As electronic and mechanical devices downscale, minor atomic-level surface deviations from ideal configurations can profoundly disrupt material performance and functionality. Achieving precise, atomic level knowledge of surface-mounted single atoms and nanoclusters is essential to understand how their properties change under working conditions and how their electronic structure can be tuned to maximize their performance and durability. However, these systems are messy and often unpredictable. To probe and master the properties of metal nanoclusters on surfaces, we employ sophisticated computational modeling tools.<\/p>\n\n\n\n