Ultra-intense laser (> 10 18 W/cm 2 ) interactions with matter are capable of producing relativistic electrons which have a variety of applications in state-of-the-art scientific and medical research conducted at universities and national laboratories across the world. Control of various aspects of these hot-electron distributions is highly desired to optimize a particular outcome. Hot-electron generation in low-contrast interactions, where significant amounts of under-dense pre-plasma are present, can be plagued by highly non-linear relativistic laser-plasma instabilities and quasi-static magnetic field generation, often resulting in less than desirable and predictable electron source characteristics. High-contrast interactions offer more controlled interactions but often at the cost of overall lower coupling and increased sensitivity to initial target conditions. An experiment studying the differences in hot-electron generation between high and low-contrast pulse interactions with solid density targets was performed on the Titan laser platform at the Jupiter Laser Facility at Lawrence Livermore National Laboratory in Livermore, CA. To date, these hot-electrons generated in the laboratory are not directly observable at the source of the interaction. Instead, indirect studies are performed using state-of-the-art simulations, constrained by the various experimental measurements. These measurements, more-often-than-not, rely on secondary processes generated by the transport of these electrons through the solid density materials which can susceptible to a variety instabilities and target material/geometry effects. Although often neglected in these types of studies, the specularly reflected light can provide invaluable insight as it is directly influenced by the interaction.In this thesis, I address the use of (personally obtained) experimental specular reflectivity measurements to indirectly study hot-electron generation in the context of high-contrast, ii relativistic laser-plasma interactions. Spatial, temporal and spectral properties of the incident and specular pulses, both near and far away from the interaction region where experimental measurements are obtained, are used to benchmark simulations designed to infer dominant hot-electron acceleration mechanisms and their corresponding energy/angular distributions. To handle this highly coupled interaction, I employed particle-in-cell modeling using a wide variety of algorithms (verified to be numerically stable and consistent with analytic expressions) and physical models (validated by experimental results) to reasonably model the interaction's sweeping range of plasma densities, temporal and spatial scales, G. E. Kemp, et al, Experimental and LSP modeling of pre-pulse effects on the laser-plasma interaction by a 527 nm laser pulse,