Single molecule superradiance for optical cycling

TL;DR

This paper demonstrates that single molecules with multiple optical cycling centers can exhibit superradiance, and uses models and design strategies to optimize these properties for laser cooling applications.

Contribution

It introduces the use of the Frenkel exciton model to accurately describe superradiant states in molecules with multiple optical centers and guides molecular design for enhanced superradiance.

Findings

Single molecules with CaO centers show superradiance.

Frenkel exciton model accurately describes superradiant states.

Designed molecules exhibit optimized superradiant properties for laser cooling.

Abstract

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.