Two-dimensional infrared and ultrafast visible pump-infrared probe spectroscopy are used to examine charge transfer and carrier mobility in organic photovoltaic materials by probing their native vibrational modes. Mixtures of electron donating polymers and electron accepting fullerenes that represent prototypical organic solar cells are examined. By studying the carbonyl (C=O) stretch of both electron donor and acceptor materials, we directly time resolve charge transfer on the few picosecond and circa one nanosecond time scales. The slower time scale results from excitons that must diffuse to the interface before charge transfer can occur. The carbonyl frequency is sensitive to the local bonding environment. The sensitivity allows us to time resolve the diffusion of electrons and holes within the materials over a range of time scales covering picoseconds to nanoseconds. The experiments provide sensitive probes of carrier dynamics that are useful for designing the next generation of efficient organic photovoltaic materials.