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Register a new userChrono CDI: Coherent diffractive imaging of time-evolving samples
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Bragg coherent x-ray diffractive imaging is a powerful technique for investigating dynamic nanoscale processes in nanoparticles immersed in reactive, realistic environments. Its temporal resolution is limited, however, by the oversampling requirements of 3D phase retrieval. Here we show that incorporating the entire measurement time series, which is typically a continuous physical process, into phase retrieval allows the oversampling requirement at each time step to be reduced leading to a subsequent improvement in the temporal resolution by a factor of 2 to 20 times. The increased time resolution will allow imaging of faster dynamics and of radiation dose sensitive samples. This approach, which we call chrono CDI, may find use in improving time resolution in other imaging techniques.
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By using phase retrieval, Bragg Coherent Diffractive Imaging (BCDI) allows tracking of three-dimensional displacement fields inside individual nanocrystals. Nevertheless, in the presence of significant (1% and higher) strains, such as in the process of a structural phase transformation, fails due to the Bragg peak distortions. Here we present an advanced BCDI algorithm enabling imaging three-dimensional strain fields in highly strained crystals. We test the algorithm on particles simulated to undergo a structural phase transformation. While the conventional algorithm fails in unambiguously reconstructing the phase morphology, our algorithm correctly retrieves the morphology of coexistent phases with a strain difference of 1%. The key novelty is the simultaneous reconstruction of multiple scans of the same nanoparticle at snapshots through the phase transformations. The algorithm enables visualizing phase transformations in nanoparticles of lithium-ion, sodium-ion nanoparticles, and other nanoparticulate materials in working conditions (operando).
Nanoscale heterogeneity (including size, shape, strain, and defects) significantly impacts material properties and how they function. Bragg coherent x-ray imaging methods have emerged as a powerful tool to investigate, in three-dimensional detail, the local material response to external stimuli in reactive environments, thereby enabling explorations of the structure-defect-function relationship at the nanoscale. Although progress has been made in understanding this relationship, coherent imaging of extended samples is relatively slow (typically requiring many minutes) due to the experimental constraints required to solve the phase problem. Here, we develop Bragg coherent modulation imaging (BCMI), which uses a modulator to solve the phase problem thereby enabling fast, local imaging of an extended sample. Because a known modulator is essential to the technique, we first demonstrate experimentally that an unknown modulator structure can be recovered by using the exit wave diversity that exists in a standard Bragg coherent diffraction imaging (BCDI) experiment. We then show with simulations that a known modulator constraint is sufficient to solve the phase problem and enable a single view of an extended sample that is sensitive to defects and dislocations. Our results pave the way for BCMI investigations of strain and defect dynamics in complex extended crystals with temporal resolution limited by the exposure time of a single diffraction pattern.
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.
Attosecond science has been transforming our understanding of electron dynamics in atoms, molecules and solids. However, to date almost all of the attoscience experiments have been based on spectroscopic measurements because attosecond pulses have intrinsically very broad spectra due to the uncertainty principle and are incompatible with conventional imaging systems. Here we report an important advance towards achieving attosecond coherent diffractive imaging. Using simulated attosecond pulses, we simultaneously reconstruct the spectrum, 17 probes and 17 spectral images of extended objects from a set of ptychographic diffraction patterns. We further confirm the principle and feasibility of this method by successfully performing a ptychographic coherent diffractive imaging experiment using a light-emitting diode with a broad spectrum. We believe this work clear the way to an unexplored domain of attosecond imaging science, which could have a far-reaching impact across different disciplines.
We present results of a coherent x-ray diffractive imaging experiment performed on a single colloidal crystal grain. The full three-dimensional (3D) reciprocal space map measured by an azimuthal rotational scan contained several orders of Bragg reflections together with the coherent interference signal between them. Applying the iterative phase retrieval approach, the 3D structure of the crystal grain was reconstructed and positions of individual colloidal particles were resolved. As a result, an exact stacking sequence of hexagonal close-packed layers including planar and linear defects were identified.
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