Femtosecond X-ray Free-electron Laser Research Articles

Single-shot three-dimensional structure determination of nanocrystals with femtosecond X-ray free-electron laser pulses.

Conventional three-dimensional (3D) structure determination methods require either multiple measurements at different sample orientations or a collection of serial sections through a sample. Here we report the experimental demonstration of single-shot 3D structure determination of an object; in this case, individual gold nanocrystals at ~5.5 nm resolution using ~10 fs X-ray free-electron laser pulses. Coherent diffraction patterns are collected from high-index-faceted nanocrystals, each struck by an X-ray free-electron laser pulse. Taking advantage of the symmetry of the nanocrystal and the curvature of the Ewald sphere, we reconstruct the 3D structure of each nanocrystal from a single-shot diffraction pattern. By averaging a sufficient number of identical nanocrystals, this method may be used to determine the 3D structure of nanocrystals at atomic resolution. As symmetry exists in many virus particles, this method may also be applied to 3D structure studies of such particles at nanometer resolution on femtosecond time scales.

Determining electronic damage to biomolecular structures in x-ray free-electron-laser imaging experiments

The use of femtosecond pulses produced by x-ray free-electron-laser (XFEL) sources to image the structures of biomolecules involves a competition between the elastic scattering of photons to form a diffraction pattern and the damage initiated by inelastic collisions with the target. Since the electron density of the biomolecule changes rapidly throughout its interaction with a femtosecond XFEL pulse, the diffraction process measured in ``diffract and destroy'' experiments is, at best, partially coherent. It has been established that a detailed knowledge of these electrodynamical processes may be used to ameliorate the effects of damage in diffractive imaging experiments. It is shown here that, subject to conventional assumptions about the nature of the interactions, it is possible to characterize the extent of electronic damage in biomolecular imaging experiments using XFELs and to use this information transferably across similar systems. We develop a physical model of the interaction of a coherent x-ray pulse with a molecular system that describes the dynamical electronic response of the molecule. The resulting insights open a way forward for the measurement of atomic processes in such systems.

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Amorphous to crystalline phase transition in carbon induced by intense femtosecond x-ray free-electron laser pulses

We present the results of an experiment where amorphous carbon undergoes a phase transition induced by femtosecond 830 eV x-ray free-electron laser pulses. The phase transition threshold fluence is found to be 282 +/- 11 mJ/cm(2). Atomic force microscopy, photoelectron microscopy, and micro-Raman spectroscopy give experimental evidence for the phase transition in terms of a volume expansion, graphitization, and change of local order of the irradiated sample area. The interaction is modeled by an accurate time-dependent treatment of the ionization dynamics coupled to a two-temperature model. At the phase transition fluence threshold the free-electron density N-e is found to be at maximum 9 x 10(20) cm(-3) while the ion (atom) temperature is found to be 1050 K, e.g., above the crystallization activation temperature reported in the literature. This low ionization rate and high atom temperature suggest a thermally activated phase transition.

Femtosecond x-ray free electron laser pulse duration measurement from spectral correlation function

We present a novel method for measuring the duration of femtosecond x-ray pulses from self-amplified spontaneous emission free electron lasers by performing statistical analysis in the spectral domain. Analytical expressions of the spectral correlation function were derived in the linear regime to extract both the pulse duration and the spectrometer resolution. Numerical simulations confirmed that the method can be also used in the nonlinear regime. The method was demonstrated experimentally at the Linac Coherent Light Source by measuring pulse durations down to 13 fs FWHM.

Monochromatization of femtosecond X-ray free-electron laser pulses by means of quasi-forbidden bragg reflections from periodic multilayer structures

It is shown that the use of quasi-forbidden second-order reflections from a periodic multilayer structure Al2O3/B4C allows monochromatization of femtosecond X-ray free-electron laser pulses at level ΔE/E ≈ 0.04% with an efficiency of ∼60%. The intensity, shape, duration, and statistical characteristics of the reflected pulses are studied.

Phase retrieval from single biomolecule diffraction pattern

In this paper, we propose the SPR (sparse phase retrieval) method, which is a new phase retrieval method for coherent x-ray diffraction imaging (CXDI). Conventional phase retrieval methods effectively solve the problem for high signal-to-noise ratio measurements, but would not be sufficient for single biomolecular imaging which is expected to be realized with femto-second x-ray free electron laser pulses. The SPR method is based on the Bayesian statistics. It does not need to set the object boundary constraint that is required by the commonly used hybrid input-output (HIO) method, instead a prior distribution is defined with an exponential distribution and used for the estimation. Simulation results demonstrate that the proposed method reconstructs the electron density under a noisy condition even some central pixels are masked.

Focusing femtosecond X-ray free-electron laser pulses by refractive lenses

The possibility of using a parabolic refractive lens with initial X-ray free-electron laser (XFEL) pulses, i.e. without a monochromator, is analysed. It is assumed that the measurement time is longer than 0.3 fs, which is the time duration of a coherent pulse (spike). In this case one has to calculate the propagation of a monochromatic wave and then perform an integration of the intensity over the radiation spectrum. Here a general algorithm for calculating the propagation of time-dependent radiation in free space and through various objects is presented. Analytical formulae are derived describing the properties of the monochromatic beam focused by a system of one and two lenses. Computer simulations show that the European XFEL pulses can be focused with maximal efficiency, i.e. as for a monochromatic wave. This occurs even for nanofocusing lenses.

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Biomolecular imaging and electronic damage using X-ray free-electron lasers

Proposals to determine biomolecular structures from diffraction experiments using femtosecond X-ray free-electron laser (XFEL) pulses involve a conflict between the incident brightness required to achieve diffraction-limited atomic resolution and the electronic and structural damage induced by the illumination. Here we show that previous estimates of the conditions under which biomolecular structures may be obtained in this manner are unduly restrictive, because they are based on a coherent diffraction model that is not appropriate to the proposed interaction conditions. A more detailed imaging model derived from optical coherence theory and quantum electrodynamics is shown to be far more tolerant of electronic damage. The nuclear density is employed as the principal descriptor of molecular structure. The foundations of the approach may also be used to characterize electrodynamical processes by performing scattering experiments on complex molecules of known structure.

Spot size characterization of focused non-Gaussian X-ray laser beams

We present a new technique for the characterization of non-Gaussian laser beams which cannot be described by an analytical formula. As a generalization of the beam spot area we apply and refine the definition of so called effective area (A(eff)) [1] in order to avoid using the full-width at half maximum (FWHM) parameter which is inappropriate for non-Gaussian beams. Furthermore, we demonstrate a practical utilization of our technique for a femtosecond soft X-ray free-electron laser. The ablative imprints in poly(methyl methacrylate) - PMMA and amorphous carbon (a-C) are used to characterize the spatial beam profile and to determine the effective area. Two procedures of the effective area determination are presented in this work. An F-scan method, newly developed in this paper, appears to be a good candidate for the spatial beam diagnostics applicable to lasers of various kinds.

Towards time resolved core level photoelectron spectroscopy with femtosecond x-ray free-electron lasers

We have performed core level photoelectron spectroscopy on a W(110) single crystal with femtosecond XUV pulses from the free-electron laser at Hamburg (FLASH). We demonstrate experimentally and through theoretical modelling that for a suitable range of photon fluences per pulse, time-resolved photoemission experiments on solid surfaces are possible. Using FLASH pulses in combination with a synchronized optical laser, we have performed femtosecond time-resolved core-level photoelectron spectroscopy and observed sideband formation on the W 4f lines indicating a cross correlation between femtosecond optical and XUV pulses.