The nitrogen-vacancy center in diamond is an attractive resource for the generation of remote entangled states owing to its optically addressable and long-lived electronic spin. However, its low native fraction of coherent photon emission, ~3%, undermines the achievable spin-photon entanglement rates. Here, we couple a nitrogen-vacancy center with a narrow extrinsically-broadened linewidth (159 MHz), hosted in a micron-thin membrane, to an open microcavity. The resulting Purcell factor of ~1.8 increases the zero-phonon line fraction to over 44%. Operation in the Purcell regime, together with an efficient collection of the zero-phonon-line photons, allows resonance fluorescence to be detected for the first time without any temporal filtering. We achieve a >10 signal-to-laser background ratio. This selective enhancement of the center’s zero-phonon transitions could increase spin-spin entanglement success probabilities beyond an order of magnitude compared to state-of-the-art implementations, and enable powerful quantum optics techniques such as wave-packet shaping or all-optical spin manipulation.
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