With renewed interest in energetic materials like aluminum, many fundamental issues concerning the ignition and combustion characteristics at nanoscales remain to be clarified. Aluminum nanoparticles (Al NP) are widely used solid-state fuels in energetic material applications due to the abundance of aluminum and high heat of reaction. The metallic Al core of Al NP must escape an alumina shell to react with oxidizers. The diffusion oxidation mechanism (DOM) of aluminum has been suggested as governing the reaction mechanism, whereby both oxygen and aluminum diffuse through the oxide shell at low heating rates of 10^4-10^6 K/s. However, Al diffusion through the encapsulating shell restricts the reaction rate between the fuel and surrounding oxide. An alternative model is proposed and known as the melt dispersion mechanism (MDM), a rapid thermomechanical mechanism for rapid heating [greater than] 10^6 K/s. This mechanism is driven by the volumetric expansion of rapidly melting Al core which ruptures the oxide shell. MDM has been widely proposed, and we present the first Al NP spallation observed at a particle scale. Plasmonic photothermal heating was needed to facilitate the rapid heating required to initiate the MDM reaction mechanism. A plasmonic grating coupled with an external laser significantly enhances the intensity of photothermal heating experienced by an Al NP. Aluminum, itself, has strong plasmon resonances throughout the visible and ultraviolet spectrum and may be tuned based on Al NP diameter. Our experimental setup encompasses a wide range of available imaging methods to increase the imaging resolution in a table-top optical microscope. A high-resolution camera with a polarization-based scattering method readily identifies whether a particle is metallic or nonmetallic based on the obtained light intensity. Spatiotemporal temperature dependence of Al NP is also observed using fluorescent dyes embedded in a polymer matrix. Finally, the photothermal heating of Al NP in different systems is modeled in COMSOL Multiphysics software using Electromagnetic Waves and Heat Transfer Modules. Based on the simulation, the estimated heating rate can determine the potential mechanism of the observed mechanism. The findings underline the crucial role of heating rates in observing particle spallation through plasmonic enhanced photothermal heating. Combustion of Al NPs is also studied with fluoropolymer and metal-oxide acting as the oxidizer. The current study aims to establish a unified theory accommodating the reaction mechanisms of aluminum particles at micro and nanoscales. The presented works investigate the material constituents starting from individual particle-scale to macro bulk-scale to understand their reaction mechanism better.