The nitrogen vacancy center in diamond in its negative charge state is a promising candidate for quantum optic experiments that require single photon emitters. Important benefits of the NV center are its high brightness and photo-stability, even at room temperature. Engineering the emission properties of NV centers with optical resonators is a widely followed approach to meet the requirements for quantum technological applications, but the effect on non-radiative decay paths is yet to be understood. Here we report on modifying the internal quantum efficiency of a single NV center in a nanodiamond coupled to a 1D photonic crystal cavity. We assess the Purcell enhancement via three independent measurement techniques and perform autocorrelation measurements at elevated excitation powers in confocal microscopy. Employing a three-level model allows us to extract the setup efficiency, individual transition rates and thus the internal quantum efficiency of our system. Combining our results, we find that the enhancement of the radiative decay rate via the Purcell effect results in an internal quantum efficiency of 90 % for cavity-coupled NV centers. Our findings will facilitate the realization of nano-scale single photon sources with near-unity internal quantum efficiencies operating at high repetition rates.
The nitrogen vacancy center in diamond in its negative charge state is a promising candidate for quantum optic experiments that require single photon emitters. Important benefits of the NV center are its high brightness and photo-stability, even at room temperature. Engineering the emission properties of NV centers with optical resonators is a widely followed approach to meet the requirements for quantum technological applications, but the effect on non-radiative decay paths is yet to be understood. Here we report on modifying the internal quantum efficiency of a single NV center in a nanodiamond coupled to a 1D photonic crystal cavity. We assess the Purcell enhancement via three independent measurement techniques and perform autocorrelation measurements at elevated excitation powers in confocal microscopy. Employing a three-level model allows us to extract the setup efficiency, individual transition rates and thus the internal quantum efficiency of our system. Combining our results, we find that the enhancement of the radiative decay rate via the Purcell effect results in an internal quantum efficiency of 90 % for cavity-coupled NV centers. Our findings will facilitate the realization of nano-scale single photon sources with near-unity internal quantum efficiencies operating at high repetition rates.
Nitrogen-vacancy (NV) centers in nanodiamond are photostable single photon emitters at room temperature and are considered to be promising candidates for integrated nanophotonics and quantum information processing. A successful implementation of NV centers in nanophotonic devices requires knowledge about the photophysical properties of each emitter such as brightness, decay rate and quantum efficiency. Recent reports show that not all NV centers in diamond nanocrystals are identical and indeed show distributions in brightness and decay rate [1,2]. Here, we report on experimental quantification of the quantum efficiency (QE) of individual nanodiamonds containing single NV centers. Additionally, we report on measurements of decay rate and brightness of single nanodiamond NV centers and discuss if/which NV centers are suitable emitters to be integrated in nanophotonic devices.
Nitrogen–vacancy (NV) centers in diamond are generally recognized as highly promising as indefinitely stable highly efficient single-photon sources. We report an experimental quantification of the brightness, radiative decay rate, nonradiative decay rate and quantum efficiency of single NV centers in diamond nanocrystals. Our experiments show that the commonly observed large spread in fluorescence decay rates of NV centers in nanodiamond is inconsistent with the common explanation of large nanophotonic mode-density variations in the ultra-small high-index crystals at near-unity quantum efficiency. We report that NV centers in 25 nm nanocrystals are essentially insensitive to local density of optical states (LDOS) variations that we induce at a dielectric interface by using liquids to vary the refractive index, and propose that quantum efficiencies in such nanocrystals are widely distributed between 0 and 20%. For single NV centers in larger 100 nm nanocrystals, we show that decay rate changes can be reversibly induced by nanomechanically approaching a mirror to change the LDOS. Using this scanning mirror method, for the first time we report calibrated quantum efficiencies of NV centers, and show that different but nominally identical nanocrystals have widely distributed quantum efficiencies between 10 and 90%. Our measurements imply that nanocrystals that are to be assembled into hybrid photonic structures for cavity QED should first be individually screened to assess fluorescence properties in detail.
The nitrogen vacancy (NV) center is the most widely studied single optical defect in diamond with great potential for applications in quantum technologies. Development of practical single-photon devices requires an understanding of the emission under a range of conditions and environments. In this work, we study the properties of a single NV center in nanodiamonds embedded in an air-like silica aerogel environment which provides a new domain for probing the emission behavior of NV centers in nanoscale environments. In this arrangement, the emission rate is governed primarily by the diamond crystal lattice with negligible contribution from the surrounding environment. This is in contrast to the conventional approach of studying nanodiamonds on a glass coverslip. We observe an increase in the mean lifetime due to the absence of a dielectric interface near the emitting dipoles and a distribution arising from the irregularities in the nanodiamond geometry. Our approach results in the estimation of the mean quantum efficiency (~0.7) of the nanodiamond NV emitters.
Efficient coupling between quantum emitters and optical cavities is essential for scalable quantum photonic technologies. Group-IV vacancy centers in diamond, particularly the negatively charged tin-vacancy center, have emerged as promising candidates due to their spectral stability, high Debye-Waller factor, and large orbital splitting in ground states. Here, we demonstrate controlled coupling of a single negatively charged tin-vacancy center hosted in a nanodiamond to a fully tunable Fabry-Pérot microcavity. At cryogenic temperatures, we access the weak-coupling regime and observe a transition from the bad-emitter regime to the bad-cavity regime as the optical transition of the color center narrows. At 4 K, a Purcell factor exceeding 1.7 is measured, confirming cavity-enhanced emission. The obtained results demonstrate the potential of Sn − V − centers in nanodiamonds as a coherent single-photon source for quantum networks.
The nitrogen-vacancy (NV) center in diamond has an optically addressable, highly coherent spin. However, an NV center even in high quality single-crystalline material is a very poor source of single photons: extraction out of the high-index diamond is inefficient, the emission of coherent photons represents just a few per cent of the total emission, and the decay time is large. In principle, all three problems can be addressed with a resonant microcavity, which significantly boosts the emission rate of coherent photons into the cavity mode based on the Purcell effect. In practice though, it has proved difficult to implement this concept: photonic engineering hinges on nano-fabrication yet it is notoriously difficult to process diamond without degrading the NV centers. \nIn this thesis, we present a microcavity scheme which employs minimally processed diamond membranes, thereby preserving the high quality of the starting material. The miniaturized plano-concave Fabry-Perot microcavity platform features full in situ spatial and spectral tunability. We demonstrate a clear change in the lifetime for multiple individual NV centers on tuning both the cavity frequency and anti-node position. The overall Purcell factor for the zero-phonon line (ZPL) of ~30 translates to an increase in the ZPL emission probability from ~3% to ~46%. \nFurthermore, we report the creation of a low-loss, broadband optical antenna giving highly directed output from a coherent single spin in the solid state. The device, the first crystalline solid-state realization of a dielectric antenna, is engineered for individual NV electronic spins in diamond. The photonic structure preserves the high spin coherence of single-crystalline diamond (T2 ~100µs). We demonstrate a directionality of close to 10 and single photon count rates approaching one MHz. The analysis of the angular emission pattern of our device suggests that 95% of the broadband NV fluorescence is channeled into a solid angle corresponding to a numerical aperture of 0.8. \nThe abovementioned approaches feature complementary benefits. The narrowband enhancement of the ZPL emission rate provided by the microcavity benefits applications in quantum information processing relying on coherent photons. With the prospect of integrating lifetime-limited emitters and achieving a high ZPL collection efficiency our results pave the way for much enhanced spin-photon and spin-spin entanglement rates. On the other hand, by channeling the major fraction of the broadband NV fluorescence into a narrow solid angle the dielectric optical antenna facilitates efficient spin readout. Our approach enables a near-unity collection efficiency which, upon mitigation of the known photon losses, renders it a potential key technology for quantum sensing applications. \n
This thesis investigates the coupling of the fluorescence of nitrogen-vacancy (NV) centers in diamond to tunable optical microresonators at ambient conditions, in particular in the regime of Purcell enhancement. We use fiber-based, open-access Fabry-Pérot cavities optimized for high finesse and ultra-small mode volume. Different regimes of cavity enhancement are studied that are complementary to each other: A first experiment relies on a high-finesse cavity with dielectric mirrors. The scaling laws of Purcell enhancement are explicitly demonstrated by a large-range variation of both the cavity mode volume (V = 16 − 600 µm^3 ) and the quality factor (Q = 6 · 10^3 − 2 · 10^6). We detect an enhancement of the emission spectral density by up to a factor of 300. The full potential of this resonator can be exploited with emitters having a linewidth which is narrower than the resonance linewidth of the cavity. This concept holds promise for the implementation of wavelength-tunable, narrow-band single-photon sources as well as the generation of indistinguishable single-photons at ambient conditions. However, for broad-band emitters like the NV center at room temperature, the emission lifetime is not affected noticeably in this configuration. In order to directly observe lifetime changes and Purcell-enhanced single-photon emission, we manufacture fiber-based cavities with silver-coated mirrors having ultra-small mode volumes, as small as V = 1.0 λ^3 = 0.34 µm^3. We demonstrate cavity-enhanced fluorescence imaging, which allows to locate and analyze several single NV centers with one cavity. The Purcell effect is evidenced by an enhanced fluorescence collection of up to 1.6 · 10^6 photons per second from single-NV centers and a tunable variation of the emission lifetime corresponding to an effective Purcell factor of up to 2. We furthermore investigate a benefcial regime of optical confinement where the Fabry-Pérot cavity mode is combined with additional mode confinement by the diamond nanocrystal itself, enabling sub-λ^3 mode volumes. We perform simulations that predict effective Purcell factors of up to 11 for NV centers and of up to 63 for silicon-vacancy centers, revealing a great potential for bright single-photon sources and effcient spin readout at ambient conditions.