The objective of this research is to develop an understanding of how molecular motions can be used to control photoinduced chemical processes. The research aims to determine what interplay of nuclear coordinates is most efficient in driving photoinduced charge transfers, a necessary first step in most photovoltaic and photocatalytic devices. Systems such as molecular crystals or polycrystalline films are promising for solar energy conversion, but the role that specific molecular structural features play in driving charge transfer is currently unknown. To determine the mechanism of processes such as ultrafast charge transfer, singlet fission, and long-range transport, a structurally sensitive technique with high time resolution is needed to monitor molecular structures along the reactive multidimensional potential energy surfaces. This work will utilize femtosecond stimulated Raman microscopy to track the nuclear dynamics driving charge transfer and to probe the effects of localized environments on long-range charge transport. By following the structural evolution of photoreactive molecular solids on the timescale of their nuclear motion, this work will provide multidimensional reaction coordinates and uncover molecular structure-function relationships. This fundamental knowledge should ultimately guide rational design of highly efficient photovoltaic and photocatalytic systems by determining how, when, and where energy is lost during charge generation and transport.