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arXiv:2012.05791 · Physical review. B./Physical review. B

Optical detection of paramagnetic defects in diamond grown by chemical vapor deposition

Clément Pellet-Mary, Paul H. Huillery, M. Perdriat, Alexandre Tallaire, Gabriel Hetet

Published Mar 24, 2021• 11 citations
arXivHTMLPDF

Abstract

The electronic spins of the nitrogen-vacancy (NV) centers in chemical-vapor-deposition (CVD) grown diamonds form ideal probes of magnetic fields and temperature, as well as promising qubits for quantum information processing. Studying and controlling the magnetic environment of NV centers in such high-purity crystals is thus essential for these applications. We demonstrate optical detection of paramagnetic species, such as hydrogen-related complexes, in a CVD-grown diamond. The resonant transfer of the NV centers' polarized electronic spins to the electronic spins of these species generates conspicuous features in the NV photoluminescence when employing magnetic field scans along the [100] crystal direction. Our results offer prospects for more detailed studies of CVD-grown processes as well as for coherent control of the spin of novel classes of hyperpolarized paramagnetic species.

DOI
10.1103/physrevb.103.l100411

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The electronic spins of the nitrogen-vacancy (NV) centers in chemical-vapor-deposition (CVD) grown diamonds form ideal probes of magnetic fields and temperature, as well as promising qubits for quantum information processing. Studying and controlling the magnetic environment of NV centers in such high-purity crystals is thus essential for these applications. We demonstrate optical detection of paramagnetic species, such as hydrogen-related complexes, in a CVD-grown diamond. The resonant transfer of the NV centers' polarized electronic spins to the electronic spins of these species generates conspicuous features in the NV photoluminescence when employing magnetic field scans along the [100] crystal direction. Our results offer prospects for more detailed studies of CVD-grown processes as well as for coherent control of the spin of novel classes of hyperpolarized paramagnetic species.
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.
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 are point defects in diamond that allow magnetic field sensing based on Optically Detected Magnetic Resonance (ODMR). They are processed in ultrapure single-domain CVD grown diamond crystals and can be operated at room temperature. This results in solid-state sensors with a wide variety of applications. Ensemble of NV centers can be used to perform wide-field magnetic imaging with sensitivity in the nT range. Single NV centers can also be processed, which allows sensing at the atomic scale. This possibility, combined with its unique coherence properties, make NV center an ideal candidate for quantum sensing.
We report detection and coherent control of a single proton nuclear spin using an electronic spin of the nitrogen-vacancy (NV) center in diamond as a quantum sensor. In addition to determining the NV–proton hyperfine parameters by employing multipulse sequences, we polarize and coherently rotate the single proton spin and detect an induced free precession. Observation of free induction decays is an essential ingredient for high resolution proton nuclear magnetic resonance, and the present work extends it to the atomic scale. We also discuss the origin of the proton as incorporation during chemical vapor deposition growth, which provides an opportunity to use protons in diamond as built-in quantum memories coupled with the NV center.
This thesis reports research conducted on point defects in single crystal diamond utilising the complementary techniques of electron paramagnetic resonance (EPR), optical absorption and photoluminescence (PL) spectroscopy. Intentional silicon-doping of chemical vapour deposition (CVD) diamond allowed the production of samples grown on differently oriented substrates and containing distinct silicon isotopic abundances. The EPR spectrum of the neutral charge state of the silicon split-vacancy centre in diamond, (Si-V)0, has been characterised in the literature. Evidence for the assignment of the 1.31 eV zero phonon line (ZPL) seen in absorption and PL to the 3A2g -> 3A1u transition arising at (Si-V)0 is presented. Reversible charge transfer between the negatively charged centre, (Si-V)− (ZPL at 1.68 eV), and (Si-V)0 enabled the determination of calibration factors relating defect concentrations to their respective ZPL intensities. Preferential alignment of trigonal centres, such as (Si-V), in CVD material grown on {110}-substrates has been observed. The formation of (Si-V) centres during CVD synthesis and via irradiation and annealing of silicon-doped diamond was studied. Variable temperature EPR spectroscopy under illumination was used to investigate the optical spin polarisation (SP) of the (Si-V)0 3A2g ground state. Two different mechanisms for the SP are considered; selective intersystem crossing of (Si-V)0, and photoionisation of (Si-V)−. The properties of (Si-V)0 are compared to those of the extensively studied negatively charged nitrogen vacancy centre, (N-V)−. The effective spin-lattice relaxation and spin polarisation rates for both centres during continuous illumination are explored using pulsed EPR methods. A new defect, labelledWAR3, with spin S = 1 2 was observed in silicon-doped diamond and characterised using multifrequency EPR. Analysis of the data revealed that WAR3 is the neutral charge state of a silicon divacancy complex decorated by a hydrogen atom, (Si-V2:H)0. The experimentally derived 29Si and 1H hyperfine parameters are in good agreement with the values calculated using the spindensity- functional technique, confirming this model and ruling out a non-planar structure.
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.