Design of Monolithic Microcavities for Enhancing Organic Quantum Emitters

Abstract Single organic molecules are a well-established platform for high-quality single-photon generation: they can emit lifetime-limited photons with high purity and indistinguishability. However, their emission is accompanied by a pronounced red-shifted phonon sideband and higher-order vibrational peaks, which reduce the fraction of photons emitted into the desired narrowband zero-phonon line. The standard approach to suppressing this unwanted emission is to integrate the emitter into a monolithic photonic nanostructure that provides Purcell enhancement. However, incorporating organic materials using clean-room techniques has proven challenging and has, in fact, so far prevented the integration of single molecules in crystalline hosts into monolithic microcavities. As a result, efficient, narrowband organic single-photon sources for applications in quantum information processing have remained elusive despite their considerable promise. Here, we propose three monolithic microcavity designs tailored to provide sufficient Purcell enhancement for organic quantum emitters. The Purcell effect induced by these cavities preferentially enhances emission into the 0–0 zero-phonon line, increasing spectral purity, photon extraction, and shortening the excited-state lifetime, which in turn relaxes the requirements for generating indistinguishable photons. The cavities have been optimized using Bayesian optimization and the adaptive Antoulas–Anderson (AAA) algorithm for rational approximation, which offer global optimization and the efficient reconstruction of spectra from scattering simulations, respectively. These structures are compatible with both standard clean-room processing and single-molecule preparation techniques. Therefore, they offer a clear route to realizing high-quality, practically monochromatic organic single-photon light sources.