Enzymes are tiny molecular machines that facilitate chemical reactions in all living things. However, some of these reactions are so complex that scientists have yet to recreate them synthetically, especially for enzymes that utilize metals. Understanding how these so-called ‘metalloenzymes’ function is critical for advancements across a broad range of fields from human health and medicine to alternative energy research, and numerous industrial applications. Unfortunately, enzymes are inherently dynamic systems and monitoring their reactions in real-time is technically challenging, so we have little information about what enables their reactivity. We propose to develop and apply a methodology for the simultaneous collection of structural and spectroscopic data that can report on atomic motions and changes to the metal centers as a function of time, thereby enhancing our understanding of these essential machines.