An emerging strategy for discovering the next generation of catalysts involves utilizing high-level computational methods to predict and screen structure/function relationships. Effective comparison of theory and experiment requires that the theoretical and experimental models map onto one another perfectly. We use novel synthetic methods, advanced characterization techniques, and density functional theory calculations to approach this ideal. In…

It will be shown that the peculiar electronic and steric properties of cyclic (alkyl)(amino)carbenes (CAACs) (1,2) and other stable singlet carbenes allow for the stabilization of unusual diamagnetic and paramagnetic main group element species. As examples, we will describe the preparation of room temperature stable boron, antimony-, and even carbon-centered neutral and cationic radicals. We will also show that CAACs allow for the isolation of…