As the need to develop alternative types of energy has become a more pressing issue, the impetus to understand fundamental energy conversion processes like photosynthesis has only increased. One particular facet of photosynthesis that has been identified as crucial to the conversion of H2O, CO2, and light to O2 and carbohydrates is a proton-coupled electron transfer (PCET) process. Numerous studies have been carried out to gain a broader understanding of PCET processes; however, the traditional tools used to study these reactions have only allowed direct observation of the ET component of PCET. While these are excellent methods for elucidating information about ET, a complete picture involves a study of both the PT and ET components of a PCET process. Our work initially has focused on systems which possess optical handles for both ET and PT, allowing us to gather unique insight into these important reactions. The development of these systems, specifically the probes that can monitor PT reactions, has also allowed us to begin to understand how PT occurs in non-aqueous environments in both the ground state and the electronic excited state.