Controlling Plasmonic Catalysis via Strong Coupling\nwith Electromagnetic Resonators

Plasmonic excitations\ndecay within femtoseconds, leaving nonthermal\n(often referred to as “hot”) charge carriers behind\nthat can be injected into molecular structures to trigger chemical\nreactions that are otherwise out of reacha process known as\nplasmonic catalysis. In this Letter, we demonstrate that strong coupling\nbetween resonator structures and plasmonic nanoparticles can be used\nto control the spectral overlap between the plasmonic excitation energy\nand the charge injection energy into nearby molecules. Our atomistic\ndescription couples real-time density-functional theory self-consistently\nto an electromagnetic resonator structure via the radiation-reaction\npotential. Control over the resonator provides then an additional\nknob for nonintrusively enhancing plasmonic catalysis, here more than\n6-fold, and dynamically reacting to deterioration of the catalysta\nnew facet of modern catalysis.