Project description:Pressure- and temperature-induced phase transitions have been studied for more than a century but very little is known about the non-equilibrium processes by which the atoms rearrange. Shock compression generates a nearly instantaneous propagating high-pressure/temperature condition while in situ X-ray diffraction (XRD) probes the time-dependent atomic arrangement. Here we present in situ pump-probe XRD measurements on shock-compressed fused silica, revealing an amorphous to crystalline high-pressure stishovite phase transition. Using the size broadening of the diffraction peaks, the growth of nanocrystalline stishovite grains is resolved on the nanosecond timescale just after shock compression. At applied pressures above 18 GPa the nuclueation of stishovite appears to be kinetically limited to 1.4±0.4 ns. The functional form of this grain growth suggests homogeneous nucleation and attachment as the growth mechanism. These are the first observations of crystalline grain growth in the shock front between low- and high-pressure states via XRD.
Project description:Plasticity is ubiquitous and plays a critical role in material deformation and damage; it inherently involves the atomistic length scale and picosecond time scale. A fundamental understanding of the elastic-plastic deformation transition, in particular, incipient plasticity, has been a grand challenge in high-pressure and high-strain-rate environments, impeded largely by experimental limitations on spatial and temporal resolution. Here, we report femtosecond MeV electron diffraction measurements visualizing the three-dimensional (3D) response of single-crystal aluminum to the ultrafast laser-induced compression. We capture lattice transitioning from a purely elastic to a plastically relaxed state within 5 ps, after reaching an elastic limit of ~25 GPa. Our results allow the direct determination of dislocation nucleation and transport that constitute the underlying defect kinetics of incipient plasticity. Large-scale molecular dynamics simulations show good agreement with the experiment and provide an atomic-level description of the dislocation-mediated plasticity.
Project description:SignificanceCompressed ultrafast photography (CUP) is currently the world's fastest single-shot imaging technique. Through the integration of compressed sensing and streak imaging, CUP can capture a transient event in a single camera exposure with imaging speeds from thousands to trillions of frames per second, at micrometer-level spatial resolutions, and in broad sensing spectral ranges.AimThis tutorial aims to provide a comprehensive review of CUP in its fundamental methods, system implementations, biomedical applications, and prospect.ApproachA step-by-step guideline to CUP's forward model and representative image reconstruction algorithms is presented with sample codes and illustrations in Matlab and Python. Then, CUP's hardware implementation is described with a focus on the representative techniques, advantages, and limitations of the three key components-the spatial encoder, the temporal shearing unit, and the two-dimensional sensor. Furthermore, four representative biomedical applications enabled by CUP are discussed, followed by the prospect of CUP's technical advancement.ConclusionsCUP has emerged as a state-of-the-art ultrafast imaging technology. Its advanced imaging ability and versatility contribute to unprecedented observations and new applications in biomedicine. CUP holds great promise in improving technical specifications and facilitating the investigation of biomedical processes.
Project description:The growth of α-quartz-based piezoelectric thin films opens the door to higher-frequency electromechanical devices than those available through top-down approaches. We report on the growth of SiO2/GeO2 thin films by pulsed laser deposition and their subsequent crystallization. By introducing a devitrifying agent uniformly within the film, we are able to obtain the α-quartz phase in the form of platelets with lateral sizes above 100 μm at accessible temperatures. Films containing different amounts of devitrifying agent are investigated, and their crystallinity is ascertained with X-ray diffraction and electron back-scatter diffraction. Our work highlights the difficulty in crystallization when competing phases arise that have markedly different crystalline orientation.
Project description:Existing streak-camera-based two-dimensional (2D) ultrafast imaging techniques are limited by long acquisition time, the trade-off between spatial and temporal resolutions, and a reduced field of view. They also require additional components, customization, or active illumination. Here we develop compressed ultrafast tomographic imaging (CUTI), which passively records 2D transient events with a standard streak camera. By grafting the concept of computed tomography to the spatiotemporal domain, the operations of temporal shearing and spatiotemporal integration in a streak camera's data acquisition can be equivalently expressed as the spatiotemporal projection of an (x,y,t) datacube from a certain angle. Aided by a new, to the best of our knowledge, compressed-sensing reconstruction algorithm, the 2D transient event can be accurately recovered in a few measurements. CUTI is exhibited as a new imaging mode universally adaptable to most streak cameras. Implemented in an image-converter streak camera, CUTI captures the sequential arrival of two spatially modulated ultrashort ultraviolet laser pulses at 0.5 trillion frames per second. Applied to a rotating-mirror streak camera, CUTI records an amination of fast-bouncing balls at 5,000 frames per second.
Project description:The growth of lamellar crystals has been studied in particular for spherulites in polymeric materials. Even though such spherulitic structures and their growth are of crucial importance for the mechanical and optical properties of the resulting polymeric materials, several issues regarding the residual stress remain unresolved in the wider context of crystal growth. To gain further insight into micro-mechanical forces during the crystallization process of lamellar crystals in polymeric materials, herein, we introduce tetraarylsuccinonitrile (TASN), which generates relatively stable radicals with yellow fluorescence upon homolytic cleavage at the central C-C bond in response to mechanical stress, into crystalline polymers. The obtained crystalline polymers with TASN at the center of the polymer chain allow not only to visualize the stress arising from micro-mechanical forces during polymer crystallization via fluorescence microscopy but also to evaluate the micro-mechanical forces upon growing polymer lamellar crystals by electron paramagnetic resonance, which is able to detect the radicals generated during polymer crystallization.
Project description:Crystallography is the standard for determining the atomic structure of molecules. Unfortunately, many interesting molecules, including an extensive array of biological macromolecules, do not form crystals. While ultrashort and intense X-ray pulses from free-electron lasers are promising for imaging single isolated molecules with the so-called “diffraction before destruction” technique, nanocrystals are still needed for producing sufficient scattering signal for structure retrieval as implemented in serial femtosecond crystallography. Here, we show that a femtosecond laser pulse train may be used to align an ensemble of isolated molecules to a high level transiently, such that the diffraction pattern from the highly aligned molecules resembles that of a single molecule, allowing one to retrieve its atomic structure with a coherent diffraction imaging technique. In our experiment with CO2 molecules, a high degree of alignment is maintained for about 100 fs, and a precisely timed ultrashort relativistic electron beam from a table-top instrument is used to record the diffraction pattern within that duration. The diffraction pattern is further used to reconstruct the distribution of CO2 molecules with atomic resolution. Our results mark a significant step toward imaging noncrystallized molecules with atomic resolution and open opportunities in the study and control of dynamics in the molecular frame that provide information inaccessible with randomly oriented molecules.
Project description:The single-shot compressed ultrafast photography (CUP) camera is the fastest receive-only camera in the world. In this Letter, we introduce an external CCD camera and a space- and intensity-constrained (SIC) reconstruction algorithm to improve the image quality of CUP. The external CCD camera takes a time-unsheared image of the dynamic scene. Unlike the previously used unconstrained algorithm, the proposed algorithm incorporates both spatial and intensity constraints based on the additional prior information provided by the external CCD camera. First, a spatial mask is extracted from the time-unsheared image to define the zone of action. Next, an intensity threshold is determined based on the similarity between the temporally projected image of the reconstructed datacube and the time-unsheared image. Both simulation and experimental studies show that the SIC reconstruction improves the spatial resolution, contrast, and general quality of the reconstructed image.
Project description:Plastic deformation of polycrystalline materials under shock wave loading is a critical characteristic in material science and engineering. However, owing to the nanosecond time scale of the shock-induced deformation process, we currently have a poor mechanistic understanding of the structural changes from atomic scale to mesoscale. Here, we observed the dynamic grain refinement of polycrystalline aluminum foil under laser-driven shock wave loading using time-resolved X-ray diffraction. Diffraction spots on the Debye-Scherrer ring from micrometer-sized aluminum grains appeared and disappeared irregularly, and were shifted and broadened as a result of laser-induced shock wave loading. Behind the front of shock wave, large grains in aluminum foil were deformed, and subsequently exhibited grain rotation and a reduction in size. The width distribution of the diffraction spots broadened because of shock-induced grain refinement and microstrain in each grain. We performed quantitative analysis of the inhomogeneous lattice strain and grain size in the shocked polycrysalline aluminum using the Williamson-Hall method and determined the dislocation density under shock wave loading.
Project description:SiO2 is one of the most fundamental constituents in planetary bodies, being an essential building block of major mineral phases in the crust and mantle of terrestrial planets (1-10 ME). Silica at depths greater than 300 km may be present in the form of the rutile-type, high pressure polymorph stishovite (P42/mnm) and its thermodynamic stability is of great interest for understanding the seismic and dynamic structure of planetary interiors. Previous studies on stishovite via static and dynamic (shock) compression techniques are contradictory and the observed differences in the lattice-level response is still not clearly understood. Here, laser-induced shock compression experiments at the LCLS- and SACLA XFEL light-sources elucidate the high-pressure behavior of stishovite on the lattice-level under in situ conditions on the Hugoniot to pressures above 300 GPa. We find stishovite is still (meta-)stable at these conditions, and does not undergo any phase transitions. This contradicts static experiments showing structural transformations to the CaCl2, α-PbO2 and pyrite-type structures. However, rate-limited kinetic hindrance may explain our observations. These results are important to our understanding into the validity of EOS data from nanosecond experiments for geophysical applications.