Today’s aerospace industry continues to exploit liquid hydrocarbon fossil fuels. Motivated by operational considerations, continued availability and cost, this is likely to be the case for many years, despite the obvious environmental concerns. The interplay of liquid atomisation, spray vaporisation and the combustion process are intricately linked. However, the physical process of fuel injection and its atomisation into tiny droplets prior to combustion remains poorly understood. Because atomisation governs the size of the fuel droplets, and therefore their subsequent evaporation rate, adjusting the injection sequence is of paramount importance and will have far-reaching repercussions on many aspects of the combustion process, for example pollutant formation. In the context of jet engines, kerosene is usually injected in its liquid form via an airblast-type fuel injector. A coflowing high-speed airstream destabilises the liquid fuel, which is thus sprayed into fine droplets into the combustion chamber. The prediction of this phenomenon for various operating conditions relevant to the aeronautical industry requires a deeper understanding of the mechanisms involved in the interaction of the two fluids. A key element in predicting the complex behaviour of spray formation and evolution in jet engines is accurate modelling of fuel atomisation. Atomisation represents one of the key challenges that remains to be undertaken to make predictive computational simulations possible. However, the inherent multi-physics and multi-scale nature of this process limits numerical investigations. Thanks to the steady progress in computer power and Computational Fluid Dynamics (CFD) methods, computational modelling of injection systems emerges as a promising tool that can drive the design of future devices. This research project sets out to investigate the atomisation process in detail, in particular in providing physical insight into the fundamental physics of the phenomenon, in conjunction with an analysis on wetting behaviours and liquid droplet tracking. High-fidelity numerical simulations are performed using a novel in-house state-of-the-art multiphase flow modelling capability, RCLSFoam. The performance of the numerical scheme is demonstrated on typical two-dimensional and three-dimensional benchmark test cases relevant to both multiphase flow modelling and atomisation, and validated against other computational methods. An informed and systematic qualitative assessment of the topological variations of the phase interface during primary atomisation of a liquid film is made through dynamical analysis, while investigating an extensive domain of operating conditions at ambient and aero-engine injection conditions relevant to industry. This analysis demonstrated the influence of shear-driven instabilities on the atomisation process. The shear stress and difference in inertia between liquid and gas are observed to play a significant role in the atomisation process. In addition, the key physical mechanisms and their competing effects have been mapped out in order to predict the evolution of the process according to the operating conditions of the injection system. The proposed cartography gathers four different atomisation mechanisms. In particular, for sufficiently high liquid injection speeds, three-dimensional wave modes were observed to co-exist (the “3-D wave mode” regime). For very low liquid flow rates, accumulated liquid at the atomising edge undergoes deformation by which droplets are generated (the “accumulation” regime). For an increasing gas injection speed and a fixed liquid velocity, the effects of surface tension were observed to result in the generation of streamwise ligaments only, which tend to pair up (the “ligament-merging” regime). Finally, “vortex action” is another observed mechanism by which the liquid film is fragmented. Overall, this research project culminated in (i) the study of dynamic wetting behaviours, with the implementation and validation against experimental data of the Kistler dynamic contact model; and (ii) the demonstration of an algorithm for droplet capture and subsequent post-processing analysis of the droplet characteristics.