measurements-long-range-electronic-correlations-during-femtosecond

Measurements of Long-range Electronic Correlations During Femtosecond Diffraction Experiments Performed on Nanocrystals of Buckminsterfullerene

The precise details of the interaction of intense X-ray pulses with matter are a topic of intense interest to researchers attempting to interpret the ...

X-ray free-electron lasers (XFELs) deliver x-ray pulses with a coherent flux that is approximately eight orders of magnitude greater than that available from a modern third-generation synchrotron source. The power density of an XFEL pulse may be so high that it can modify the electronic properties of a sample on a femtosecond time scale. Exploration of the interaction of intense coherent x-ray pulses and matter is both of intrinsic scientific interest and of critical importance to the interpretation of experiments that probe the structures of materials using high-brightness femtosecond XFEL pulses. We report observations of the diffraction of extremely intense 32-fs nanofocused x-ray pulses by a powder sample of crystalline C60. We find that the diffraction pattern at the highest available incident power significantly differs from the one obtained using either third-generation synchrotron sources or XFEL sources operating at low output power and does not correspond to the diffraction pattern expected from any known phase of crystalline C60. We interpret these data as evidence of a long-range, coherent dynamic electronic distortion that is driven by the interaction of the periodic array of C60 molecular targets with intense x-ray pulses of femtosecond duration.

X-ray laser-induced electron dynamics observed by femtosecond diffraction from nanocrystals of Buckminsterfullerene.

Since the discovery of high-transition-temperature (high-T(c)) superconductivity in layered copper oxides, many researchers have searched for similar behaviour in other layered metal oxides involving 3d-transition metals, such as cobalt and nickel. Such attempts have so far failed, with the result that the copper oxide layer is thought to be essential for superconductivity. Here we report that Na(x)CoO2*yH2O (x approximately 0.35, y approximately 1.3) is a superconductor with a T(c) of about 5 K. This compound consists of two-dimensional CoO2 layers separated by a thick insulating layer of Na+ ions and H2O molecules. There is a marked resemblance in superconducting properties between the present material and high-T(c) copper oxides, suggesting that the two systems have similar underlying physics.

Superconductivity in two-dimensional CoO2 layers.

A novel approach to X-ray diffraction data analysis for nondestructive determination of the shape of nanoscale particles and clusters in three-dimensions is illustrated with representative examples of composite nanostructures. The technique is insensitive to the X-ray coherence, which allows 3-D reconstruction of a modal image without tomographic synthesis and in situ analysis of large (over a several cubic millimeters) volume of material with a spatial resolution of few nanometers, rendering the approach suitable for laboratory facilities.

3-D X-ray diffraction imaging with nanoscale resolution using incoherent radiation.

A method is proposed that uses maximum entropy analysis of a Young's two-slit interference pattern for the measurement of the spectrum of a high-harmonic-generation light source. The approach is tested using experimental data, and the results are found to be consistent with those obtained directly using a grazing incidence spectrometer.

High-harmonic-generation spectrum reconstruction from Young's double-slits interference pattern using the maximum entropy method.

The recent development of X-ray free-electron laser sources has created new opportunities for the structural analysis of protein nanocrystals. The extremely small sizes of the crystals, as well as imperfections of the crystal structure, result in an interference phenomenon in the diffraction pattern. With decreasing crystallite size the structural imperfections play a role in the formation of the diffraction pattern that is comparable in importance to the size effects and should be taken into account during the data analysis and structure reconstruction processes. There now exists a need to develop new methods of protein structure determination that do not depend on the availability of good-quality crystals and that can treat proteins under conditions close to the active form. This paper demonstrates an approach that is specifically tailored to nanocrystalline samples and offers a unique crystallographic solution.

Continuous X-ray diffractive field in protein nanocrystallography.

Serial femtosecond X-ray crystallography (SFX) has created new opportunities in the field of structural analysis of protein nanocrystals. The intensity and timescale characteristics of the X-ray free-electron laser sources used in SFX experiments necessitate the analysis of a large collection of individual crystals of variable shape and quality to ultimately solve a single, average crystal structure. Ensembles of crystals are commonly encountered in powder diffraction, but serial crystallography is different because each crystal is measured individually and can be oriented via indexing and merged into a three-dimensional data set, as is done for conventional crystallography data. In this way, serial femtosecond crystallography data lie in between conventional crystallography data and powder diffraction data, sharing features of both. The extremely small sizes of nanocrystals, as well as the possible imperfections of their crystallite structure, significantly affect the diffraction pattern and raise the question of how best to extract accurate structure-factor moduli from serial crystallography data. Here it is demonstrated that whole-pattern fitting techniques established for one-dimensional powder diffraction analysis can be feasibly extended to higher dimensions for the analysis of merged SFX diffraction data. It is shown that for very small crystals, whole-pattern fitting methods are more accurate than Monte Carlo integration methods that are currently used.

Article	Year
X-ray laser-induced electron dynamics observed by femtosecond diffraction from nanocrystals of Buckminsterfullerene. Science advances\| PubMed ID: 27626076	2016
Superconductivity in two-dimensional CoO2 layers. Nature\| PubMed ID: 12621429	2003
3-D X-ray diffraction imaging with nanoscale resolution using incoherent radiation. Nano letters\| PubMed ID: 17419659	2007
High-harmonic-generation spectrum reconstruction from Young's double-slits interference pattern using the maximum entropy method. Optics letters\| PubMed ID: 18923616	2008
Continuous X-ray diffractive field in protein nanocrystallography. Acta crystallographica. Section A, Foundations of crystallography\| PubMed ID: 23250067	2013
Whole-pattern fitting technique in serial femtosecond nanocrystallography. IUCrJ\| PubMed ID: 27006776	2016

Ruben A. Dilanian

Biography

JoVE Journal Publications

Other Publications