The AMOS program closely couples experimental and theory efforts to provide deep insight into the fundamental interactions that drive key chemical processes in simple molecules, complex molecular systems and molecules in complex environments including interfacial systems. The program’s core strengths are the development of unique experimental and theoretical tools and methods to provide the most detailed and comprehensive insight into correlated electron-electron and coupled electron-nuclear dynamics in atoms and molecules, as well as the flow of energy and charge in atomic, molecular, and interfacial aggregates and assemblies. As such, the program acts as a seed and enabler for next generation theory and experimental tools that provide atomic-scale, real-time access to the chemical transformations of basic energy sciences.