All‐atom molecular dynamics (MD) and Eulerian continuum simulations, performed using the LAMMPS and SCIMITAR3D codes, respectively, were used to study thermo‐mechanical aspects of the shock‐induced collapse of an initially cylindrical 50 nm diameter pore in single crystals of 1,3,5‐triamino‐2,4,6‐trinitrobenzene (TATB). Three impact speeds, 0.5 km s−1, 1.0 km s−1 and 2.0 km s−1, were used to generate the shocks. These impact conditions are expected to yield collapse mechanisms ranging from predominantly visco‐plastic to hydrodynamic. For the MD studies, three crystal orientations (relative to shock‐propagation direction) were examined that span the limiting cases with respect to the crystalline anisotropy in TATB. An isotropic constitutive model was used for the continuum simulations, thus crystal anisotropy is absent. The evolution of spatiotemporally resolved quantities during collapse is reported including local pressure, temperature, pore size and shape, and material flow. Multiple models for the melting curve and specific heat were studied. Within the isotropic elastic/perfectly plastic continuum framework and for the range of impact conditions studied, the specific heat and melting curve sub‐models are shown to have modest effects on the continuum hotspot predictions in the present inert calculation. Treating the MD predictions as ‘ground truth’, albeit with a classical rather than quantum‐like heat capacity, it is clear that – at a minimum – an extension of the constitutive model to account for crystal plasticity and anisotropic strength will be required for a high‐fidelity continuum description.

All-atom molecular dynamics (MD) simulations were used to study shock wave loading in oriented single crystals of the highly anisotropic triclinic molecular crystal 1,3,5-triamino-2,4,6-trinitrobenzene (TATB). The crystal structure consists of planar hydrogen-bonded sheets of individually planar TATB molecules that stack into graphitic-like layers. Shocks were studied for seven systematically prepared crystal orientations with limiting cases that correspond to shock propagation exactly perpendicular and exactly parallel to the graphitic-like layers. The simulations were performed for initially defect-free crystals using a reverse-ballistic configuration that generates explicit, supported shocks. Final longitudinal stress components are between ≈8.5 and ≈10.5 GPa for the 1.0 km s–1 impact speed studied. Orientation-dependent properties are reported including shock speeds, stresses, temperatures, compression ratios, and local material strain rates. Spatiotemporal maps of the temperature, stress tensor, material flow, and molecular orientations reveal complicated processes that arise for specific shock directions. The results indicate that TATB shock response is highly sensitive to crystal orientation, with significant qualitative differences for the time evolution of the stress tensor and temperature, elastic/inelastic compression response, defect formation and growth, critical von Mises stress, and strain rates during shock rise that span nearly an order of magnitude. A variety of inelastic deformation mechanisms are identified, ranging from crumpling of graphitic-like layers to dislocation-mediated plasticity to intense shear strain localization. To our knowledge, these are the first systematic MD simulations and analysis of explicit shock wave propagation along nontrivial crystal directions in a triclinic molecular crystal.

Material models for single-crystal β-HMX are systematically examined in the context of continuum pore-collapse simulations. Continuum predictions using five different isotropic material models are compared head-to-head with molecular dynamics (MD) predictions for a 50 nm cylindrical pore in β-HMX subject to a range of shock strengths. Shock waves were generated using a reverse-ballistic configuration, propagating along [010] in the MD simulations. The continuum models are improved hierarchically, drawing on temperature- and pressure-dependent MD-derived material parameters. This procedure reveals the sensitivity of the continuum predictions of pore collapse to the underlying thermophysical models. The study culminates in an MD-calibrated isotropic rate- and temperature-dependent strength model, which includes appropriate submodels for the temperature-dependent melting point of β-HMX [M. P. Kroonblawd and R. A. Austin, Mech. Mater. 152, 103644 (2021)], pressure-dependent shear modulus [A. Pereverzev and T. Sewell, Crystals 10, 1123 (2020)], and temperature-dependent specific heat, that produces continuum pore-collapse results similar to those predicted by MD. The resulting MD-informed model should improve the fidelity of simulations to predict the detonation initiation of HMX-based energetic materials containing micrometer-scale pores.

All-atom molecular dynamics simulations were used to study shock wave loading in oriented single crystals of the highly anisotropic triclinic molecular crystal 1,3,5-triamino-2,4,6-trinitrobenzene (TATB). The crystal structure consists of planar hydrogen-bonded sheets of individually planar TATB molecules that stack into graphitic-like layers. Shocks were studied for seven systematically prepared crystal orientations with limiting cases that correspond to shock propagation exactly perpendicular and exactly parallel to the graphitic-like layers. The simulations were performed for initially defect-free crystals using a reverse-ballistic configuration that generates explicit, supported shocks. Final longitudinal stress components are between »8.5 GPa and »10.5 GPa for the 1.0 km s^-1 impact speed studied. Orientation-dependent properties are reported including shock speeds, stresses, temperatures, compression ratios, and local material strain rates. Spatio-temporal maps of the temperature, stress tensor, material flow, and molecular orientations reveal complicated processes that arise for specific shock directions. The results indicate that TATB shock response is highly sensitive to crystal orientation, with significant qualitative differences for the time evolution of the stress tensor and temperature, elastic/inelastic compression response, defect formation and growth, critical von Mises stress, and strain rates during shock rise that span nearly an order of magnitude. A variety of inelastic deformation mechanisms are identified, ranging from crumpling of graphitic-like layers to dislocation-mediated plasticity to intense shear strain localization. To our knowledge, these are the first systematic MD simulations and analysis of explicit shock wave propagation along non-trivial crystal directions in a triclinic molecular crystal.

We present a machine learning framework to train and validate neural networks to predict the anisotropic elastic response of a monoclinic organic molecular crystal known as β$$ \beta $$‐HMX in the geometrical nonlinear regime. A filtered molecular dynamic (MD) simulations database is used to train neural networks with a Sobolev norm that uses the stress measure and a reference configuration to deduce the elastic stored free energy functional. To improve the accuracy of the elasticity tangent predictions originating from the learned stored free energy, a transfer learning technique is used to introduce additional tangential constraints from the data while necessary conditions (e.g., strong ellipticity, crystallographic symmetry) for the correctness of the model are either introduced as additional physical constraints or incorporated in the validation tests. Assessment of the neural networks is based on (1) the accuracy with which they reproduce the bottom‐line constitutive responses predicted by MD, (2) the robustness of the models measured by detailed examination of their stability and uniqueness, and (3) the admissibility of the predicted responses with respect to mechanics principles in the finite‐deformation regime. We compare the training efficiency of the neural networks under different Sobolev constraints and assess the accuracy and robustness of the models against MD benchmarks for β$$ \beta $$‐HMX.