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 ...

University of Melbourne

The concept of an x-ray telescope based on the optics of the eye of certain types of crustacea has been in currency for nearly thirty years. However, it is only in the last decade that the technology to make the telescope and the opportunity to mount it on a suitable space platform have combined to allow the idea to become a reality. Accordingly, we have undertaken a detailed simulation study, updating previous simplified models, to properly characterise the performance of the instrument in orbit. The study reveals details of how the particular characteristics of the lobster-eye optics affect the sensitivity of the instrument and allow us to implement new ideas in data extraction methods.

Detailed simulation of a Lobster-eye telescope.

This Letter demonstrates that coherent diffractive imaging (CDI), in combination with phase-diversity methods, provides reliable and artefact free high-resolution images. Here, using x rays, experimental results show a threefold improvement in the available image contrast. Furthermore, in conditions requiring low imaging dose, it is demonstrated that phase-diverse CDI provides a factor of 2 improvement in comparison to previous CDI techniques.

Phase-diverse coherent diffractive imaging: high sensitivity with low dose.

As the resolution in coherent diffractive imaging improves, interexposure and intraexposure sample dynamics, such as motion, degrade the quality of the reconstructed image. Selecting data sets that include only exposures where tolerably little motion has occurred is an inefficient use of time and flux, especially when detector readout time is significant. We provide an experimental demonstration of an approach in which all images of a data set exhibiting sample motion are combined to improve the quality of a reconstruction. This approach is applicable to more general sample dynamics (including sample damage) that occur during measurement.

Dynamic sample imaging in coherent diffractive imaging.

We introduce theoretically and demonstrate experimentally a contrast transfer function based phase retrieval algorithm that reconstructs the projected thickness of an homogeneous sample using a polychromatic x-ray source. We show excellent quantitative recovery of test samples in 2D using a synchrotron source with significant harmonic contamination, and in 3D using a laboratory source.

Quantitative phase imaging with polychromatic x-ray sources.

This paper demonstrates the application of the high sensitivity, low radiation dose imaging method recently presented as phase diverse coherent diffraction imaging, to the study of biological and other weakly scattering samples. The method is applied, using X-ray illumination, to quantitative imaging of the granular precursors of underwater adhesive produced by the marine sandcastle worm, Phragmatopoma californica. We are able to observe the internal structure of the adhesive precursors in a number of states.

Mapping granular structure in the biological adhesive of Phragmatopoma californica using phase diverse coherent diffractive imaging.

We report experimental demonstrations of a quantitative technique for elemental mapping. The technique operates in full-field imaging mode and uses three intensity measurements at energies across an absorption edge of an element of interest to obtain its elemental distribution. The experimental results show that the technique can overcome some limitations in the conventional Absorption Edge Contrast Imaging. The technique allows for an accurate determination of the elemental distribution in a compound sample even at a low level of percentage composition. It is also robust to the choice of energy intervals.

Multi-wavelength elemental contrast absorption imaging.

Ptychographic coherent diffractive imaging (CDI) has been extensively applied using both x rays and electrons. The extension to atomic resolution has been elusive. This Letter demonstrates ptychographic electron diffractive imaging at atomic resolution, permitting identification of structure in a boron nitride helical cone at a resolution of order 1 Å, beyond that of comparative Z-contrast images. A scanning transmission electron microscope is used to create a diverging illumination in a defocused Fresnel CDI geometry, providing a robust strategy leading to a unique solution.

Atom-scale ptychographic electron diffractive imaging of boron nitride cones.

We describe the spatial coherence properties of a cold atom electron source in the framework of a quasihomogeneous wavefield. The model is used as the basis for direct measurements of the transverse spatial coherence length of electron bunches extracted from a cold atom electron source. The coherence length is determined from the measured visibility of a propagated electron distribution with a sinusoidal profile of variable spatial frequency. The electron distribution was controlled via the intensity profile of an atomic excitation laser beam patterned with a spatial light modulator. We measure a lower limit to the coherence length at the source of lc = 7.8 ± 0.9 nm.

Spatial coherence of electron bunches extracted from an arbitrarily shaped cold atom electron source.

X-ray tomography can provide structural information of whole cells in close to their native state. Radiation-induced damage, however, imposes a practical limit to image resolution, and as such, a choice between damage, image contrast, and image resolution must be made. New coherent diffractive imaging techniques, such Fresnel Coherent Diffractive Imaging (FCDI), allows quantitative phase information with exceptional dose efficiency, high contrast, and nano-scale resolution. Here we present three-dimensional quantitative images of a whole eukaryotic cell by FCDI at a spatial resolution below 70 nm with sufficient phase contrast to distinguish major cellular components. From our data, we estimate that the minimum dose required for a similar resolution is close to that predicted by the Rose criterion, considerably below accepted estimates of the maximum dose a frozen-hydrated cell can tolerate. Based on the dose efficiency, contrast, and resolution achieved, we expect this technique will find immediate applications in tomographic cellular characterisation.

Whole-cell phase contrast imaging at the nanoscale using Fresnel coherent diffractive imaging tomography.

Phase-diverse X-ray coherent diffractive imaging (CDI) provides a route to high sensitivity and spatial resolution with moderate radiation dose. It also provides a robust solution to the well-known phase-problem, making on-line image reconstruction feasible. Here we apply phase-diverse CDI to a cellular sample, obtaining images of an erythrocyte infected by the sexual stage of the malaria parasite, Plasmodium falciparum, with a radiation dose significantly lower than the lowest dose previously reported for cellular imaging using CDI. The high sensitivity and resolution allow key biological features to be identified within intact cells, providing complementary information to optical and electron microscopy. This high throughput method could be used for fast tomographic imaging, or to generate multiple replicates in two-dimensions of hydrated biological systems without freezing or fixing. This work demonstrates that phase-diverse CDI is a valuable complementary imaging method for the biological sciences and ready for immediate application.

Rapid, low dose X-ray diffractive imaging of the malaria parasite Plasmodium falciparum.

We present a deterministic approach to the ptychographic retrieval of the wave at the exit surface of a specimen of condensed matter illuminated by X-rays. The method is based on the solution of an overdetermined set of linear equations, and is robust to measurement noise. The set of linear equations is efficiently solved using the conjugate gradient least-squares method implemented using fast Fourier transforms. The method is demonstrated using a data set obtained from a gold-chromium nanostructured test object. It is shown that the transmission function retrieved by this linear method is quantitatively comparable with established methods of ptychography, with a large decrease in computational time, and is thus a good candidate for real-time reconstruction.

Fast deterministic ptychographic imaging using X-rays.

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.

Article	Year
Detailed simulation of a Lobster-eye telescope. Optics express\| PubMed ID: 19654826	2009
Phase-diverse coherent diffractive imaging: high sensitivity with low dose. Physical review letters\| PubMed ID: 21231742	2011
Dynamic sample imaging in coherent diffractive imaging. Optics letters\| PubMed ID: 21633413	2011
Quantitative phase imaging with polychromatic x-ray sources. Optics express\| PubMed ID: 21643063	2011
Mapping granular structure in the biological adhesive of Phragmatopoma californica using phase diverse coherent diffractive imaging. Ultramicroscopy\| PubMed ID: 21762656	2011
Multi-wavelength elemental contrast absorption imaging. Optics express\| PubMed ID: 22274185	2011
Atom-scale ptychographic electron diffractive imaging of boron nitride cones. Physical review letters\| PubMed ID: 22401205	2012
Spatial coherence of electron bunches extracted from an arbitrarily shaped cold atom electron source. Optics express\| PubMed ID: 22418153	2012
Whole-cell phase contrast imaging at the nanoscale using Fresnel coherent diffractive imaging tomography. Scientific reports\| PubMed ID: 23887204	2013
Rapid, low dose X-ray diffractive imaging of the malaria parasite Plasmodium falciparum. Ultramicroscopy\| PubMed ID: 24209602	2014
Fast deterministic ptychographic imaging using X-rays. Microscopy and microanalysis : the official journal of Microscopy Society of America, Microbeam Analysis Society, Microscopical Society of Canada\| PubMed ID: 24851899	2014
X-ray laser-induced electron dynamics observed by femtosecond diffraction from nanocrystals of Buckminsterfullerene. Science advances\| PubMed ID: 27626076	2016

Corey T. Putkunz

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