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Engineering of the photonic environment of single nitrogen-vacancy centers in diamond

Daniel Riedel

Published Jan 1, 2017• 2 citations
Publisher

Abstract

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

DOI
10.5451/unibas-006828637

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Deterministic enhancement of coherent photon generation from a nitrogen-vacancy center in ultrapure diamond (Conference Presentation)

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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.

Quantum Photonic Devices•Sep 19, 2017•4 citations

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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.

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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.

International Conference on Transparent Optical Networks•Jun 1, 2011•1 citation
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.
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.
A quantumnetwork would allow the distribution of a quantum state over many spatially separated quantum nodes which individually possess the ability to generate, process and store quantum information. Connecting these nodes through quantum communication channels would enable sending quantum information over arbitrarily long distances, secret key distribution with guaranteed secure communication and distributed quantum computing. An appealing platform for implementation of quantum networks is the nitrogen-vacancy (NV) center in diamond. An NV center is an optically active defect in diamond created by the substitution of two adjacent carbon atoms in the diamond crystal matrix by a nitrogen atom and a neighboring vacancy. The NV center fits remarkably well in the described quantum network framework. Its electronic spin can be optically initialized, read out in a single shot, coherently manipulated and coupled to the nearby carbon-13 nuclear spins. These properties represent necessary ingredients of a multi-qubit quantum node. The possibility of the entanglement between the state of the NV center spin and a photon establishes a photonic quantum link which can enable the entanglement of the quantum nodes, forming a quantum network. First building blocks of the proposed quantum networks based on NV centers were demonstrated by performing entanglement between two distant NV centers separated by more than a kilometer. However, the current success rate of the entangling protocols is greatly reduced due to the low emission probability of the NV center photons into the resonant zero phonon line (ZPL) and the inefficient photon extraction from the diamond. This is the central problem which prevents promoting our experiments beyond proof-of-principle demonstration towards practical implementation of the proposed quantumnetworks. The goal of this thesis is tackling these issues by coupling NV centers to optical cavities which would greatly increase the rate of generation and collection of the ZPL photons through themechanism of Purcell enhancement. The design and the fabrication of the components constituting a diamond-basedFabry-Perot microcavity, as used in this thesis, are described in Chapter 4. For large enhancement of the NV center resonant emission, a low cavity mode volume is necessary. This is achieved by inserting a micrometers thin diamond slab into the cavity architecture; we present the fabrication details of such samples. Chapter 5 describes the fabrication of an integrated platform for microwave signal delivery to the NV centers within a diamond membrane in the cavity architecture. Microwave striplines and arrays of unique markers are embedded in the mirror onto which the diamond is bonded. We investigate the mirror optical properties post fabrication and find that the fabrication method preserves the mirror optical performance. We describe the diamond bonding method and demonstrate addressing of the NV center spin. In Chapter 6 we probe the properties of the cavity with the embedded diamond membrane through measurements of the cavity finesse. We investigate the cavity finesse dependence on length, mode structure and temperature. We further explore the operation at cryogenic temperatures by probing the effect of cryostation vibration on the cavity linewidth. Finally, in Chapter 7 we discuss ways of improving the existing experimental capabilities, outline the first steps for demonstrating enhancement of the NV center resonant emission and suggest future experiments that can be performed with this system. We conclude that coupling of the NV centers to the cavities developed in this research could lead to an increase of remote entanglement success rates by more than three orders of magnitude.
The negatively charged nitrogen vacancy centre in diamond is known for its coherent spin properties and optical interface, and thus is regarded a promising candidate for quantum information applications [1]. Realisation of an efficient spin-photon interface with the NV centre is made challenging however by the fact that, in bulk diamond, only 3-4% of spontaneously emitted photons occur in the zero phonon line (ZPL). Placing NV centre in an optical cavity is being explored by several groups [2][3][4] as an effective way to selectively enhance the coherent emission of NVs and thereby increase the efficiency of the coherent spin-photon coupling. Previous work reported successful coupling of the NV in nano-diamond to an open access micro-cavity and observed enhanced ZPL emission [5]. However the NV centres in nano-diamond suffer from broadened zero phonon transition and poor spin coherence. By fabricating NV centres in a ~micrometre thick membrane of high purity single crystal material we can take advantage of the tunability of open access cavities, and at the same time, provide close-to-bulk crystal environment to maintain the coherent spin properties of the NV centres. Here we report our work on the tunable cavity coupling of the ZPL of a NV centre in a 1.2micrometre-thick diamond membrane at 4K. The diamond membrane is fabricated from a 0.5mm-thick E6 CVD diamond plate where ion implantation is carried out on both surfaces to create NV centres at the depth of around 70nm. The plate is then machined into 30micrometre-thick slices, and thinned by ICP-RIE with a combination of Ar/Cl[6] and pure oxygen plasma etching recipes. The open cavity consists of a concave mirror (99.99% reflectivity) deposited on a template fabricated using Focused Ion Beam (FIB) milling[7] and a planar mirror (99.8% reflectivity) which supports the membrane. For bare cavities with mirror radii of curvature (RoC) of 12micrometre, we measured a finesse of F~2000 and mode volume as small as 0.75micrometre^3. In-situ tuning of the cavity resonance is achieved with piezoelectric actuators. When mounted in our bath cryostat the cavity modes have dominant Lorentzian line profiles which indicate a passive stability of the cavity length of better than 0.15nm. No active locking is currently deployed. With the presence of a diamond membrane inside the cavities, the measured finesse and mode volume of a cavity with 12micrometre RoC are found to be around 300 and 3 micrometre^3, respectively. We attribute the reduction in finesse to scattering at the membrane-air and membrane-mirror interfaces. On coupling to the ZPL of a target NV centre, we record a factor of 4 increase in the saturated intensity of ZPL fluorescence compared to that measured from the same NV centre in absence of the concave mirror. This result is consistent with the calculated Purcell factor of 16 combined with a relatively low efficiency of light extraction (estimated to be around 19%) from the cavity due to the scattering losses.
Nitrogen vacancy centres in diamond have shown strong potential for use as qubits in quantum computing. However, nitrogen vacancy centres have a low percentage of overall emission emitted through the Zero Phonon Line (ZPL). In addition, the fabrication of NV centres with controlled positioning is limited. This thesis presents the ZPL linewidth characterisation of NV centres fabricated using laser writing and laser diffusion. Only one out of the six NV centres characterised showed a <100 MHz average single scan linewidth, which suggests that the laser diffusion process needs to improved. The low ZPL emission can be enhanced by cavity coupling to Fabry-Pérot microcavities. Fabry-Pérot microcavities are susceptible to vibrations, which will decouple the cavity from the NV centre and reduce the photon enhancement. A cavity stabilisation system based on cavity fringe stabilisation is implemented, and the results of the stability are presented. The Fabry-Pérot microcavity can be stabilised with 0.13 nm using fringe stabilisation. High collection efficiency of the emission is also desired for maximising the entanglement rate and is reduced by optical aberrations. For NV centres in bulk diamond, using Solid Immersion Lenses (SILs) removes the spherical aberration that is introduced when collecting NV emission through a planar interface. This thesis presents the results of modelling the aberrations for NV centres cavity coupled to a Fabry-Pérot microcavity and for hemispherical SILs on diamond. The wavefronts of the aberrations introduced by the planar mirror of the microcavity and the aberrations introduced by the positioning error of the SIL are modelled numerically. A deformable mirror is implemented into a confocal microscope to monitor the aberrations of the photonic devices and the results are compared with the numerical model. For Fabry-Pérot microcavities, the intensity loss caused by the aberrations introduced by the planar mirror was predicted to be less than 10 \% due to the thin mirror substrate and low numerical aperture of the cavity mode. This prediction was consistent with the experimental results where an effective 3 \% increase in light collection was observed with aberration correction. For the SILs, the model predicts that the collection efficiency is more sensitive to the lateral positioning of the SIL relative to the NV centre than the axial positioning error.
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.