Liquid fragmentation phenomenon is explored from both a fundamental (fully resolved) and an engineering (modeled) perspective. The dual objectives compliment each other by providing an avenue to gain further understanding into fundamental processes of atomization as well as to use the newly acquired knowledge to address practical concerns. A compressible five-equation interface model based on a Roe-type scheme for the simulation of material boundaries between immiscible fluids with arbitrary equation of state is developed and validated. The detailed simulation model accounts for surface-tension, viscous, and body-force effects, in addition to acoustic and convective transport. The material interfaces are considered as diffused zones and a mixture model is given for this transition region. The simulation methodology combines a high-resolution discontinuity capturing method with a low-dissipation central scheme resulting in a hybrid approach for the solution of time- and space-accurate interface problems. Several multi-dimensional test cases are considered over a wide range of physical situations involving capillary, viscosity, and gravity effects with simultaneous presence of large viscosity and density ratios. The model is shown to accurately capture interface dynamics as well as to deal with dynamic appearance and disappearance of material boundaries. Simulation of atomization processes and its interaction with the flow field in practical devices is the secondary objective of this study. Three modeling requirements are identified to perform Large-Eddy Simulation (LES) of spray combustion in engineering devices. In concurrence with these requirements, LES of an experimental liquid-fueled Lean Direct Injection (LDI) combustor is performed using a subgrid mixing and combustion model. This approach has no adjustable parameters and the entire flow-path through the inlet swirl vanes is resolved. The inclusion of the atomization aspects within LES eliminates the need to specify dispersed-phase size-velocity correlations at the inflow boundary. Kelvin-Helmholtz (or aerodynamic) breakup model by Reitz is adopted for the combustor simulation. Two simulations (with and without breakup) are performed and compared with measurements of Cai et al. Time-averaged velocity prediction comparison for both gas- and liquid-phase with available data show reasonable agreement. The major impact of breakup is on the fuel evaporation in the vicinity of the injector. Further downstream, a wide range of drop sizes are recovered by the breakup simulation and produces similar spray quality as in the no-breakup case.