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ACS Nano

Room-Temperature Picosecond Single-Photon Emission from a Silicon Vacancy Center in Diamond

Hengming Li, Deniz Acil, Andrew M. Boyce, Nicholas Yama, Christian Pederson, Srivatsa Chakravarthi, Kai‐Mei C. Fu, Maiken H. Mikkelsen

Published May 15, 2025• 11 citations
Publisher

Abstract

Artificially tailoring quantum emitters by coupling them to optical cavities is critical for applications such as all-photonic quantum computing and quantum key distribution. Among quantum emitters, diamond defect centers, with their atomic-like characteristics, have drawn intense interest for quantum applications. However, the spontaneous emission lifetime of single photons from diamond defects has been limited to several hundred picoseconds, partly due to challenges in realizing cavities in diamond with sufficiently small mode volumes. Here, we sandwich an only 10 nm diamond membrane with implanted negatively charged silicon vacancy centers (SiV – ) between a gold mirror and arrays of nanodisks, resulting in ultrafast single-photon sources with lifetimes as short as 5.5 ps. This corresponds to an improvement in the radiative spontaneous emission rate of over 700-fold, also termed the Purcell factor, and is the result of a greatly enhanced local density of states in the ultrasmall mode-volume cavities. Furthermore, the cavity-coupled single SiV – centers exhibit a 4800-fold photoluminescence enhancement with a single-photon generation rate of up to 361 Mcps at room temperature. These results could refine the engineering of diamond defect centers and position other solid-state platforms as strong quantum-information contenders when coupled to ultrasmall mode-volume cavities, thus illustrating the potential for large-scale, artificially tailored single-photon sources.

DOI
10.1021/acsnano.5c02273

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Artificially tailoring quantum emitters by coupling them to optical cavities is critical for applications such as all-photonic quantum computing and quantum key distribution. Among quantum emitters, diamond defect centers, with their atomic-like characteristics, have drawn intense interest for quantum applications. However, the spontaneous emission lifetime of single photons from diamond defects has been limited to several hundred picoseconds, partly due to challenges in realizing cavities in diamond with sufficiently small mode volumes. Here, we sandwich an only 10 nm diamond membrane with implanted negatively charged silicon vacancy centers (SiV – ) between a gold mirror and arrays of nanodisks, resulting in ultrafast single-photon sources with lifetimes as short as 5.5 ps. This corresponds to an improvement in the radiative spontaneous emission rate of over 700-fold, also termed the Purcell factor, and is the result of a greatly enhanced local density of states in the ultrasmall mode-volume cavities. Furthermore, the cavity-coupled single SiV – centers exhibit a 4800-fold photoluminescence enhancement with a single-photon generation rate of up to 361 Mcps at room temperature. These results could refine the engineering of diamond defect centers and position other solid-state platforms as strong quantum-information contenders when coupled to ultrasmall mode-volume cavities, thus illustrating the potential for large-scale, artificially tailored single-photon sources.
Quantum emitters are an integral component for a broad range of quantum technologies, including quantum communication, quantum repeaters, and linear optical quantum computation. Solid-state color centers are promising candidates for scalable quantum optics due to their long coherence time and small inhomogeneous broadening. However, once excited, color centers often decay through phonon-assisted processes, limiting the efficiency of single-photon generation and photon-mediated entanglement generation. Herein, we demonstrate strong enhancement of spontaneous emission rate of a single silicon-vacancy center in diamond embedded within a monolithic optical cavity, reaching a regime in which the excited-state lifetime is dominated by spontaneous emission into the cavity mode. We observe 10-fold lifetime reduction and 42-fold enhancement in emission intensity when the cavity is tuned into resonance with the optical transition of a single silicon-vacancy center, corresponding to 90% of the excited-state energy decay occurring through spontaneous emission into the cavity mode. We also demonstrate the largest coupling strength (g/2π = 4.9 ± 0.3 GHz) and cooperativity (C = 1.4) to date for color-center-based cavity quantum electrodynamics systems, bringing the system closer to the strong coupling regime.
Quantum communication places stringent requirements on single-photon sources. Here we report a theoretical study of the cavity Purcell enhancement of two diamond point defects, the nickel-nitrogen (NE8) and silicon-vacancy (SiV) centers, for high-performance, near on-demand single-photon generation. By coupling the centers strongly to high-finesse optical photonic-band-gap cavities with modest quality factor Q=O(104)Q=O({10}^{4})Q=O(104) and small mode volume $V=O({\ensuremath{\lambda}}^{3})$, these system can deliver picosecond single-photon pulses at their zero-phonon lines with probabilities of 0.954 (NE8) and 0.812 (SiV) under a realistic optical excitation scheme. The undesirable blinking effect due to transitions via metastable states can also be suppressed with $O({10}^{\ensuremath{-}4})$ blinking probability. We analyze the application of these enhanced centers, including the previously studied cavity-enhanced nitrogen-vacancy (NV) center, to long-distance Bennett-Brassard 1984 protocol quantum key distribution (QKD) in fiber-based, open-air terrestrial and satellite-ground setups. In this comparative study, we show that they can deliver performance comparable with decoy state implementation with weak coherent sources, and are most suitable for open-air communication.
Silicon-vacancy (SiV) color centers in diamond offer novel possibilities to probe light-matter interaction in nano-quantum optics and provide a scalable quantum system suitable for single-photon emission. However, their effective count-rate is still limited by non-radiative decay channels, radiation at wide angles and total internal reflection at the diamond interface. Recently optical antennas have been utilized in order to modify light-matter interaction at the nanoscale. Acting as resonators, they are able to increase the spontaneous emission rate of quantum emitters by several orders of magnitude in a broad spectral range. Because coupling a quantum emitter to a nano-antenna requires close proximity between the two systems, we implant Si ions on very thin diamond membranes that provide the required dimension for near-field interaction in a controlled manner and investigate the optical properties of SiV color centers in such diamond membranes. We consider gold nano-cones as nano-antennas, fabricated by focused electron beam induced deposition (EBID), followed by sputtering and focused ion beam (FIB) milling. The finite-difference time-domain (FDTD) calculations show that gold nano-cones can provide more than four orders of magnitude enhancement in the Purcell factor with an antenna efficiency (AE) of 80%.
Solid-state quantum emitters such as the N-VVV center in diamond have applications ranging from single-photon sources to quantum sensors, with some quantum properties preserved even under ambient conditions. A central challenge is to access these quantum properties efficiently, by catching as much emitted light as possible. In this study a tunable optical microcavity, with a mode volume as small as one wavelength cubed, is used to enhance spontaneous emission of single N-VVV centers in diamond, via the Purcell effect. This allows the authors to extract large amounts of light from several individually addressable emitters, and to control their spontaneous-emission rate.
A key requirement for many applications in solid-state quantum sciences is a high fluence of indistinguishable photons. The spontaneous emission of these photons is governed by the coupling of an excited quantum system to electromagnetic vacuum fluctuations. In our experiment, we enhance this coupling by engineering a tunable Fabry-Perot microcavity. The quantum system we study is the nitrogen-vacancy (NV) center in diamond, a workhorse for quantum science and engineering, due to its optical transitions and the coherent electron spin system it hosts. Our device consists of a high-quality, nano-fabricated, single-crystalline diamond membrane bonded to a planar mirror; the cavity is completed by a second, concave mirror. Using piezo positioners, we achieve full spectral and spatial tunability and freedom in selecting NVs with favorable emission properties in our low-temperature (4 Kelvin) experiments. Upon tuning of the cavity into resonance, we find significant enhancement of the 637 nm zero phonon line for several individual NVs which is accompanied by a strong reduction of the overall photoluminescence (PL) lifetime. We infer a 30-fold enhancement of the zero-phonon transition rate at best. The fraction of the PL emission associated to this resonant transition is thereby increased from 3% to 46%. Our results constitute a significant leap on the route towards the implementation of fast long-distance quantum networks, which are currently limited by the photon emission rate in their nodes. Furthermore, our versatile design is readily applicable to other solid-state quantum emitters like color centers in silicon carbide.
Deterministic coupling of single solid-state emitters to nanocavities is the key for integrated quantum information devices. We here fabricate a photonic crystal cavity around a preselected single silicon-vacancy color center in diamond and demonstrate modification of the emitters internal population dynamics and radiative quantum efficiency. The controlled, room-temperature cavity coupling gives rise to a resonant Purcell enhancement of the zero-phonon transition by a factor of 19, coming along with a 2.5-fold reduction of the emitter's lifetime.