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arXiv:1503.05666 · Applied Physics Letters

Nanoimplantation and Purcell enhancement of single nitrogen-vacancy centers in photonic crystal cavities in diamond

Janine Riedrich‐Möller, Sébastien Pezzagna, Jan Meijer, Christoph Pauly, Frank Mücklich, Matthew Markham, Andrew Mark Edmonds, Christoph Becher

Published Jun 1, 2015• 84 citations
arXivHTMLPDF

Abstract

We present the controlled creation of single nitrogen-vacancy (NV) centers via ion implantation at the center of a photonic crystal cavity which is fabricated in an ultrapure, single crystal diamond membrane. High-resolution placement of NV centers is achieved using collimation of a 5 keV-nitrogen ion beam through a pierced tip of an atomic force microscope. We demonstrate coupling of the implanted NV centers' broad band fluorescence to a cavity mode and observe Purcell enhancement of the spontaneous emission. The results are in good agreement with a master equation model for the cavity coupling.

DOI
10.1063/1.4922117

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We present the controlled creation of single nitrogen-vacancy (NV) centers via ion implantation at the center of a photonic crystal cavity which is fabricated in an ultrapure, single crystal diamond membrane. High-resolution placement of NV centers is achieved using collimation of a 5 keV-nitrogen ion beam through a pierced tip of an atomic force microscope. We demonstrate coupling of the implanted NV centers' broad band fluorescence to a cavity mode and observe Purcell enhancement of the spontaneous emission. The results are in good agreement with a master equation model for the cavity coupling.
We demonstrate a self-aligned lithographic technique for precision generation of nitrogen vacancy (NV) centers within photonic nanostructures on bulk diamond substrates. The process relies on a lithographic mask with nanoscale implantation apertures for NV creation, together with larger features for producing waveguides and photonic nanocavities. This mask allows targeted nitrogen ion implantation, and precision dry etching of nanostructures on bulk diamond. We demonstrate high-yield generation of single NVs at pre-determined nanoscale target regions on suspended diamond waveguides. We report implantation into the mode maximum of diamond photonic crystal nanocavities with a single-NV per cavity yield of ∼26% and Purcell induced intensity enhancement of the zero-phonon line. The generation of NV centers aligned with diamond photonic structures marks an important tool for scalable production of optically coupled spin memories.
Towards building large-scale integrated photonic systems for quantum information processing, spatial and spectral alignment of single quantum systems to photonic nanocavities is required. Here, we demonstrate spatially targeted implantation of nitrogen vacancy (NV) centers into the mode maximum of 2-d diamond photonic crystal cavities with quality factors up to 8000, achieving an average of 1:1 0:2 NVs per cavity. Nearly all NV-cavity systems have significant emission intensity enhancement, reaching a cavity-fed spectrally selective intensity enhancement, Fint, of up to 93. Although spatial NV-cavity overlap is nearly guaranteed within about 40 nm, spectral tuning of the NV’s zero-phonon-line (ZPL) is still necessary after fabrication. To demonstrate spectral control, we temperature tune a cavity into an NV ZPL, yielding FZPL int ~ 5 at cryogenic temperatures.
Nitrogen-vacancy (NV) centers feature outstanding properties such as a spin coherence time of up to 1 s as well as a level structure offering the possibility to initialize, coherently manipulate, and optically read-out the spin degree of freedom of the ground state. However, only about 3% of their photon emission is channeled into the zero phonon line (ZPL), limiting both the rate of indistinguishable single photons and the signal-to-noise ratio (SNR) of coherent spin-photon interfaces. We here report on the enhancement of the SNR of the optical spin read-out achieved by tuning the mode of a two-dimensional photonic crystal (PhC) cavity into resonance with the NV-ZPL. PhC cavities are fabricated by focused ion beam milling in thin reactive ion etched ultrapure single crystal diamond membranes featuring modes with Q-factors of up to 8250 at mode volumes below one cubic wavelength. NV centers are produced in the cavities in a controlled fashion by a high resolution atomic force microscope implantation technique. On cavity resonance, we observe a lifetime shortening from 9.0 ns to 8.0 ns as well as an enhancement of the ZPL emission by almost one order of magnitude. Although on resonance the collection efficiency of ZPL photons and the spin-dependent fluorescence contrast are reduced, the SNR of the optical spin read-out is almost tripled for the cavity-coupled NV centers.
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.
Precise control over the spatial distribution and charge state of nitrogen-vacancy (NV) centers in diamond is a key requirement for further advancing this platform in quantum sensing and photonic applications. Here, we investigate nitrogen ion implantation as a scalable method to engineer NV centers in bulk single-crystalline (SC) and a 5 μ m -thick polycrystalline (PC) diamond membrane. Nitrogen-doped regions (1–80 ppm) were fabricated using a 0.7 MeV ion beam and high-temperature annealing, with NV center formation verified by confocal fluorescence imaging and spectral analysis. In SC bulk diamond, we estimate the NV concentration from spectral analysis and model the fluorescence response as a function of implantation dose, capturing both the initial increase at low concentrations and a saturation behavior at higher doses due to quenching mechanisms. In contrast, PC diamond membranes show a weaker dependence at low implantation fluences, consistent with pre-existing nitrogen impurities, thus making a statistical model significantly more complex. The activation yield is found to be of order of 1%, which is lower than in N-rich diamond samples, as implanted N is predominantly interstitial. Photoluminescence spectroscopy indicates that NV 0 is the dominant charge state in both materials, with a laser-power-dependent redistribution between neutral and negative charge states. Optically detected magnetic resonance (ODMR) measurements in SC bulk diamond resolve the hyperfine structure and allow extraction of the dephasing time ( T 2 ∗ ), while in PC diamond membranes, where NV centers tend do form near the grain boundaries, the ODMR signals are observed but spectral resolution is currently limited by impurities, grain-dependent NV orientations, and photoluminescence background.