Theoretical study of electronic damage in single particle imaging experiments at XFELs for pulse durations 0.1 - 10 fs

X-ray free-electron lasers (XFELs) may allow to employ the single particle imaging (SPI) method to determine the structure of macromolecules that do not form stable crystals. Ultrashort pulses of 10 fs and less allow to outrun complete disintegration by Coulomb explosion and minimize radiation damage due to nuclear motion, but electronic damage is still present. The major contribution to the electronic damage comes from the plasma generated in the sample that is strongly dependent on the amount of Auger ionization. Since the Auger process has a characteristic time scale on the order of femtoseconds, one may expect that its contribution will be significantly reduced for attosecond pulses. Here, we study the effect of electronic damage on the SPI at pulse durations from 0.1 fs to 10 fs and in a large range of XFEL fluences to determine optimal conditions for imaging of biological samples. We analyzed the contribution of different electronic excitation processes and found that at fluences higher than $10^{13}$-$10^{15}$ photons/$mu$m$^2$ (depending on the photon energy and pulse duration) the diffracted signal saturates and does not increase further. A significant gain in the signal is obtained by reducing the pulse duration from 10 fs to 1 fs. Pulses below 1 fs duration do not give a significant gain in the scattering signal in comparison with 1 fs pulses. We also study the limits imposed on SPI by Compton scattering.

Intensity interferometry of single x-ray pulses from a synchrotron storage ring

We report on measurements of second-order intensity correlations at the high brilliance storage ring PETRA III using a prototype of the newly developed Adaptive Gain Integrating Pixel Detector (AGIPD). The detector recorded individual synchrotron radiation pulses with an x-ray photon energy of 14.4 keV and repetition rate of about 5 MHz. The second-order intensity correlation function was measured simultaneously at different spatial separations that allowed to determine the transverse coherence length at these x-ray energies. The measured values are in a good agreement with theoretical simulations based on the Gaussian Schell-model.

Ptychography imaging of the phase vortices in the x-ray beam formed by nanofocusing lenses

We present the ptychography reconstruction of the x-ray beam formed by nanofocusing lenses (NFLs) containing a number of phase singularities (vortices) in the vicinity of the focal plane. As a test object Siemens star pattern was used with the finest features of 50 nm for ptychography measurements. The extended ptychography iterative engine (ePIE) algorithm was applied to retrieve both complex illumination and object functions from the set of diffraction patterns. The reconstruction revealed the focus size of 91.4$pm$1.1 nm in horizontal and 70$pm$0.3 nm in vertical direction at full width at half maximum (FWHM). The complex probe function was propagated along the optical axis of the beam revealing the evolution of the phase singularities.

Hanbury Brown and Twiss interferometry at a free-electron laser

We present measurements of second- and higher-order intensity correlation functions (so-called Hanbury Brown and Twiss experiment) performed at the free-electron laser (FEL) FLASH in the non-linear regime of its operation. We demonstrate the high transverse coherence properties of the FEL beam with a degree of transverse coherence of about 80% and degeneracy parameter of the order 10^9 that makes it similar to laser sources. Intensity correlation measurements in spatial and frequency domain gave an estimate of the FEL average pulse duration of 50 fs. Our measurements of the higher-order correlation functions indicate that FEL radiation obeys Gaussian statistics, which is characteristic to chaotic sources.

Impact of ultrafast electronic damage in single particle x-ray imaging experiments

In single particle coherent x-ray diffraction imaging experiments, performed at x-ray free-electron lasers (XFELs), samples are exposed to intense x-ray pulses to obtain single-shot diffraction patterns. The high intensity induces electronic dynamics on the femtosecond time scale in the system, which can reduce the contrast of the obtained diffraction patterns and adds an isotropic background. We quantify the degradation of the diffraction pattern from ultrafast electronic damage by performing simulations on a biological sample exposed to x-ray pulses with different parameters. We find that the contrast is substantially reduced and the background is considerably strong only if almost all electrons are removed from their parent atoms. This happens at fluences of at least one order of magnitude larger than provided at currently available XFEL sources.