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arXiv:1407.1434 · Applied Physics Letters

Highly tunable formation of nitrogen-vacancy centers via ion implantation

Sorawis Sangtawesin, T.O. Brundage, Zachary Atkins, J. R. Petta

Published Aug 11, 2014• 37 citations
arXivHTMLPDF

Abstract

We demonstrate highly tunable formation of nitrogen-vacancy (NV) centers using 20 keV 15N+ ion implantation through arrays of high-resolution apertures fabricated with electron beam lithography. By varying the aperture diameters from 80 to 240 nm, as well as the average ion fluences from 5×1010 to 2 × 1011 ions/cm2, we can control the number of ions per aperture. We analyze the photoluminescence on multiple sites with different implantation parameters and obtain ion-to-NV conversion yields of 6%–7%, consistent across all ion fluences. The implanted NV centers have spin dephasing times T2* ∼ 3 μs, comparable to naturally occurring NV centers in high purity diamond with natural abundance 13C. With this technique, we can deterministically control the population distribution of NV centers in each aperture, allowing for the study of single or coupled NV centers and their integration into photonic structures.

DOI
10.1063/1.4892971

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•Jul 7, 2025•0 citations
We demonstrate highly tunable formation of nitrogen-vacancy (NV) centers using 20 keV 15N+ ion implantation through arrays of high-resolution apertures fabricated with electron beam lithography. By varying the aperture diameters from 80 to 240 nm, as well as the average ion fluences from 5×1010 to 2 × 1011 ions/cm2, we can control the number of ions per aperture. We analyze the photoluminescence on multiple sites with different implantation parameters and obtain ion-to-NV conversion yields of 6%–7%, consistent across all ion fluences. The implanted NV centers have spin dephasing times T2* ∼ 3 μs, comparable to naturally occurring NV centers in high purity diamond with natural abundance 13C. With this technique, we can deterministically control the population distribution of NV centers in each aperture, allowing for the study of single or coupled NV centers and their integration into photonic structures.
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.
The negatively-charged nitrogen-vacancy (NV) center is the most studied optical center in diamond and is very important for applications in quantum information science. Many proposals for integrating NV centers in quantum and sensing applications rely on their tailored fabrication in ultra pure host material. In this study, we use ion implantation to controllably introduce nitrogen into high purity, low nitrogen chemical vapor deposition diamond samples. The properties of the resulting NV centers are studied as a function of implantation temperature, annealing temperature, and implantation fluence. We compare the implanted NV centers with native NV centers present deep in the bulk of the as-grown samples. The results for implanted NV centers are promising but indicate, at this stage, that the deep native NV centers possess overall superior optical properties. In particular, the implanted NV centers obtained after annealing at 2000 °C under a stabilizing pressure of 8 GPa showed an ensemble linewidth of 0.17 nm compared to 0.61 nm after annealing at 1000 °C. Over the same temperature range, the ensemble NV−/NV0 ratio increased by a factor of ∼5, although this was accompanied by an overall decrease in the NV count.
Abstract Nitrogen vacancy (NV) centers in diamond are a platform for several important quantum technologies, including sensing, communication and elementary quantum processors. In this letter we demonstrate the creation of NV centers by implantation using a deterministic single ion source. For this we sympathetically laser-cool single N 2 + 15 molecular ions in a Paul trap and extract them at an energy of 5.9 keV. Subsequently the ions are focused with a lateral resolution of 121(35) nm and are implanted into a diamond substrate without any spatial filtering by apertures or masks. After high-temperature annealing, we detect the NV centers in a confocal microscope and determine a conversion efficiency of about 0.6%. The 15NV centers are characterized by optically detected magnetic resonance on the hyperfine transition and coherence time.
Creating dense and shallow nitrogen-vacancy (NV) ensembles with good spin properties is a prerequisite for developing diamond-based quantum sensors exhibiting better performance. Ion implantation is a key enabling tool for precisely controlling spatial localization and density of NV color centers in diamond. However, it suffers from a low creation yield, while higher ion fluences significantly damage the crystal lattice. In this work, we realize N2+ ion implantation in the 30–40 keV range at high temperatures. At 800 °C, NV's ensemble photoluminescence emission is three to four times higher than room temperature implanted films, while narrow electron spin resonance linewidths of 1.5 MHz, comparable to well-established implantation techniques, are obtained. In addition, we found that ion fluences above 2 × 1014 ions/cm2 can be used without graphitization of the diamond film, in contrast to room temperature implantation. This study opens promising perspectives in optimizing diamond films with implanted NV ensembles that could be integrated into quantum sensing devices.
Creating dense and shallow nitrogen vacancy (NV) ensembles with good spin properties, is a prerequisite for developing diamond-based quantum sensors exhibiting better performance. Ion implantation is a key enabling tool for precisely controlling spatial localisation and density of NV colour centres in diamond. However, it suffers from a low creation yield, while higher ion fluences significantly damage the crystal lattice. In this work, we realize N2 ion implantation in the 30 to 40 keV range at high temperatures. At 800 C, NV ensemble photoluminescence emission is three to four times higher than room temperature implanted films, while narrow electron spin resonance linewidths of 1.5 MHz, comparable to well established implantation techniques are obtained. In addition, we found that ion fluences above 2E14 ions per cm2 can be used without graphitization of the diamond film, in contrast to room temperature implantation. This study opens promising perspectives in optimizing diamond films with implanted NV ensembles that could be integrated into quantum sensing devices.
A nitrogen vacancy (NV) center in diamond is known as a solid-state spin quantum bit (qubit) at room temperature. The fabrication of scalable quantum registers based on NV centers is a long-standing issue. In 2005, spin-spin interaction between NV-N pairs, which were fabricated by N2 ion implantation, was reported. An entanglement between two electron-spin qubits becomes an excellent quantum information processing component, as accomplished by an NV-NV pair with a nanometer-scale distance in 2010 and 2013. More recently,strongly dipolar coupled NV-NV pairs were realized by 14N 30 keV implantationvia nanoholes in PMMA resist mask. The creation yields of NV-NV pairs dramatically improved, and the nanohole implantation had been thought to be the most promising technique to integrate NV centers. However, the problem of the technique is the finite size of nanoholes. The distribution of nitrogen atoms is determined by both ion straggling and nanohole diameter. The scaling of NV centers is stagnant up to two for several years. To overcome the barrier of triple NV centers, our previous research gave a ground-breaking idea of a highly populated NV center complex by introducing a molecular ion implantation technique in 2019. Since the molecular ion is regarded as an idea point source, the distribution of nitrogen atoms is determined by only ion straggling. Therefore, our proposed method is more effective than other implantation techniques including nanohole implantation. Instead of a pure nitrogen cluster which is commonly unstable, the stable organic molecular ions (adenine; C5N5H5) were utilized as the ion source. We successfully implanted C5N4Hn ions into single crystalline diamonds. Three NV centers were integrated, and the dipolar interactions among them were successfully observed. In 2022, we succeeded in creating more than 5 NV centers by phthalocyanine (C32H18N8) ion implantation. The next challenge is the implantation of isotopically enriched molecular ions. The isotopically enriched ion contains 13C and 15N. The implantation of isotopically enriched molecular ions is able to create 15NV-13C hybrid quantum registers. In this presentation, we will show the development of the isotopically enriched molecular ion beam and the characterization of created NV centers by laboratory-built confocal microscopy (CFM) and optically detected magnetic resonance (ODMR).