Abstract: Many chemical reactions utilize organometallic complexes as catalysts. These complexes find use in reactions as varied as bond activation, polymerization, and isomerization. An understanding of the mechanism can be obtained indirectly from many techniques including matrix isolation, reactant modification, and intermediate isolation. A tool that directly monitors the reaction under the conditions of the synthesis is, however, of greater general use in obtaining a detailed picture of the reaction. Ultrafast, UV-pump, IR-probe spectroscopy is such a tool, allowing for experimental monitoring of complex reaction dynamics in the condensed phase. Organometallic complexes are well suited to this type of experiment since many of the ligands have strong infrared absorptions that are highly dependent on the electronic nature of the metal center. Further, organometallic complexes that are ultimately utilized in synthetic applications undergo many fundamental condensed phase processes. It is these fundamental processes and the reactions that ultimately result that are the topic of this thesis. This thesis outlines the construction of a new ultrafast laser system with an emphasis on the generation of tunable mid-infrared pulses, data collection, and data analysis. This system is then used to investigate the formation of vinylidene complexes with group 6 hexacarbonyl complexes. As the first step in polymerization reactions, the formation of vinylidene complexes is of general interest. Our findings indicate that this is a higher energy process than originally thought and that solvation and rearrangement are important steps preceding this chemical event. The rearrangement of alkyne complexes is directly comparable to that of alcohols and silanes. This comparison led to a comprehensive experimental and theoretical investigation of such rearrangements in long chain alcohols. In these studies, we find that inter- and intramolecular descriptions of the rearrangement are not different when the reaction is considered as diffusive motion along a barrier. These labels have been utilized extensively in the past and our findings indicate that this may be inappropriate. As a primary process in reaction dynamics, such a conclusion provides a new context for linkage isomerization reactions. The last project outlined in this thesis is centered on understanding the mechanistic details of boryl mediated carbon-hydrogen bond activation. Transition-metal boryl complexes have shown to be effective catalysts in the selective functionalization of hydrocarbons. Experimental studies which trace the reactive pathways for these complexes provide important insight which can aid in the development of future synthetic schemes. We have investigated the ultrafast reactivity of these complexes in both saturated and unsaturated hydrocarbons and have found multiple photolytically induced reaction channels. Additionally, we have confirmed that the bond activation process is high in energy and must be studied on the nano- to millisecond timescale.