Defect Polaritons from First Principles.

Control over the optical properties of defects in solid-state materials is necessary for their application in quantum technologies. In this study, we demonstrate, from first principles, how to tune these properties via the formation of defect polaritons in an optical cavity. We show that the polaritonic splitting that shifts the absorption energy of the lower polariton is much higher than can be expected from a Jaynes-Cummings interaction. We also find that the absorption intensity of the lower polariton increases by several orders of magnitude, suggesting a possible route toward overcoming phonon-limited single-photon emission from defect centers. These findings are a result of an effective continuum of electronic transitions near the lowest-lying electronic transition that dramatically enhances the strength of the light-matter interaction. We expect our findings to spur experimental investigations of strong light-matter coupling between defect centers and cavity photons for applications in quantum technologies.