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Mesoscale imperfections, such as pores and voids, can strongly modify the properties and the mechanical response of materials under extreme conditions. Tracking the material response and microstructure evolution during void collapse is crucial for understanding its performance. In particular, imperfections in the ablator materials, such as voids, can limit the efficiency of the fusion reaction and ultimately hinder ignition. To characterize how voids influence the response of materials during dynamic loading and seed hydrodynamic instabilities, we have developed a tailored fabrication procedure for designer targets with voids at specific locations. Our procedure uses SU-8 as a proxy for the ablator materials and hollow silica microspheres as a proxy for voids and pores. By using photolithography to design the targets’ geometry, we demonstrate precise and highly reproducible placement of a single void within the sample, which is key for a detailed understanding of its behavior under shock compression. This fabrication technique will benefit high-repetition rate experiments at x-ray and laser facilities. Insight from shock compression experiments will provide benchmarks for the next generation of microphysics modeling.

Many questions regarding dynamic materials could be answered by using time-resolved ultra-fast imaging techniques to characterize the physical and chemical behavior of materials in extreme conditions and their evolution on the nanosecond scale. In this work, we perform multi-frame phase-contrast imaging (PCI) of micro-voids in low density polymers under laser-driven shock compression. At the Matter in Extreme Conditions (MEC) Instrument at the Linac Coherent Light Source (LCLS), we used a train of four x-ray free electron laser (XFEL) pulses to probe the evolution of the samples. To visualize the void and shock wave interaction, we deployed the Icarus V2 detector to record up to four XFEL pulses, separated by 1-3 nanoseconds. In this work, we image elastic waves interacting with the micro-voids at a pressure of several GPa. Monitoring how the material’s heterogeneities, like micro-voids, dictate its response to a compressive wave is important for benchmarking the performances of inertial confinement fusion energy materials. For the first time in a single sample, we have combined an ultrafast x-ray framing camera and four XFEL pulse train to create an ultrafast movie of micro-void evolution under laser-driven shock compression. Eventually, we hope this technique will resolve the material density as it evolves dynamically under laser shock compression.

Inertial confinement fusion (ICF) holds increasing promise as a potential source of abundant, clean energy, but has been impeded by defects such as micro-voids in the ablator layer of the fuel capsules. It is critical to understand how these micro-voids interact with the laser-driven shock waves that compress the fuel pellet. At the Matter in Extreme Conditions (MEC) instrument at the Linac Coherent Light Source (LCLS), we utilized an x-ray pulse train with ns separation, an x-ray microscope, and an ultrafast x-ray imaging (UXI) detector to image shock wave interactions with micro-voids. To minimize the high- and low-frequency variations of the captured images, we incorporated principal component analysis (PCA) and image alignment for flat-field correction. After applying these techniques we generated phase and attenuation maps from a 2D hydrodynamic radiation code (xRAGE), which were used to simulate XPCI images that we qualitatively compare with experimental images, providing a one-to-one comparison for benchmarking material performance. Moreover, we implement a transport-of-intensity (TIE) based method to obtain the average projected mass density (areal density) of our experimental images, yielding insight into how defect-bearing ablator materials alter microstructural feature evolution, material compression, and shock wave propagation on ICF-relevant time scales.

The response of forsterite, Mg2SiO4, under dynamic compression is of fundamental importance for understanding its phase transformations and high‐pressure behavior. Here, we have carried out an in situ X‐ray diffraction study of laser‐shocked polycrystalline and single‐crystal forsterite (a‐, b‐, and c‐ orientations) from 19 to 122 GPa using the Matter in Extreme Conditions end‐station of the Linac Coherent Light Source. Under laser‐based shock loading, forsterite does not transform to the high‐pressure equilibrium assemblage of MgSiO3 bridgmanite and MgO periclase, as has been suggested previously. Instead, we observe forsterite and forsterite III, a metastable polymorph of Mg2SiO4, coexisting in a mixed‐phase region from 33 to 75 GPa for both polycrystalline and single‐crystal samples. Densities inferred from X‐ray diffraction data are consistent with earlier gas‐gun shock data. At higher stress, the response is sample‐dependent. Polycrystalline samples undergo amorphization above 79 GPa. For [010]‐ and [001]‐oriented crystals, a mixture of crystalline and amorphous material is observed to 108 GPa, whereas the [100]‐oriented forsterite adopts an unknown phase at 122 GPa. The first two sharp diffraction peaks of amorphous Mg2SiO4 show a similar trend with compression as those observed for MgSiO3 in both recent static‐ and laser‐driven shock experiments. Upon release to ambient pressure, all samples retain or revert to forsterite with evidence for amorphous material also present in some cases. This study demonstrates the utility of femtosecond free‐electron laser X‐ray sources for probing the temporal evolution of high‐pressure silicate structures through the nanosecond‐scale events of shock compression and release.

A supervised machine learning algorithm, called locally adaptive discriminant analysis (LADA), has been developed to locate boundaries between identifiable image features that have varying intensities. LADA is an adaptation of image segmentation, which includes techniques that find the positions of image features (classes) using statistical intensity distributions for each class in the image. In order to place a pixel in the proper class, LADA considers the intensity at that pixel and the distribution of intensities in local (nearby) pixels. This paper presents the use of LADA to provide, with statistical uncertainties, the positions and shapes of features within ultrafast images of shock waves. We demonstrate the ability to locate image features including crystals, density changes associated with shock waves, and material jetting caused by shock waves. This algorithm can analyze images that exhibit a wide range of physical phenomena because it does not rely on comparison to a model. LADA enables analysis of images from shock physics with statistical rigor independent of underlying models or simulations., United States. Office of Naval Research (Grant N00014-16-1-2090), United States. Office of Naval Research (Grant N00014-15-1-2694)

Nitromethane (NM), a high explosive (HE) with low sensitivity, is known to undergo photolysis upon ultraviolet (UV) irradiation. The optical transparency, homogeneity, and extensive study of NM make it an ideal system for studying photodissociation mechanisms in conventional HE materials. The photochemical processes involved in the decomposition of NM could be applied to the future design of controllable photoactive HE materials. In this study, the photodecomposition of NM from the nπ* state excited at 266 nm is being investigated on the femtosecond time scale. UV femtosecond transient absorption (TA) spectroscopy and excited state femtosecond stimulated Raman spectroscopy (FSRS) are combined with nonadiabatic excited state molecular dynamics (NA-ESMD) simulations to provide a unified picture of NM photodecomposition. The FSRS spectrum of the photoproduct exhibits peaks in the NO2 region and slightly shifted C-N vibrational peaks pointing to methyl nitrite formation as the dominant photoproduct. A total photolysis quantum yield of 0.27 and an nπ* state lifetime of ∼20 fs were predicted from NA-ESMD simulations. Predicted time scales revealed that NO2 dissociation occurs in 81 ± 4 fs and methyl nitrite formation is much slower having a time scale of 452 ± 9 fs corresponding to the excited state absorption feature with a decay of 480 ± 17 fs observed in the TA spectrum. Although simulations predict C-N bond cleavage as the primary photochemical process, the relative time scales are consistent with isomerization occurring via NO2 dissociation and subsequent rebinding of the methyl radical and nitrogen dioxide.

Pentaerythritol tetranitrate (PETN), a high explosive, initiates with traditional shock and thermal mechanisms. In this study, the tetrazine-substituted derivative of PETN, pentaerythritol trinitrate chlorotetrazine (PetrinTzCl), is being investigated for a photochemical initiation mechanism that could allow control over the chemistry contributing to decomposition leading to initiation. PetrinTzCl exhibits a photochemical quantum yield (QYPC) at 532 nm not evident with PETN. Using static spectroscopic methods, we observe energy absorption on the tetrazine (Tz) ring that results in photodissociation yielding N2, Cl-CN, and Petrin-CN as the major photoproducts. The QYPC was enhanced with increasing irradiation intensity. Experiment and theoretical calculations imply this excitation mechanism follows sequential photon absorption. Dynamic simulations demonstrate that the relaxation mechanism leading to the observed photochemistry in PetrinTzCl is due to vibrational excitation during internal conversion. PetrinTzCl's single photon stability and intensity dependence suggest this material could be stable in ambient lighting, yet possible to initiate with short-pulsed lasers.

We describe the data analysis procedures for an emerging interferometric technique for measuring motion across a two-dimensional image at a moment in time, i.e. a snapshot 2d-VISAR.

We have developed the capability to perform in situ coherent anti-Stokes Raman scattering (CARS) spectroscopy on materials that are dynamically compressed using the Janus laser at Lawrence Livermore National Laboratory. We measured the CARS spectrum of α-quartz that was shocked above the Hugoniot elastic limit along the c-axis to 19.0 GPa. These data show that the Si-O-Si angle, which is natively 144° becomes a distribution of angles ranging from 139° to 146°. The data also observe a significant increase in the broad peak above 600 cm-1 that is attributed to defects in amorphous silica. Previous studies have shown these features in shock recovered α-quartz samples that have undergone varying amounts of amorphization, and these data show strong evidence of amorphization of quartz at a pressure below that of the amorphization observed in the shock-recovered samples.

We report theoretical considerations and preliminary data on various forms of coherent Raman spectroscopy that have been considered as candidates for measurement of temperature in condensed phase experiments with picosecond time resolution. Due to the inherent broadness and congestion of vibrational features in condensed phase solids, particularly at high temperatures and pressures, only approaches that rely on the ratio of anti-Stokes to Stokes spectral features are considered. Methods that rely on resolution of vibrational progressions, calibration of frequency shifts with temperature and pressure in reference experiments, or detailed comparison to calculation are inappropriate or impossible for our applications. In particular, we consider femtosecond stimulated Raman spectroscopy (FSRS), femtosecond/picosecond hybrid coherent Raman spectroscopy (multiplex CARS), and optical heterodyne detected femtosecond Raman induced Kerr Effect spectroscopy (OHD-FRIKES). We show that only FSRS has the ability to measure temperature via an anti-Stokes to Stokes ratio of peaks.

Coherent anti-Stokes Raman spectroscopy (CARS) is reported following shock loading for the liquids phenylacetylene (18 and 13 GPa), cyclohexane (17 GPa), and acrylonitrile (17 GPa). The evolution of the spectra over the first 300 ps was recorded in each case. All spectra show monotonic decay of all peaks with increasing time after shock. No new peaks due to either chemical reaction or pressure shifting of the vibrational frequencies were observable. This loss of signal after shock is attributed to the decreased coherence time in the shock heated liquids, which leads to rapid signal loss in the nonresonant background free version of CARS used in the measurements. These results suggest that more complex methods may be required to measure picosecond shock induced chemistry with coherent Raman techniques that are free of nonresonant background interference.

With an ultrafast framing camera, we image the propagation of a shock wave on the nanosecond time-scale. Four frame x-ray phase-contrast radiographs are acquired using the pulse train from an x-ray free electron laser.