Single molecule superradiance for optical cycling

Herein, we show that single molecules containing multiple optical cycling centers (CaO moieties) can exhibit superradiant phenomena. We demonstrate the accuracy of the Frenkel exciton model at describing these superradiant states via comparisons to high-level electronic structure methods. We then rationally design molecules with superradiant properties optimized for laser cooling. Lastly, we demonstrate how multi-photon superradiant phenomena can occur in these novel molecular systems.