We introduced a new technique, double pulse excitation SOFSRS, to study the role of phonon lattice vibrations in exciton transport in crystalline pentacene and successfully distinguish between driving and spectator modes. By combining selective phonon excitation and ultrafast Raman spectro-microscopy, we track the evolution of excited state species during exciton transport. We compare amplification of each phonon mode with the single pulse dynamics to identify their functional role in exciton transport for the first time. The 91 cm -1 phonon mode drives exciton transport selectively along the slow transport axis. Two phonon modes at 161 cm -1 and 176 cm -1 drive an increase in excited state population, which we can attribute to either an increase in singlet fission or to an increase in the rate of transport. We hope to see integration of selective phonon mode excitation into other ultrafast scattering microscopies to explicitly determine their role in altering exciton diffusion constants. Our work sets the stage for using selective double pulse SOFSRS to answer questions regarding the complex interplay of phonon mode vibrations and exciton transport dynamics, which will inform the design of materials for more efficient photovoltaics.