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Register a new userSingle-shot 3D structure determination of nanocrystals with femtosecond X-ray free electron laser pulses
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Coherent diffraction imaging (CDI) using synchrotron radiation, X-ray free electron lasers (X-FELs), high harmonic generation, soft X-ray lasers, and optical lasers has found broad applications across several disciplines. An active research direction in CDI is to determine the structure of single particles with intense, femtosecond X-FEL pulses based on diffraction-before-destruction scheme. However, single-shot 3D structure determination has not been experimentally realized yet. Here we report the first experimental demonstration of single-shot 3D structure determination of individual nanocrystals using ~10 femtosecond X-FEL pulses. Coherent diffraction patterns are collected from high-index-faceted nanocrystals, each struck by a single X-FEL pulse. Taking advantage of the symmetry of the nanocrystal, we reconstruct the 3D structure of each nanocrystal from a single-shot diffraction pattern at ~5.5 nm resolution. As symmetry exists in many nanocrystals and virus particles, this method can be applied to 3D structure studies of such particles at nanometer resolution on femtosecond time scales.
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X-ray Absorption Spectroscopy (XAS) is a widely used X-ray diagnostic method. While synchrotrons have large communities of XAS users, its use on X-Ray Free Electron Lasers (XFEL) facilities has been rather limited. At a first glance, the relatively narrow bandwidth and the highly fluctuating spectral structure of XFEL sources seem to prevent high-quality XAS measurements without accumulating over many shots. Here, we demonstrate for the first time the collection of single-shot XAS spectra on an XFEL, with error bars of only a few percent, over tens of eV. We show how this technique can be extended over wider spectral ranges towards Extended X-ray Absorption Fine Structure (EXAFS) measurements, by concatenating a few tens of single-shot measurements. Such results open indisputable perspectives for future femtosecond time resolved XAS studies, especially for transient processes that can be initiated at low repetition rate.
The fluctuations of the longitudinal coherence length expected from the worlds first hard X-ray Free Electron Laser, the Linac Coherent Light Source, are investigated. We analyze, on a shot-to-shot basis, series of power spectra generated from 1D-FEL simulations. We evaluate how the intrinsic noise in the spectral profile of the X-ray beam reflects on its longitudinal coherence length. We show that the spectral stability of the LCLS beam will allow coherent X-ray experiments with a reasonable acquisition time. We also propose a scheme to deliver single-mode X-ray radiation using a narrow bandpass monochromator.
The quantum mechanical motion of electrons in molecules and solids occurs on the sub-femtosecond timescale. Consequently, the study of ultrafast electronic phenomena requires the generation of laser pulses shorter than 1 fs and of sufficient intensity to interact with their target with high probability. Probing these dynamics with atomic-site specificity requires the extension of sub-femtosecond pulses to the soft X-ray spectral region. Here we report the generation of isolated GW-scale soft X-ray attosecond pulses with an X-ray free-electron laser. Our source has a pulse energy that is six orders of magnitude larger than any other source of isolated attosecond pulses in the soft X-ray spectral region, with a peak power in the tens of gigawatts. This unique combination of high intensity, high photon energy and short pulse duration enables the investigation of electron dynamics with X-ray non-linear spectroscopy and single-particle imaging.
We put forward a co-axial pump(optical)-probe(X-rays) experimental concept and show performance of the optical component. A Bessel beam generator with a central 100 micrometers-diameter hole (on the optical axis) was fabricated using femtosecond (fs) laser structuring inside a silica plate. This flat-axicon optical element produces a needle-like axial intensity distribution which can be used for the optical pump pulse. The fs-X-ray free electron laser (X-FEL) beam of sub-1 micrometer diameter can be introduced through the central hole along the optical axis onto a target as a probe. Different realisations of optical pump are discussed. Such optical elements facilitate alignment of ultra-short fs-pulses in space and time and can be used in light-matter interaction experiments at extreme energy densities on the surface and in the volume of targets. Full advantage of ultra-short 10 fs X-FEL probe pulses with fs-pump(optical) opens an unexplored temporal dimension of phase transitions and the fastest laser-induced rates of material heating and quenching. A wider field of applications of fs-laser-enabled structuring of materials and design of specific optical elements for astrophotonics is presented.
The experimental characterization of the spatial and temporal coherence properties of the free-electron laser in Hamburg (FLASH) at a wavelength of 8.0 nm is presented. Double pinhole diffraction patterns of single femtosecond pulses focused to a size of about 10 microns by 10 microns were measured. A transverse coherence length of 6.2 microns in the horizontal and 8.7 microns in the vertical direction was determined from the most coherent pulses. Using a split and delay unit the coherence time of the pulses produced in the same operation conditions of FLASH was measured to be 1.75 fs. From our experiment we estimated the degeneracy parameter of the FLASH beam to be on the order of $10^{10}$ to $10^{11}$, which exceeds the values of this parameter at any other source in the same energy range by many orders of magnitude.
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