We present both theoretical and experimental results on fluorescence of single defect centers in diamond nanocrystals embedded in a planar dielectric microcavity. From a theoretical point of view, we show that the overall fluorescence collection efficiency using moderate numerical aperture microscope objective can be enhanced by using a low quality factor microcavity. This could be used in particular for low temperature applications where the numerical aperture of collection microscope objectives is limited due to the experimental constraints. We experimentally investigate the control of the fluorescence spectrum of the emitted light from a single center. We show the simultaneous narrowing of the room temperature broadband emission spectrum and the increase of the fluorescence spectral density.
We present both theoretical and experimental results on fluorescence of single defect centers in diamond nanocrystals embedded in a planar dielectric microcavity. From a theoretical point of view, we show that the overall fluorescence collection efficiency using moderate numerical aperture microscope objective can be enhanced by using a low quality factor microcavity. This could be used in particular for low temperature applications where the numerical aperture of collection microscope objectives is limited due to the experimental constraints. We experimentally investigate the control of the fluorescence spectrum of the emitted light from a single center. We show the simultaneous narrowing of the room temperature broadband emission spectrum and the increase of the fluorescence spectral density.
Single negatively charged nitrogen-vacancy (NV-) defect centres in diamond are attractive systems for the implementation of solid state quantum information processing (QIP) and quantum key distribution (QKD). In both approaches, the coupling of an individual NV-centre to a resonant microcavity is of interest: it would improve the optical readout of the NV-centre electron spin state in QIP and enhance the collection efficiency of the single photon fluorescence in QKD while increasing the coherence length of the emission. We theoretically demonstrate that, at room temperature, the coupling to a single-mode Fabry-Perot microcavity can be used to obtain a fluorescence spectrum narrowing without loss of total intensity. We also experimentally demonstrate the control of the fluorescence spectrum of a single NV-centre by adjusting the thickness of the microcavity. Finally, we report a doubling of the emission spectral density with respect to the single mirror configuration.
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.
We report experimental studies of microsphere-enhanced fluorescence collection of nitrogen vacancy (NV) centers using silica microspheres with diameters ranging between 15 and 50 μm and employing 20× and 40× objectives with numerical aperture of 0.42 and 0.64, respectively. Photoluminescence-excitation saturation counts as high as 95 kHz have been observed. These studies show that due to the effective collimation of fluorescence by the microsphere, objectives with relatively low numerical aperture (NA) can be used without sacrificing collection enhancement, in agreement with a theoretical model based on Mie scattering. The large enhancement of fluorescence collection with relatively low NA objectives, which feature extralong working distance and are relatively inexpensive, can potentially enable wider use of NV-based quantum sensing in real world applications.
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
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.
Color centers in diamond, among them the negatively charged germanium vacancy (GeV−), are promising candidates for many applications of quantum optics, such as a quantum network. For efficient implementation, the optical transitions need to be coupled to a single optical mode. Here, we demonstrate the transfer of a nanodiamond containing a single ingrown GeV− center with excellent optical properties to an open Fabry–Pérot microcavity by nanomanipulation utilizing an atomic force microscope. Coupling of the GeV− defect to the cavity mode is achieved, while the optical resonator maintains a high finesse of F=7700, and a 48-fold spectral density enhancement is observed. This article demonstrates the integration of a GeV− defect with a Fabry–Pérot microcavity under ambient conditions with the potential to extend the experiments to cryogenic temperatures toward an efficient spin-photon platform.