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Production of phosphorus-vacancy centers in diamond for optical and spin characterization

Ben Llewelyn Green, Mark E. Newton, Karl Johnston

Published Jan 10, 2018• 1 citation
OpenAlex

Abstract

The nitrogen-vacancy (NV) point defect center in diamond has recently received significant research interest, with over 850 papers published on the topic in the last 10 years.This interest is a result of optically-pumped spin polarization and optical readout of spin state with high fidelity: potential applications include high-spatial resolution magnetometry, quantum computing and quantum communications.Despite its favorable spin properties, the NV emission is highly broadband leading to low efficiencies for processes which require coherent light interactions e.g.photonic entanglement -a requirement for long distance quantum communication and distributed quantum computing.Further work in diamond has identified group-IV-vacancy pairs (SiV, GeV, SnV) with superlative optical properties (up to 70% coherent emission) but poor spin properties.Therefore, further work is required to identify a point defect which simultaneously possesses long spin lifetimes and narrow optical emission.We propose a route to the production of the previously-unidentified phosphorusvacancy (PV) via implantation of 31 Al (decays to 31 Si with 98.4% efficiency and t 1⁄ 2 = 644 ms), and its optical identification through monitoring the decay of 31 SiV to 31 PV with t 1⁄ 2 = 157 min, and the rise of PV by photoluminescence.PV will subsequently be studied using both ensemble and single-centercapable state-of-the-art characterization equipment to determine its optical and spin properties, which we expect to be extremely interesting in line with SiV, GeV, SnV and NV in diamond.Requested shifts: 6 shifts, (split into 2 runs over 1 years)

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The nitrogen-vacancy (NV) point defect center in diamond has recently received significant research interest, with over 850 papers published on the topic in the last 10 years.This interest is a result of optically-pumped spin polarization and optical readout of spin state with high fidelity: potential applications include high-spatial resolution magnetometry, quantum computing and quantum communications.Despite its favorable spin properties, the NV emission is highly broadband leading to low efficiencies for processes which require coherent light interactions e.g.photonic entanglement -a requirement for long distance quantum communication and distributed quantum computing.Further work in diamond has identified group-IV-vacancy pairs (SiV, GeV, SnV) with superlative optical properties (up to 70% coherent emission) but poor spin properties.Therefore, further work is required to identify a point defect which simultaneously possesses long spin lifetimes and narrow optical emission.We propose a route to the production of the previously-unidentified phosphorusvacancy (PV) via implantation of 31 Al (decays to 31 Si with 98.4% efficiency and t 1⁄ 2 = 644 ms), and its optical identification through monitoring the decay of 31 SiV to 31 PV with t 1⁄ 2 = 157 min, and the rise of PV by photoluminescence.PV will subsequently be studied using both ensemble and single-centercapable state-of-the-art characterization equipment to determine its optical and spin properties, which we expect to be extremely interesting in line with SiV, GeV, SnV and NV in diamond.Requested shifts: 6 shifts, (split into 2 runs over 1 years)
Abstract The nitrogen-vacancy (NV) center in diamond is a promising quantum system for magnetometry applications exhibiting optical readout of minute energy shifts in its spin sub-levels. Key material requirements for NV ensembles are a high NV − concentration, a long spin coherence time and a stable charge state. However, these are interdependent and can be difficult to optimize during diamond growth and subsequent NV creation. In this work, we systematically investigate the NV center formation and properties in bulk chemical vapor deposition (CVD) diamond. The nitrogen flow during growth is varied by over four orders of magnitude, resulting in a broad range of single substitutional nitrogen concentrations of 0.2–20 parts per million. For a fixed nitrogen concentration, we optimize electron-irradiation fluences with two different accelerated electron energies, and we study defect formation via optical characterizations. We discuss a general approach to determine the optimal irradiation conditions, for which an enhanced NV concentration and an optimum of NV charge states can both be satisfied. We achieve spin–spin coherence times T 2 ranging from 45.5 to 549 μ s for CVD diamonds containing 168 to 1 parts per billion NV − centers, respectively. This study shows a pathway to engineer properties of NV-doped CVD diamonds for improved sensitivity.
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.
We demonstrate optical spin polarization of the neutrally charged silicon-vacancy defect in diamond (SiV^{0}), an S=1 defect which emits with a zero-phonon line at 946 nm. The spin polarization is found to be most efficient under resonant excitation, but nonzero at below-resonant energies. We measure an ensemble spin coherence time T_{2}>100 μs at low-temperature, and a spin relaxation limit of T_{1}>25 s. Optical spin-state initialization around 946 nm allows independent initialization of SiV^{0} and NV^{-} within the same optically addressed volume, and SiV^{0} emits within the telecoms down-conversion band to 1550 nm: when combined with its high Debye-Waller factor, our initial results suggest that SiV^{0} is a promising candidate for a long-range quantum communication technology.
The nitrogen-vacancy (NV) center is a point defect in diamond and has been championed as a promising solid-state "artificial atom." NV center properties such as its bright luminescence, room-temperature optical readout of spin states, and long spin decoherence lifetime make it an excellent system for applications in quantum information processing, high sensitivity magnetometry, and biotagging. In all applications, near-surface NVs are desirable. However, it has been found that the favorable properties of the NV center are significantly diminished as the NV center nears the surface. \nThis dissertation presents efforts in understanding the effect of the surface on the luminescence of NV centers less than a wavelength of light from the surface. We use plasma assisted etching to, independently, change the surface termination and bring the NV closer to the surface. We find that treating the surface with CF4 plasma results in a deposited polymerous fluorocarbon which helps stabilize nearby NVs. We propose using a downstream etcher to bring NVs closer to the surface, while minimizing damage and maintaining NV luminescence. Finally, we enhance emission of these near-surface NVs by coupling them into a hybrid diamond plasmonic cavity. The fabricated devices result in a measured Q of 170, higher than other previously fabricated diamond plasmonic devices.
The silicon-vacancy (SiV) and nitrogen-vacancy (NV) centers in diamond are commonly regarded as prototypical defects for solid-state quantum information processing. Here, we show that when silicon and nitrogen are simultaneously introduced into the diamond lattice, these defects can strongly interact and form larger complexes. Nitrogen atoms strongly bind to Si and SiV centers, and complex formation can occur. Using a combination of hybrid density functional theory and group theory, we analyze the electronic structure and provide various useful physical properties, such as hyperfine structure, quasilocal vibrational modes, and a zero-phonon line, to enable experimental identification of these complexes. We demonstrate that the presence of substitutional silicon adjacent to nitrogen significantly shifts the donor level toward the conduction band, resulting in an activation energy for the SiN center that is comparable to phosphorus. We also find that the neutral SiNV center is of particular interest due to its photon emission at $\ensuremath{\sim}1530\phantom{\rule{0.28em}{0ex}}\mathrm{nm}$, which falls within the CCC band of telecom wavelengths and its paramagnetic nature. In addition, the optical transition associated with the SiNV0{\mathrm{SiNV}}^{0}SiNV0 color center exhibits very small electron-phonon coupling (Huang-Rhys factor = 0.78) resulting in high quantum efficiency (Debye-Waller factor = 46%) for single-photon emission. These features render this new center very attractive for a potential application in scalable quantum telecommunication networks.
Point defects in semiconductors are becoming central to quantum technologies. They can be used as spin qubits interfacing with photons, which are fundamental for building quantum networks. Currently, the most prominent quantum defect in diamond is the nitrogen-vacancy (NV) center. However, it suffers from spectral diffusion that negatively impacts optical coherence and is due to the coupling of the emission energy with uncontrolled electric fields. The group IV vacancy complexes on the other hand have shown to be significantly more spectrally-stable as they are centrosymmetric and thus immune to the linear Stark shift. They however suffer from several issues ranging from low operation temperature to low optical efficiency due to dark states and difficulty in stabilizing the right defect charge state. Here we search for alternative to the group IV vacancy complex in diamond by systematically evaluating all possible vacancy complex using high-throughput first-principles computational screening. We identify the defects that combine centrosymmetry, emission in the visible range, as well as favorable and achievable electronic structure promoting higher operation temperature and defect levels well within the band gap. We find ZnV−2V^{-2}V−2 to be especially appealing.