Plasmonically Enhanced Superradiance of Broken-Symmetry Diamond Color Center Arrays Inside Core-Shell Nanoresonators

Nanomaterials (Basel). 2022 Jan 22;12(3):352. doi: 10.3390/nano12030352.

Abstract

Superradiance was demonstrated in broken-symmetry arrays of SiV diamond color centers embedded into concave plasmonic nanoresonators. The coupled configurations, including the diamond-silver (bare) and diamond-silver-diamond (coated) nanoresonators' geometry parameters as well as the emitters' azimuthal orientation and distance from the metal, were numerically optimized. An objective function consisting of the total fluorescence enhancement multiplied by the corrected emission quantum efficiency was used to design nanoresonators that promote superradiance. A larger total fluorescence enhancement was achieved via a larger number of emitters in both geometries, in coated spherical and in bare ellipsoidal nanoresonators. The superradiance performance was better in the case of a smaller number of emitters in bare spherical and coated ellipsoidal nanoresonators and in the case of a larger number of emitters in coated spherical and bare ellipsoidal nanoresonators. Ellipsoidal geometry is advantageous independent of composition and seeding. The configurations optimal for non-cooperative fluorescence enhancement and superradiance are coincidental. A radiative rate enhancement proportional to the number of emitters was found in wide spectral regions; therefore, superradiance implies N-fold enhancements coexist at excitation and emission. In ellipsoidal nanoresonators, the better superradiance achieved via a smaller quality-factor is accompanied by larger frequency pulling.

Keywords: broken-symmetry; cooperativity; nanoresonator; plasmonics; superradiance.