Improved emission of SiV diamond color centers embedded into concave plasmonic core-shell nanoresonators

TL;DR

This paper demonstrates the numerical optimization of concave silver core-shell nanoresonators to significantly enhance the excitation and emission of embedded SiV diamond color centers, achieving up to millions-fold radiative rate enhancements.

Contribution

It introduces a novel optimization approach for nanoresonator design that maximizes simultaneous excitation and emission enhancements of SiV centers with high quantum efficiency.

Findings

Achieved up to 2.03 million-fold Px enhancement.

Optimized nanoresonators reach over 50% quantum efficiency.

Decentralization of emitters reduces enhancement due to multipolar modes.

Abstract

Configuration of three different concave silver core-shell nanoresonators was numerically optimized to enhance the excitation and emission of embedded silicon vacancy (SiV) diamond color centers simultaneously. According to the tradeoff between the radiative rate enhancement and quantum efficiency (QE) conditional optimization was performed to ensure ~2-3-4 and 5-fold apparent cQE enhancement of SiV color centers with ~10% intrinsic QE. The enhancement spectra, as well as the near-field and charge distribution were inspected to uncover the physics underlying behind the optical responses. The conditionally optimized coupled systems were qualified by the product of the radiative rate enhancements at the excitation and emission, which is nominated as Px factor. The optimized spherical core-shell nanoresonator containing a centralized emitter is capable of enhancing considerably the emission via bonding dipolar resonance. The Px factor is 529-fold with 49.7% cQE at the emission. Decentralization of the emitter leads to appearance of higher order multipolar modes, which is not advantageous caused by their nonradiative nature. Transversal and longitudinal dipolar resonances of the optimized ellipsoidal core-shell resonator were tuned to the excitation and emission, respectively. The simultaneous enhancements result in 6.2x10^5 Px factor with 50.6% cQE at the emission. Rod-shaped concave core-shell nanoresonators exploit similarly transversal and longitudinal dipolar resonances, moreover they enhance the fluorescence more significantly due to their antenna-like geometry. Px factor of 8.34x10^5 enhancement is achievable while the cQE is 50.3% at the emission. The enhancement can result in 2.03x10^6-fold Px factor, when the criterion regarding the minimum QE is set to 20%.