Resolving Detonation NanoDiamond Size Evolution and Morphology at Sub-Microsecond Time-Scales During High-Explosive Detonations
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.
- Research Organization:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Organization:
- Lawrence Livermore National Laboratory; USDOE National Nuclear Security Administration (NNSA) - Office of Defense Nuclear Nonproliferation; USDOE Office of Science (SC), Basic Energy Sciences (BES); Lawrence Berkeley National Laboratory (LBNL)
- DOE Contract Number:
- AC02-06CH11357
- OSTI ID:
- 1567064
- Journal Information:
- Journal of Physical Chemistry. C, Vol. 123, Issue 31
- Country of Publication:
- United States
- Language:
- English
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