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This work presents a systematic study of the mechanochemical processes leading to chemical reactions occurring due to effects of high-strain-rate deformation associated with uniaxial strain and uniaxial stress impact loading in highly heterogeneous metal powder-based reactive materials, specifically compacted mixtures of Ti/Al/B powders. This system was selected because of the large exothermic heat of reaction in the Ti+2B reaction, which can support the subsequent Al-combustion reaction. The unique deformation state achievable by such high-pressure loading methods can drive chemical reactions, mediated by microstructure-dependent meso-scale phenomena. Design of the next generation of multifunctional energetic structural materials (MESMs) consisting of metal-metal mixtures requires an understanding of the mechanochemical processes leading to chemical reactions under dynamic loading to properly engineer the materials. The highly heterogeneous and hierarchical microstructures inherent in compacted powder mixtures further complicate understanding of the mechanochemical origins of shock-induced reaction events due to the disparate length and time scales involved. A two-pronged approach is taken where impact experiments in both the uniaxial stress (rod-on-anvil Taylor impact experiments) and uniaxial strain (instrumented parallel-plate gas-gun experiments) load configurations are performed in conjunction with highly-resolved microstructure-based simulations replicating the experimental setup. The simulations capture the bulk response of the powder to the loading, and provide a look at the meso-scale deformation features observed under conditions of uniaxial stress or strain. Experiments under uniaxial stress loading reveal an optimal stoichiometry for Ti+2B mixtures containing up to 50% Al by volume, based on a reduced impact velocity threshold required for impact-induced reaction initiation as evidenced by observation of light emission. Uniaxial strain experiments on the Ti+2B binary mixture show possible expanded states in the powder at pressures greater than 6 GPa, consistent with the Ballotechnic hypothesis for shock-induced chemical reactions. Rise-time dispersive signatures are consistently observed under uniaxial strain loading, indicating complex compaction phenomena, which are reproducible by the meso-scale simulations. The simulations show the prevalence of shear banding and particle agglomeration in the uniaxial stress case, providing a possible rationale for the lower observed reaction threshold. Bulk shock response is captured by the uniaxial strain meso-scale simulations and is compared with PVDF stress gauge and VISAR traces to validate the simulation scheme. The simulations also reveal the meso-mechanical origins of the wave dispersion experimentally recorded by PVDF stress gauges.

<p>Raman spectroscopy is a molecular spectroscopy technique that uses monochromatic light to provide a fingerprint to identify structural components and chemical composition. Depending on the changes in the unit-cell parameters and volume under the application of stress and temperature, the Raman spectrum undergoes changes in the wavenumber of Raman-active modes that allow identification of sample characteristics. Due to the various advantage of mechanical Raman spectroscopy (MRS), the use of this technique in the characterization and modeling of chemical changes under stress and temperature have gained popularity. </p> <p> Quantitative information regarding the local behavior of interfaces in an inhomogeneous material during shock loading is limited due to challenges associated with time and spatial resolution. Recently, we have extended the use of MRS to high-strain rate experiments to capture the local thermomechanical response of mock energetic material and obtain material properties during shock wave propagation. This was achieved by developing a novel method for <i>in‑situ</i> measurement of the thermo‑mechanical response from mock energetic materials in a time‑resolved manner with 5 ns resolution providing an estimation on local pressure, temperature, strain rate, and local shock viscosity. The results show the solid to liquid phase transition of sucrose under shock compression. The viscous behavior of the binder was also characterized through measurement of shock viscosity at strain rates higher than 10⁶/s using microsphere impact experiments.</p> <p> This technique was further extended to perform Raman spectral imaging over a microscale domain of the sample with a nano-second resolution. This was achieved by developing a laser-array Raman spectral imaging technique where simultaneous deconvolution of Raman spectra over the sample domain was achieved and Raman spectral image was reconstructed on post-processing. We developed a Raman spectral imaging system using a laser array and analysis was performed over the interface of sucrose crystals bonded using an epoxy binder. This study provides the Raman spectra over the microstructure domain which enabled the detection of localized melting under shock compression. The distribution of shock pressure and temperature over the microstructure was obtained using mechanical Raman analysis. The study shows the effects of an actual interface on the propagation of shock waves where a higher dissipation of shock energy was observed compared to an ideal interface. This increase in shock dissipation is accompanied by a decrease in both the maximum temperature, as well as the maximum pressure within the microstructure during shock wave propagation.</p>

This work focuses on understanding the impact-initiated combustion of aluminum powder compacts. Aluminum is typically one of the components of intermetallic-forming structural energetic materials (SEMs), which have the desirable combination of rapid release of thermal energy and high yield strength. Aluminum powders of various sizes and different levels of mechanical pre-activation are investigated to determine their reactivity under uniaxial stress rod-on-anvil impact conditions, using a 7.62 mm gas gun. The compacts reveal light emission due to combustion upon impact at velocities greater than 170 m/s. Particle size and mechanical pre-activation influence the initiation of aluminum combustion reaction through particle-level processes such as localized friction, strain, and heating, as well as continuum-scale effects controlling the amount of energy required for compaction and deformation of the powder compact during uniaxial stress loading. Compacts composed of larger diameter aluminum particles (~70µm) are more sensitive to impact initiated combustion than those composed of smaller diameter particles. Additionally, mechanical pre-activation by high energy ball milling (HEBM) increases the propensity for reaction initiation. Direct imaging using high-speed framing and IR cameras reveals light emission and temperature rise during the compaction and deformation processes. Correlations of these images to meso-scale CTH simulations reveal that initiation of combustion reactions in aluminum powder compacts is closely tied to mesoscale processes, such as particle-particle interactions, pore collapse, and particle-level deformation. These particle level processes cannot be measured directly because traditional pressure and velocity sensors provide spatially averaged responses. In order to address this issue, quantum dots (QDs) are investigated as possible meso-scale pressure sensors for probing the shock response of heterogeneous materials directly. Impact experiments were conducted on a QD-polymer film using a laser driven flyer setup at the University of Illinois Urbana-Champaign (UIUC). Time-resolved spectroscopy was used to monitor the energy shift and intensity loss as a function of pressure over nanosecond time scales. Shock compression of a QD-PVA film results in an upward shift in energy (or a blueshift in the emission spectra) and a decrease in emission intensity. The magnitude of the shift in energy and the drop in intensity are a function of the shock pressure and can be used to track the particle scale differences in the shock pressure. The encouraging results illustrate the possible use of quantum dots as mesoscale diagnostics to probe the mechanisms involved in the impact initiation of combustion or intermetallic reactions.