, with good agreement obtained.
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| 7. |
- Fritz, D. M., et al.
(författare)
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Ultrafast bond softening in bismuth : Mapping a solid's interatomic potential with X-rays
- 2007
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Ingår i: Science. - : American Association for the Advancement of Science (AAAS). - 0036-8075 .- 1095-9203. ; 315:5812, s. 633-636
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Tidskriftsartikel (refereegranskat)abstract
- Intense femtosecond laser excitation can produce transient states of matter that would otherwise be inaccessible to laboratory investigation. At high excitation densities, the interatomic forces that bind solids and determine many of their properties can be substantially altered. Here, we present the detailed mapping of the carrier density-dependent interatomic potential of bismuth approaching a solid-solid phase transition. Our experiments combine stroboscopic techniques that use a high-brightness linear electron accelerator-based x-ray source with pulse-by-pulse timing reconstruction for femtosecond resolution, allowing quantitative characterization of the interatomic potential energy surface of the highly excited solid.
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| 8. |
- Hau-Riege, S. P., et al.
(författare)
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Damage threshold of inorganic solids under free-electron-laser irradiation at 32.5 nm wavelength
- 2007
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Ingår i: Applied Physics Letters. - : AIP Publishing. - 0003-6951 .- 1077-3118. ; 90:17, s. 173128-
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Tidskriftsartikel (refereegranskat)abstract
- Samples of B4C, amorphous C, chemical-vapor-deposition-diamond C, Si, and SiC were exposed to single 25 fs long pulses of 32.5 nm free-electron-laser radiation at fluences of up to 2.2 J/cm(2). The samples were chosen as candidate materials for x-ray free-electron-laser optics. It was found that the threshold for surface damage is on the order of the fluence required for thermal melting. For larger fluences, the crater depths correspond to temperatures on the order of the critical temperature, suggesting that the craters are formed by two-phase vaporization.
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| 9. |
- Hillyard, P. B., et al.
(författare)
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Carrier-density-dependent lattice stability in InSb
- 2007
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Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 98:12, s. 125501-
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Tidskriftsartikel (refereegranskat)abstract
- The ultrafast decay of the x-ray diffraction intensity following laser excitation of an InSb crystal has been utilized to observe carrier dependent changes in the potential energy surface. For the first time, an abrupt carrier dependent onset for potential energy surface softening and the appearance of accelerated atomic disordering for a very high average carrier density have been observed. Inertial dynamics dominate the early stages of crystal disordering for a wide range of carrier densities between the onset of crystal softening and the appearance of accelerated atomic disordering.
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| 10. |
- Lindenberg, AM, et al.
(författare)
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Atomic-scale visualization of inertial dynamics
- 2005
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Ingår i: Science. - : American Association for the Advancement of Science (AAAS). - 1095-9203 .- 0036-8075. ; 308:5720, s. 392-395
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Tidskriftsartikel (refereegranskat)abstract
- The motion of atoms on interatomic potential energy surfaces is fundamental to the dynamics of liquids and solids. An accelerator-based source of femtosecond x-ray pulses allowed us to follow directly atomic displacements on an optically modified energy landscape, leading eventually to the transition from crystalline solid to disordered liquid. We show that, to first order in time, the dynamics are inertial, and we place constraints on the shape and curvature of the transition-state potential energy surface. Our measurements point toward analogies between this nonequilibrium phase transition and the short-time dynamics intrinsic to equilibrium liquids.
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| 11. |
- Lindenberg, A.M., et al.
(författare)
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Ultrafast x-ray measurements of inertial atomic-scale motion
- 2005
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Ingår i: Quantum Electronics and Laser Science Conference. ; , s. 742-744
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Konferensbidrag (refereegranskat)abstract
- Using a new, accelerator-based source of femtosecond x-rays, we directly measure atomic displacements on an optically-modified potential energy surface. It is shown that the short time dynamics are predominantly inertial in character.
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| 12. |
- Lindenberg, A. M., et al.
(författare)
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X-ray diffuse scattering measurements of nucleation dynamics at femtosecond resolution.
- 2008
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Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 100:13, s. 135502-1-135502-5
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Tidskriftsartikel (refereegranskat)abstract
- Femtosecond time-resolved small and wide angle x-ray diffuse scattering techniques are applied to investigate the ultrafast nucleation processes that occur during the ablation process in semiconducting materials. Following intense optical excitation, a transient liquid state of high compressibility characterized by large-amplitude density fluctuations is observed and the buildup of these fluctuations is measured in real time. Small-angle scattering measurements reveal snapshots of the spontaneous nucleation of nanoscale voids within a metastable liquid and support theoretical predictions of the ablation process.
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| 13. |
- Trigo, M., et al.
(författare)
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Fourier-transform inelastic X-ray scattering from time- and momentum-dependent phonon-phonon correlations
- 2013
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Ingår i: Nature Physics. - 1745-2473. ; 9:12, s. 790-794
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Tidskriftsartikel (refereegranskat)abstract
- The macroscopic characteristics of a material are determined by its elementary excitations, which dictate the response of the system to external stimuli. The spectrum of excitations is related to fluctuations in the density-density correlations and is typically measured through frequency-domain neutron(1) or X-ray(2-4) scattering. Time-domain measurements of these correlations could yield a more direct way to investigate the excitations of solids and their couplings both near to and far from equilibrium. Here we show that we can access large portions of the phonon dispersion of germanium by measuring the diffuse scattering from femtosecond X-ray free-electron laser pulses. A femtosecond optical laser pulse slightly quenches the vibrational frequencies, producing pairs of high-wavevector phonons with opposite momenta. These phonons manifest themselves as time-dependent coherences in the displacement correlations(5) probed by the X-ray scattering. As the coherences are preferentially created in regions of strong electron-phonon coupling, the time-resolved approach is a natural spectroscopic tool for probing low-energy collective excitations in solids, and their microscopic interactions.
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| 14. |
- Chapman, H N, et al.
(författare)
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Coherent imaging at FLASH
- 2009
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Ingår i: Journal of Physics, Conference Series. - : IOP Publishing. - 1742-6588 .- 1742-6596. ; 186:1, s. 012051-
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Tidskriftsartikel (refereegranskat)abstract
- We have carried out high-resolution single-pulse coherent diffractive imaging at the FLASH free-electron laser. The intense focused FEL pulse gives a high-resolution low-noise coherent diffraction pattern of an object before that object turns into a plasma and explodes. In particular we are developing imaging of biological specimens beyond conventional radiation damage resolution limits, developing imaging of ultrafast processes, and testing methods to characterize and perform single-particle imaging.
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| 15. |
- Hau-Riege, S. P., et al.
(författare)
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Force Field Benchmark of Organic Liquids : Density, Enthalpy of Vaporization, Heat Capacities, Surface Tension, Isothermal Compressibility, Volumetric Expansion Coefficient, and Dielectric Constant
- 2007
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Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 98:14, s. 145502-
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Tidskriftsartikel (refereegranskat)abstract
- At the recently built FLASH x-ray free-electron laser, we studied the reflectivity of Si/C multilayers with fluxes up to 3×1014W/cm2. Even though the nanostructures were ultimately completely destroyed, we found that they maintained their integrity and reflectance characteristics during the 25-fs-long pulse, with no evidence for any structural changes over lengths greater than 3Å. This experiment demonstrates that with intense ultrafast pulses, structural damage does not occur during the pulse, giving credence to the concept of diffraction imaging of single macromolecules.
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| 16. |
- Larsson, Jörgen, et al.
(författare)
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Opportunities and challenges using short-pulse X-ray sources.
- 2005
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Ingår i: Second International Conference on Photo-Induced Phase Transitions: Cooperative, Nonlinear and Functional Properties. - : IOP Publishing. - 1742-6588 .- 1742-6596. ; 21, s. 87-94
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Konferensbidrag (refereegranskat)abstract
- Free-electron lasers will change the way we carry out time-resolved X-ray experiments. At present date, we use laser-produced plasma sources or synchrotron radiation. Laser-produced plasma sources have short pulses, but unfortunately large pulse-to-pulse fluctuations and large divergence. Synchrotron radiation from third generation source provide collimated and stable beams, but unfortunately long pulses. This means that either the time-resolution is limited to 100 ps or rather complex set-ups involving slicing or streak cameras are needed. Hard X-ray free-electron lasers will combine the best properties of present-day sources and increase the number of photons by many orders of magnitude. Already today, a precursor to the free-electron lasers has been built at Stanford Linear Accelerator Centre (SLAC). The Sub-Picosecond Photon Source (SPPS) has already shown the opportunities and challenges of using short-pulse X-ray sources.
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