The primary events of photosynthesis occur on ultrafast timescales with high quantum efficiency. Elucidating the design principles of photosynthetic systems remains an outstanding challenge that has the potential to impact our design of artificial light-harvesting materials. I will discuss our development of a multispectral multidimensional spectrometer (MMDS) enabling measurements spanning the ultraviolet, visible and mid-infrared as well as combination spectroscopies, over timescales of femtoseconds to seconds. I will illustrate some of the capabilities of the MMDS instrument through our efforts to probe the electronic structure and charge separation mechanisms of several light-harvesting systems.