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Perfect preferential orientation of nitrogen-vacancy defects in a synthetic diamond sample

Margarita Lesik, Jean‐Philippe Tetienne, A Tallaire (20076945), J Achard (20076948), V Mille (20076951), A. Gicquel, Jean-François Roch, V. Jacques

Published Nov 2, 2024• 78 citations
OpenAlex

Abstract

We show that the orientation of nitrogen-vacancy (NV) defects in diamond can be efficiently controlled through chemical vapor deposition growth on a (111)-oriented diamond substrate. More precisely, we demonstrate that spontaneously generated NV defects are oriented with a ∼97% probability along the [111] axis, corresponding to the most appealing orientation among the four possible crystallographic axes. Such a nearly perfect preferential orientation is explained by analyzing the diamond growth mechanism on a (111)-oriented substrate and could be extended to other types of defects. This work is a significant step towards the design of optimized diamond samples for quantum information and sensing applications. © 2014 AIP Publishing LLC.

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We show that the orientation of nitrogen-vacancy (NV) defects in diamond can be efficiently controlled through chemical vapor deposition growth on a (111)-oriented diamond substrate. More precisely, we demonstrate that spontaneously generated NV defects are oriented with a ∼97% probability along the [111] axis, corresponding to the most appealing orientation among the four possible crystallographic axes. Such a nearly perfect preferential orientation is explained by analyzing the diamond growth mechanism on a (111)-oriented substrate and could be extended to other types of defects. This work is a significant step towards the design of optimized diamond samples for quantum information and sensing applications. © 2014 AIP Publishing LLC.
We show that the orientation of nitrogen-vacancy (NV) defects in diamond can be efficiently controlled through chemical vapor deposition growth on a (111)-oriented diamond substrate. More precisely, we demonstrate that spontaneously generated NV defects are oriented with a ∼97% probability along the [111] axis, corresponding to the most appealing orientation among the four possible crystallographic axes. Such a nearly perfect preferential orientation is explained by analyzing the diamond growth mechanism on a (111)-oriented substrate and could be extended to other types of defects. This work is a significant step towards the design of optimized diamond samples for quantum information and sensing applications.
The negatively charged nitrogen-vacancy (${\mathrm{NV}}^{\ensuremath{-}}$) center in diamond is an attractive candidate for applications that range from magnetometry to quantum information processing. Here we show that only a fraction of the nitrogen (typically <0.5<0.5<0.5%) incorporated during homoepitaxial diamond growth by chemical vapor deposition (CVD) is in the form of undecorated ${\mathrm{NV}}^{\ensuremath{-}}$ centers. Furthermore, studies on CVD diamond grown on (110)(110)(110)-oriented substrates show a near 100% preferential orientation of NV centers along only the [111][111][111] and [1‾1‾1][\overline{1}\overline{1}1][111] directions, rather than the four possible orientations. The results indicate that NV centers grow in as units, as the diamond is deposited, rather than by migration and association of their components. The NV unit of the ${\mathrm{NVH}}^{\ensuremath{-}}$ is similarly preferentially oriented, but it is not possible to determine whether this defect was formed by H capture at a preferentially aligned NV center or as a complete unit. Reducing the number of NV orientations from four orientations to two orientations should lead to increased optically detected magnetic resonance contrast and thus improved magnetic sensitivity in ensemble-based magnetometry.
Nitrogen-vacancy (NV) centers in diamond have attracted significant interest because of their excellent spin and optical characteristics for quantum information and metrology. To exploit these characteristics, precise control of the orientation of the NV axis in the lattice is essential. Here we show that the orientation of more than 99% of the NV centers can be aligned along the [111] axis by chemical vapor deposition homoepitaxial growth on (111) substrates. We also discuss the alignment mechanisms. Our result enables a fourfold improvement in the magnetic field sensitivity and opens new avenues to the optimum design of NV center devices.
We demonstrate preferential orientation of nitrogen-vacancy (NV) color centers along two of four possible crystallographic axes in diamonds grown by chemical vapor deposition on the 100{100}100 face. We identify the relevant growth regime and present a possible explanation of this effect. We show that preferential orientation provides increased optical readout contrast for NV multispin measurements, including enhanced ac magnetic-field sensitivity, thus providing an important step towards high-fidelity multispin-qubit quantum information processing, sensing, and metrology.
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 centers in diamond have gained widespread attention as quantum systems that can be applied in quantum information devices. The excellent properties of quantum devices can be enhanced using preferentially oriented nitrogen-vacancy (NV) centers. However, thus far, orientation control has been achieved only via chemical vapor deposition. In this study, we demonstrate the creation of preferentially oriented NV centers via laser writing. The alignment ratio of ensemble NV centers is biased along the direction parallel to [111], depending on the femtosecond laser polarization, causing an increase of 55% in contrast to the optically magnetic resonance signal at maximum compared with 25% in random orientation. Based on time-dependent density-functional theory (TDDFT) simulations and experimental observations, such complex polarization dependence can be attributed to the anisotropy of electron excitation. This technique provides a new optical fabrication method for engineered materials and devices used in quantum technology.