Predicting optically driven excitations is key to tailoring experimental conditions for optimal charge and energy transfer in several energy-centric areas, including ultrafast spectroscopy, photochemistry, molecular electronics, photocatalysis, and surface spectroscopic techniques. Collectively, the four synergistic approaches used in this DOE SciDAC project address far-from-equilibrium phenomena with advanced scientific computing, behavior of properties in electric/magnetic fields, and ultimately controlling chemical/material processes under the influence of driven excitations to predict their long-term dynamics. Finally, the LBNL team members in this project are also directly involved in the architecture exploration path for NERSC10 and beyond, which ensures that this project has direct relevance to upcoming DOE ASCR and exascale initiatives.