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Assessment of the associated particle technique with high-resolution gamma-ray spectroscopy for in-field identification of chemical warfare agents and explosives

In this work, high-resolution prompt γ-ray neutron activation analysis (PGNAA) is performed using the associated particle (AP) technique with a deuterium-tritium neutron generator and high-purity germanium detector. Although the time resolution is inferior compared to similar systems employing fast scintillation γ-ray detectors, the strong background suppression combined with the high γ-ray energy resolution provides an important boost in sensitivity to certain key elements, especially relevant to field measurements of complex chemicals encased within thick layers of metal, such as in the case of recovered chemical warfare (CW) munitions. Results for various CW and explosive simulants contained within mock munitions are presented and compared with results obtained from traditional PGNAA measurements without the aid of the AP technique. Significant improvements in identification and discrimination between certain chemicals are achieved with the high energy resolution AP technique.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Detection of Inorganic Salt-Based Homemade Explosives (HME) by Atmospheric Flow Tube–Mass Spectrometry

Using a commercial mass spectrometer interfaced with an atmospheric flow tube (AFT) allowed detection of a variety of inorganic compounds used as oxidizers in homemade explosives at picogram levels. The AFT provides reaction times between 3-5 seconds with flows of 6 L/min, enabling detection levels, after thermal desorption, similar to those previously demonstrated for RDX vapors in the low parts-per-quadrillion range. The thermal desorption of chlorate and perchlorate salts resulted in the production of the corresponding anions which have higher electron affinities than the nitrate reactant ions. A dielectric barrier discharge, used as the ionization source, produced the nitrate reactant ions. In some instances, the molecular salt formed adducts with the nitrate, chlorate, and/or perchlorate anions, giving insight into the original identity of the salt cation. Urea nitrate, guanidine nitrate, and potassium nitrate were also detected as adducts with the nitrate reactant ion. Direct room-temperature vapor detection of urea nitrate and hydrogen peroxide, which have relatively high vapor pressures compared to the other salts in this study, is also demonstrated. Room-temperature vapor detection of chlorate and perchlorate salts is possible by the addition of a dilute acid which converts the salt into a more volatile acidic form. A discussion of the instrumentation, methods used, and the ionization chemistry is provided.

chlorate, perchlorate, nitrate, detection, hydroge↗

Anisotropic Hot Spot Formation at a Grain Boundary in Shock-Compressed TATB High Explosive Crystal

Secondary high explosives (HEs) exhibit rich microstructure that promotes the formation of hot spots responsible for detonation initiation, but the role of microstructural interfaces remains poorly quantified. To this end, we develop extensions for the generalized crystal-cutting method (GCCM) to prepare molecular dynamics (MD) simulation cells containing grain boundaries (GBs) and other crystal–crystal interfaces with prescribed tilt and twist orientations. Using the GCCM, we perform MD simulations of shock interactions with a GB between the (001) and (100) crystal facets in the secondary HE TATB (1,3,5-triamino-2,4,6-trinitrobenzene). Our MD simulations reveal a strong directional dependence to the formation of a hot spot at the GB interface. In particular, transmission of the shock from the (001) grain to the (100) grain yields a hot spot in the (100) grain at the GB interface, whereas no hot spot is produced when an equivalent shock transits the GB in the opposite direction. We trace the origin of this GB anisotropy to three dominant factors: (1) the intrinsic differences in shock-deformation mechanisms and wave structures for the bulk (100) and (001) grains, which leads to distinct geometries and mechanical impedances upon shock arrival to the GB depending on which grains are donor or acceptor for the transmitted shock; (2) the different time intervals separating the initial shock rise and the formation of steady wave structures in the respective donor–acceptor configurations; and (3) the differences in time scales required to re-establish local thermal equilibrium. Interfacial hot spots form when these factors combine to impede development of a steady two-wave structure and instead induce a localized, pseudosingly shocked region that undergoes a higher rate of work production (resulting in a higher temperature) compared to when the steady two-wave structure develops further from the interface. The extensions to the GCCM approach presented here are anticipated to facilitate a wide range of MD studies that focus on understanding the role of crystal–crystal interfaces in molecular materials.

organic↗

Characterization of detonation soot produced during steady and overdriven conditions for three high explosive formulations

The detonation of high explosives (HE) produces a dense fluid of molecular gases and solid carbon. The solid detonation carbon contains various carbon allotropes such as detonation nanodiamonds, onion-like carbon, graphite and amorphous carbon, with the formation of the different forms dependent upon pressure, temperature and the environmental conditions of the detonation. We have collected solid carbon residues from controlled detonations of three HE formulations (Composition B-3, PBX 9501, and PBX 9502). Soot was collected from experiments designed to produce both steady and overdriven conditions, and from detonations in both an ambient (air) atmosphere and in an inert Ar atmosphere. Differences in solid carbon residues were quantified using X-ray photoelectron spectroscopy and carbon isotope measurements. Environmental conditions, HE formulation, and peak pressures influenced the amount of and isotopic composition of the carbon in the soot. Detonations in an Ar atmosphere produced greater amounts of carbon soot with lower δ 13 C values than those in ambient air. Therefore, solid carbon residues continued to evolve after detonation due to excess oxygen in the ambient air detonations. As well, higher peak pressures in overdriven conditions produced less carbon soot with, in general, higher δ 13 C values. Consequently, while overdriven conditions only produced peak pressures for a limited duration, it was enough to influence the composition of the solid carbon residues.

36 MATERIALS SCIENCE↗

Temperature of shocked plastic bonded explosive PBX 9502 measured with spontaneous Stokes/anti-Stokes Raman

Raman spectra and velocimetry of shocked PBX 9502 (plastic bonded explosive composed of 95% triaminotrinitrobenzene (TATB) and 5% 3M Company Kel F-800 polymer binder) are reported with the Stokes/anti-Stokes ratio used to determine temperature after the shock reflects from a lithium fluoride window. Final pressures up to 14.5 GPa were tested, but the pressure induced absorption of TATB caused the Raman signal to decrease exponentially with pressure. The reflected shock temperature could be determined to 7 GPa, with an average increase of 14.9 K/GPa. Suggestions to adapt the technique to permit thermometry at higher temperatures are discussed, as are comparisons to a recently proposed equation of state for PBX 9502.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Reactive flow modeling of the polymer bonded explosive LX-17 double shock experiments

Overdriven double shock experiments provide a measurement of the properties of the reaction product states of the 1-3-5-triamino-2-4-6trinitrobenzene-based explosive LX-17. These experiments used two flyer materials mounted on the end of a projectile to send an initial shock through the LX-17, followed by a second shock of a higher magnitude into the detonation products. The experimental results are compared to 2D reactive flow modeling. A reactive flow model that describes only the kinetics of the LX-17 decomposition fails to accurately reproduce the decay of the first shock or the curvature or strength of the second shock. A new model is proposed in which the carbon condensate produced in the reaction zone is controlled by a kinetic rate. This allows the carbon condensate to be initially out of chemical equilibrium with the product gas. Finally, this new model reproduces the initial detonation peak and decay and matches the curvature of the second shock; however, it still over-predicts the strength of the second shock.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Novel PBX formulations containing thermally-expandable microspheres for on-demand control of explosive behavior

In this work, we present the formulation and analysis of inert Plastic-Bonded eXplosive (PBX)-surrogates loaded with thermally expandable microspheres (TEMs). TEMs consist of a thermoplastic acrylonitrile shell (10-50 µm diameter) encapsulating an inert low boiling hydrocarbon. Upon heating, the TEMs expand as the shell softens while the hydrocarbon gasifies, increasing the internal pressure and expanding the particle by as much as 120 vol%. We hypothesize that TEM expansion within a PBX will introduce tunable changes in local density and porosity, and ultimately the shock sensitivity. This paper focuses on microstructural analysis of surrogate PBX-TEM formulations, both before and after thermally- induced TEM expansion. The formulations were analyzed by scanning electron microscopy (SEM), ultra-small angle neutron scattering (USANS), and X-ray Computed Tomography (x-ray CT) under various thermal conditions. Evidence suggests that TEM expansion within a PBX is a viable method to impart microstructural changes that are predicted to have a measurable, on-demand effect on the initiation sensitivity. Future work includes development of PBX-TEM formulations with HMX and shock initiation experiments.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Kinetics of Carbon Condensation in Detonation of High Explosives: First-Order Phase Transition Theory Perspective

We report the kinetics of carbon condensation, or carbon clustering, in detonation of carbon-rich high explosives is modeled by solving a system of rate equations for concentrations of carbon particles. Unlike previous efforts, the rate equations account not only for the aggregation of particles but also for their fragmentation in a thermodynamically consistent manner. Numerical simulations are performed, yielding the distribution of particle concentrations as a function of time. In addition to that, analytical expressions are obtained for all the distinct steps and regimes of the condensation kinetics, which facilitates the analysis of the numerical results and allows one to study the sensitivity of the kinetic behavior to the variation of system parameters. The latter is important because the numerical values of many parameters are not reliably known at present. The theory of the kinetics of first-order phase transitions is found adequate to describe the general kinetic trends of carbon condensation, as described by the rate equations. Such physical phenomena and processes as the coagulation, nucleation, growth, and Ostwald ripening are observed, and their dependence on various system parameters is studied and reported. It is believed that the present work will become useful when analyzing the present and future results for the kinetics of carbon condensation, obtained from experiments or atomistic simulations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Flash x-ray radiography analysis of detonation wave propagation in additive-manufactured high explosives

Recent research has demonstrated that additive manufacturing (AM) can be used to produce directionally sensitive high explosives (HEs), but detonation wave propagation in AM HEs with variable internal structure has not been studied. In this work, samples were printed using a 73 wt. % octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine-based HE ink. Flash x-ray radiography imaging was used to observe density changes in two imaging planes of each sample during detonation, and high-speed imaging was used to calculate the detonation velocity at the HE surface. The detonation front initially appears to fail in internal channel regions of the HE, but late reactions occurred in two samples, which increased the material bulk density by 2.8%, possibly due to shock convergence phenomena. The calculated detonation wave pressure similarly increased, but the accuracy of the results is uncertain because of the deviation of the low bulk density printed samples from the cast charge principal isentrope. Here, this work demonstrates that structure can be effectively utilized to guide detonation wave propagation through HE charges.

3D printing↗

Validation of a detonation product equation of state for an insensitive high explosive via slab geometry expansion tests

Slab expansion (SLABEX) tests are conducted to validate a process for calibrating the detonation products equation of state (EOS) of a high explosive (HE). The SLABEX tests use rectangular slabs of PBX 9502, a polymer-bonded HE formulation consisting of 95 wt.% 1,3,5-triamino-2,4,6-trinitrobenzene bound with Kel F-800, a co-polymer of chlorotrifluoroethylene and vinylidene-fluoride. Three PBX 9502 slab thicknesses are examined, each confined symmetrically by two rectangular copper (Cu) plates approximately one-tenth the thickness of the HE slab. For the duration of each experiment, the detonation flow along the central axis of the PBX 9502 slab remains two-dimensional. The lateral flow velocity component of the outer surfaces of the expanding Cu plates is measured, along with the steady axial detonation speed along the central axis of the SLABEX. Hydrodynamic simulations of the Cu plate expansion in the SLABEX geometry, driven by the energy stored in the detonation products by the detonation combustion event, are conducted using a Jones–Wilkins–Lee EOS for the detonation products. This EOS form was recently parameterized for PBX 9502 in the cylinder expansion test geometry using a newly developed calibration technique [Voelkel et al., Combust. Flame 246, 112373 (2022)]. Good agreement between the experiment and prediction is found in each SLABEX test, demonstrating that the detonation product EOS calibration technique produces EOSs that are predictive when applied to other geometries.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

Uncertainty quantification for high explosive reactant and product equations of state

Equations of state (EOSs) are typically represented as physics-informed models with tunable parameters that are adjusted to replicate calibration data as closely as possible. Uncertainty quantification (UQ) allows for the development of an ensemble of EOS parameters that are consistent with the calibration data instead of a single EOS. In this work, we perform UQ for the reactant and product EOSs for a variety of high explosives (HEs). In doing so, we demonstrate a strategy for dealing with heterogeneous (both experimental and calculated) data. We also use a statistical distance metric to quantify the differences between the various HEs using the UQ results.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Modification of Richtmyer–Meshkov instabilities via layered explosive charge design

In this numerical study, we investigate the effects of layered high explosive (HE) charge design on Richtmyer–Meshkov instability (RMI) in metal plates with sinusoidal surface features. The detonation wave from the HE induces a shock in the metal target that subsequently interacts with the surface features; this results in vortex formation and ultimately RMI. Here, we seek to modify RMI by altering the detonation wave characteristics. The modification is investigated in a twofold manner: first, by varying the initial design of the unconfined surface of the target and second, by varying the charge design and composition. Within a limited scope of this design space, a wide variety of behaviors related to RMI growth are observed. Mechanistic actions, including exaggerated front curvature, behind these modifications are proposed. Charge designs, which modify RMI the most for a select target design, are then presented.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

Measuring thermal profiles in high explosives using neural networks

We present a new method for calculating the temperature profile of high explosive (HE) material using a Convolutional Neural Network (CNN). To train/test the CNN, we have developed a hybrid experiment/simulation method for collecting acoustic and temperature data. We experimentally heat cylindrical containers of HE material until detonation/deflagration, where we continuously measure the acoustic bursts through the HE using multiple acoustic transducers lined around the exterior container circumference. However, measuring the temperature profile in the HE in an experiment would require inserting a large number of thermal probes, which would disrupt the heating process. Thus, we use two thermal probes, one at the HE center and one at the wall. We then use numerical simulation of the heating process to calculate the temperature distribution and correct the simulated temperatures based on the experimental center and wall temperatures. We calculate temperature errors on the order of 15 °C, which is ∼12% of the range of temperatures in the experiment. We also investigate how the algorithm’s accuracy is affected by the number of acoustic receivers used to collect each measurement and the resolution of the temperature prediction. This work provides a means of assessing the safety status of HE material, which cannot be achieved using existing temperature measurement methods. In addition, it has implications for a range of other applications where internal temperature profile measurements would provide critical information. These applications include detecting chemical reactions, observing thermodynamic processes such as combustion, monitoring metal or plastic casting, determining the energy density in thermal storage capsules, and identifying abnormal battery operations.

97 MATHEMATICS AND COMPUTING↗

Grid resolution requirement of chemical explosive mode analysis for large eddy simulations of premixed turbulent combustion

Full Article Figures & data References Citations Metrics Reprints & Permissions Read this article Abstract The grid resolution requirement for trustworthy Chemical Explosive Mode Analysis (CEMA) in Large Eddy Simulation (LES) of premixed turbulent combustion is proposed. Explicit filtering, to emulate the effect of the LES filter, is applied to one-dimensional laminar flame and three-dimensional planar turbulent flames across a wide range of Karlovitz numbers (5 - 239). The identification of the flame front by CEMA is found relatively insensitive to the cell size (Δ), while the combustion mode identification shows more significant sensitivity. Specifically, increasing Δ falsely enhances the auto-ignition and local extinction modes and suppresses the diffusion-assisted mode. Limited dependence of the CEMA performance on the turbulent combustion regime (Karlovitz number) is observed. A simple grid size criterion for reliable CEMA mode identification in LES is proposed as Δ ≲ δ L /2; The criterion can be relaxed to Δ ≲ δ L in the laminar flame limit. Furthermore, theoretical analysis is conducted on an idealised chemistry-diffusion system. The effects of the filtering process and turbulence on the local combustion mode are demonstrated, which is consistent with the numerical observations. Further, by incorporating turbulent combustion models in CEMA, potential improvement in identifying local combustion modes can be expected.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

New constraints on the Al 25 ( p , γ ) reaction and its influence on the flux of cosmic γ rays from classical nova explosions

The astrophysical 25 Al(p,γ) 26 Si reaction represents one of the key remaining uncertainties in accurately modeling the abundance of radiogenic 26 Al ejected from classical novae. Specifically, the strengths of key proton-unbound resonances in 26 Si, that govern the rate of the 25 Al(p,γ) reaction under explosive astrophysical conditions, remain unsettled. Here, we present a detailed spectroscopy study of the 26 Si mirror nucleus 26 Mg. We have measured the lifetime of the 3 + , 6.125-MeV state in 26 Mg to be 19(3) fs and provide compelling evidence for the existence of a 1 – state in the T = 1, A = 26 system, indicating a previously unaccounted for ℓ = 1 resonance in the 25 Al(p,γ) reaction. Using the presently measured lifetime, together with the assumption that the likely 1 – state corresponds to a resonance in the 25 Al + p system at 435.7(53) keV, we find considerable differences in the 25 Al(p,γ) reaction rate compared to previous works. Furthermore, based on current nova models, we estimate that classical novae may be responsible for up to ≈ 15% of the observed galactic abundance of 26 Al.

20 ≤ A ≤ 38↗

First Proton-Induced Cross Sections on a Stored Rare Ion Beam: Measurement of Te 118 ( p , γ ) for Explosive Nucleosynthesis

We present the first nuclear cross-section measurements of (p,$\gamma$) and (p,n) reactions on 118 Te at energies relevant for the $\gamma$-process nucleosynthesis. Absolute cross-section values for center-of-mass energies of 6, 7 and 10 MeV are provided, together with a theoretical extrapolation to the Gamow window. This experiment marks the first time that direct proton-induced reactions have been measured on a radioactive ion beam at the Experimental Storage Ring (ESR) at GSI, Darmstadt. This paves the way for a large variety of measurements, delivering new constraints for explosive nucleosynthesis and for physics beyond nuclear stability.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Studying of Explosive Electron Emission From “Whisker” Cathode Using X-Ray Point-Projection Radiography

The results of direct observation of the initial phase of explosive electron emission using high-resolution X-ray radiography in X-pinch radiation are reported here. The confirmation of common “Ecton” theory was not found within achieved temporal and spatial resolutions. A mechanism involving the surface breakdown of whiskers that leads to plasma development is proposed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

A Study of Thin Foil Explosion

The explosion of thin flat and cylindrical foils has been studied here on the BIN (270 kA, 100-ns rise time), XP (500 kA, 100-ns rise time), and COBRA (1.0 MA, 100-ns rise time) pulsedpower generators. On all three generators, hybrid and standard 4-wire X-pinches were used to provide soft X-ray radiography with better than 3-μm spatial resolution and 1-ns temporal resolution. This enabled a detailed exploration of the dependence of the exploded structure of the foil on its initial structure and the current density flowing through it. With sufficient current density in the foils, bubbles were observed to form in the center of the foils; the higher the current density, the larger is the bubble diameters.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗