Evolution of Carbon Clusters in the Detonation Products of the Triaminotrinitrobenzene (TATB)-Based Explosive PBX 9502

Abstract

The detonation of carbon-rich high explosives yields solid carbon as a major constituent of the product mixture, and depending on the thermodynamic conditions behind the shock front, a variety of carbon allotropes and morphologies may form and evolve. We applied time-resolved small-angle X-ray scattering (TR-SAXS) to investigate the dynamics of carbon clustering during detonation of PBX 9502, an explosive composed of 1,3,5-triamino-2,4,6-trinitrobenzene (TATB) and 5 wt % fluoropolymer binder. Solid carbon formation was probed from 0.1 to 2.0 μs behind the detonation front and revealed rapid carbon cluster growth which reached a maximum after ∼200 ns. The late-time carbon clusters had a radius of gyration of 3.3 nm which is consistent with 8.4 nm diameter spherical particles and matched particle sizes of recovered products. Simulations using a clustering kinetics model were found to be in good agreement with the experimental measurements of cluster growth when invoking a freeze-out temperature, and temporal shift associated with the initial precipitation of solid carbon. Product densities from reactive flow models were compared to the electron density contrast obtained from TR-SAXS, and used to approximate the carbon cluster composition as a mixture of 20% highly ordered (diamond-like) and 80% disordered carbon forms, which will inform future product equation of state models for solid carbon in PBX 9502 detonation product mixtures.