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Experimental 3D Coherent Diffractive Imaging from photon-sparse random projections

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 Added by Klaus Giewekemeyer
 Publication date 2018
  fields Physics
and research's language is English




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The routine atomic-resolution structure determination of single particles is expected to have profound implications for probing the structure-function relationship in systems ranging from energy materials to biological molecules. Extremely-bright, ultrashort-pulse X-ray sources---X-ray Free Electron Lasers (XFELs)---provide X-rays that can be used to probe ensembles of nearly identical nano-scale particles. When combined with coherent diffractive imaging, these objects can be imaged; however, as the resolution of the images approaches the atomic scale, the measured data are increasingly difficult to obtain and, during an X-ray pulse, the number of photons incident on the two-dimensional detector is much smaller than the number of pixels. This latter concern, the signal sparsity, materially impedes the application of the method. We demonstrate an experimental analog using a synchrotron X-ray source that yields signal levels comparable to those expected from single biomolecules illuminated by focused XFEL pulses. The analog experiment provides an invaluable cross-check on the fidelity of the reconstructed data that is not available during XFEL experiments. We establish---using this experimental data---that a sparsity of order $1.3times10^{-3}$ photons per pixel per frame can be overcome, lending vital insight to the solution of the atomic-resolution XFEL single particle imaging problem by experimentally demonstrating 3D coherent diffractive imaging from photon-sparse random projections.



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Coherent diffractive imaging (CDI) has been widely applied in the physical and biological sciences using synchrotron radiation, XFELs, high harmonic generation, electrons and optical lasers. One of CDIs important applications is to probe dynamic phenomena with high spatio-temporal resolution. Here, we report the development of a general in situ CDI method for real-time imaging of dynamic processes in solution. By introducing a time-invariant overlapping region as a real-space constraint, we show that in situ CDI can simultaneously reconstruct a time series of the complex exit wave of dynamic processes with robust and fast convergence. We validate this method using numerical simulations with coherent X-rays and performing experiments on a materials science and a biological specimen in solution with an optical laser. Our numerical simulations further indicate that in situ CDI can potentially reduce the radiation dose by more than an order of magnitude relative to conventional CDI. As coherent X-rays are under rapid development worldwide, we expect in situ CDI could be applied to probe dynamic phenomena ranging from electrochemistry, structural phase transitions, charge transfer, transport, crystal nucleation, melting and fluid dynamics to biological imaging.
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