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Advanced Materials

Near‐Surface Spectrally Stable Nitrogen Vacancy Centres Engineered in Single Crystal Diamond

Alastair D. Stacey, David Simpson, Timothy J Karle, Brant C. Gibson, Víctor M. Acosta, Zhihong Huang, Kai‐Mei C. Fu, Charles Santori, Raymond G. Beausoleil, Liam Paul McGuinness, Kumaravelu Ganesan, Snjezana Tomljenovic‐Hanic, Andrew D. Greentree, Steven Prawer

Published May 25, 2012• 29 citations
Publisher

Abstract

A method for engineering thin (<100 nm) layers of homoepitaxial diamond containing high quality, spectrally stable, isolated nitrogen-vacancy (NV) centres is reported. The photoluminescence excitation linewidth of the engineered NVs are as low as 140 MHz, at temperatures below 12 K, while the spin properties are at a level suitable for quantum memory and spin register applications. This methodology of NV fabrication is an important step toward scalable and practical diamond based photonic devices suitable for quantum information processing.

DOI
10.1002/adma.201201074

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A method for engineering thin (<100 nm) layers of homoepitaxial diamond containing high quality, spectrally stable, isolated nitrogen-vacancy (NV) centres is reported. The photoluminescence excitation linewidth of the engineered NVs are as low as 140 MHz, at temperatures below 12 K, while the spin properties are at a level suitable for quantum memory and spin register applications. This methodology of NV fabrication is an important step toward scalable and practical diamond based photonic devices suitable for quantum information processing.
We detail the passivation of ultra-high purity diamond and subsequent homoepitaxial growth of thin diamond layers containing spectrally stable nitrogen vacancy (NV) centres. We demonstrate a reduction of three orders of magnitude in the density of fluorescent NV centres in single crystal diamond due to hydrogen plasma treatment. This reduced fluorescence extends to a depth of 80 μm below the diamond surface and provides a clean slate upon which subsequent growth and characterisation of high quality isolated NV centres is possible. The photoluminescence excitation linewidth of NV centres in a 100 nm thick layer are measured to be as low as 140 MHz at T < 12 K, with favourable spin properties. The combination of these two methods is an important step toward scalable and practical diamond based photonic devices suitable for quantum information processing.
The nitrogen-vacancy center (NV) in diamond, with its exceptional spin coherence and convenience in optical spin initialization and readout, is increasingly used both as a quantum sensor and as a building block for quantum networks. Employing photonic structures for maximizing the photon collection efficiency in these applications typically leads to broadened optical linewidths for the emitters, which are commonly created via nitrogen ion implantation. With studies showing that only native nitrogen atoms contribute to optically coherent NVs, a natural conclusion is to either avoid implantation completely or substitute nitrogen implantation by an alternative approach to vacancy creation. Here, we demonstrate that implantation of carbon ions yields a comparable density of NVs as implantation of nitrogen ions and that it results in NV populations with narrow optical linewidths and low charge-noise levels even in thin diamond microstructures. We measure a median NV linewidth of 150 MHz for structures thinner than 5 μm, with no trend of increasing linewidths down to the thinnest measured structure of 1.9 μm. We propose a modified NV creation procedure in which the implantation is carried out after instead of before the diamond fabrication processes and confirm our results in multiple samples implanted with different ion energies and fluences.
The electronic spin associated with the nitrogen vacancy (NV) color center in diamond is an excellent candidate for a solid-state qubit functioning as a quantum register or sensor. However, the lack of thin film technologies for crystalline diamond with low impurity levels hampers the development of photonic interfaces to such diamond-based qubits. We present a method for manufacturing slabs of diamond of 200 nm thickness and several microns in extent from high-purity single crystal chemical vapor deposition diamond. We measure spin coherence times approaching 100 μ s and observe increased photoluminescence collection from shallow implant NV centers in these slabs. We anticipate these slabs to be appealing as quantum memory nodes in hybrid diamond nanophotonic systems.
The nanometer‐scale engineering of single nitrogen‐vacancy (NV) centres in diamond can be obtained by low‐energy (keV) nitrogen implantation with limited straggling. However, shallow NV centres (a few nanometres deep) generally have inferior overall properties than deeply implanted or deep native NV centres, due to the surface proximity. It has already been shown that the spin coherence time of shallow NVs is improved by overgrowth of a thin diamond layer. However the influence of the overgrowth on the survival, the optical properties and the charge state of the centres has not been studied in detail. In this article, we have overgrown three diamond samples (containing NV centres implanted at different depths) using different procedures. We show the successful overgrowth of a pattern of very shallow (2 nm) implanted NV centres using an optimised overgrowth process. Furthermore, the charge state of ensembles and single NV centres was found to be shifted from NV0 to NV− and stabilised in the negative charge state after overgrowth. The combination of low‐energy high‐resolution ion implantation and high‐purity chemical vapour deposition (CVD) overgrowth procedures opens the way towards the fabrication of scalable and efficient quantum devices based on single defects in diamond. Left: implanted pattern of very shallow NV centres (depth ∼2 nm) using a pierced AFM tip. Right: same pattern after CVD overgrowth of a 4 μm‐thick diamond layer.
Scalable realizations of quantum network technologies utilizing the nitrogen vacancy center in diamond require creation of optically coherent NV centers in close proximity to a surface for coupling to optical structures. We create single NV centers by 15^{15}15N ion implantation and high-temperature vacuum annealing. Origin of the NV centers is established by optically detected magnetic resonance spectroscopy for nitrogen isotope identification. Near lifetime-limited optical linewidths (<<< 60 MHz) are observed for the majority of the normal-implant (7∘^\circ∘, ≈\approx≈ 100 nm deep) 15^{15}15NV centers. Long-term stability of the NV−^-− charge state and emission frequency is demonstrated. The effect of NV-surface interaction is investigated by varying the implantation angle for a fixed ion-energy, and thus lattice damage profile. In contrast to the normal implant condition, NVs from an oblique-implant (85∘^\circ∘, ≈\approx≈ 20 nm deep) exhibit substantially reduced optical coherence. Our results imply that the surface is a larger source of perturbation than implantation damage for shallow implanted NVs. This work supports the viability of ion implantation for formation of optically stable NV centers. However, careful surface preparation will be necessary for scalable defect engineering.
Nitrogen-vacancy (NV) centers in single-crystal CVD diamond are promising candidates for quantum sensing due to their remarkable optical and spin properties [1]. These defects exhibit stable photoluminescence (PL), long spin coherence times, and high sensitivity to external fields [2]. In this study, we present a room-temperature PL characterization of NV centers excited with a 532 nm laser. The setup was optimized for high signal-to-noise ratio and spectral resolution. Key parameters analyzed include emission intensity, zero-phonon line (ZPL) at ~637 nm, phonon sidebands, and the charge state distribution between NV⁰ and NV⁻. The NV⁻ state, crucial for spin-based sensing, is evaluated to understand its stability under different nitrogen doping conditions [3]. The relative intensities of NV⁰ and NV⁻ provide insights into nitrogen incorporation and vacancy formation. These results contribute to optimizing synthesis conditions for enhanced NV⁻ concentration, supporting the advancement of diamond-based quantum sensing technologies.