Sub-us Aggregation During Detonation Synthesis of Nanodiamond
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Engineering topics
Publications and source records attributed to Lauderbach, Lisa M..
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In this work, we explore the structural evolution of highly oriented pyrolytic graphite (HOPG) under detonation-induced shock conditions using in situ synchrotron x-ray diffraction in the ns timescale. We observe the formation of hexagonal diamond (lonsdaleite) at pressures above 50 GPa, in qualitative agreement with recent gas gun experiments. First-principles density functional calculations reveal that under uniaxial compression, the energy barrier for the transition toward hexagonal diamond is lower than that for cubic diamond. Finally, no indication of cubic diamond formation was observed up to >70 GPa.
Carbon particulates generated during detonation depend upon high explosive type, composition, and detonation conditions. Although explosive composition greatly affects particulates, the focus of this work is on how detonation geometries that induce much higher temperatures and pressures in the high explosive lead to differing particulate morphologies. In this study, two geometries were used: Detonations were initiated in Composition B cylinders at one end in conventional detonations and initiated at both ends to produce colliding detonations. Each of these detonations was observed on the sub-μs timescale using fast radiography capturing images of the front moving through the cylinder, and colliding detonation fronts in real-time. These imaging experiments were complemented with time-resolved small-angle x-ray scattering (SAXS) experiments that were able to observe and determine the varying condensed carbon morphologies at different locations and times in each detonation. The detonations could be timed in such a way that the spatial and temporal dependence of the carbon morphology could be superimposed onto radiography images collected at the same point in time. The complementary approach is able to show that the carbon condensates are much larger when formed in the elevated temperature and pressure conditions near the location of colliding detonation fronts. Thermochemical modeling suggests that these larger particulates form either in the diamond phase or on the liquidus line of the carbon phase diagram. The increase in size observed by SAXS may correlate well with the increased residence time deeply in the diamond phase. Finally, these particulates can be described as nano-sized phases with some surface texture or otherwise near-surface intra-particle heterogeneity.
Characterization of the initial morphology of detonation nanodiamond (DND) has been the focus of many research studies that aim to develop fundamental understanding of carbon condensation under extreme conditions. Identifying the pathways of DND formation has the potential for significant impact in many of the controlled synthesis of nanoscale carbon with tailored functionality; currently, a wide range of possible (and conflicting) mechanisms of nucleation and growth have been proposed and further research is essential. Building a comprehensive understanding of DND formation is challenging because it requires in situ characterization on the sub-µs time-scale during a high explosive detonation. In this study, time resolved small angle X-ray scattering (TR-SAXS) is used to reveal the early-stage DND morphology from < 0.1 μs to 6 μs after the detonation front passes through the X-ray beam path. We address the ambiguity of models previously reported for analysis of small angle scattering from DND by comparing (i) in situ, TR-SAXS recorded during early-stage particulate formation and (ii) ex situ SAXS and transmission electron microscopy measurements (TEM) of products recovered from detonation of the same high-explosive within a carefully designed ice chamber. The SAXS from both late-time ( > 1 μs) in situ and recovered DND exhibit consistent features in the I(q) curve. Such close similarity allows a high fidelity SAXS model derived from the ex situ SAXS and TEM measurements to be applied to the in situ data, which yields new insight into the early stage (< 1µs) morphology of DND. Our analysis indicates a size-distribution of DND particles is observed within 0.1 μs post-detonation and have a mean core diameter slightly below 4 nm and surface texture that consists of hemispherical protrusions that extend ~ 1 nm from the surface. Beyond ~ 0.3 μs, the size distribution increases slightly, while the surface texture persists for several microseconds after the detonation. Combined with thermochemical simulations, these results indicate that during detonation of Composition B, carbon is condensed into nanoscale diamond much faster than previously reported in other studies. Furthermore, the surface texture of the DND is shown to arise during condensation rather than via subsequent graphitization.
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27 psi has been determined to be the maximum allowable pressure for contact operations with PETN at LLNL. Pressures above this limit can be tested, but samples must be prepared via remote handling operations. This document summarizes the safety review and discussion that took place at LLNL to define this pressure limit.