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arXiv:2006.07761 · Applied Physics Letters

Detection and control of single proton spins in a thin layer of diamond grown by chemical vapor deposition

Kento Sasaki, Hideyuki Watanabe, Hitoshi Sumiya, Kohei M. Itoh, Eisuke Abe

Published Sep 14, 2020• 11 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1063/5.0016196

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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.
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 nitrogen-vacancy (NV) center in diamond is a promising candidate for development of quantum communication and simulation devices which are based on the control of coupled quantum systems. It offers an optical readout of its spin state, exhibits long coherence times and allows to coherently control nearby nuclear spins, e.g. from 13C nuclei, even at room-temperature. For successful demonstration of such systems however, controlling the nuclear spin environment, and thus tuning the coupling strengths is crucial to allow the fabrication of a scalable platforms. The combination of Chemical Vapor Deposition (CVD) of diamond as a method with isotopic control on the diamond composition and ion implantation as a tool to reliably create NV centers is a perfect toolkit to study the realization such quantum systems.
We report the formation of perfectly aligned, high-density, shallow nitrogen vacancy (NV) centers on the (111) surface of a diamond. The study involved step-flow growth with a high flux of nitrogen during chemical vapor deposition (CVD) growth, which resulted in the formation of a highly concentrated (>1019 cm−3) nitrogen layer approximately 10 nm away from the substrate surface. Photon counts obtained from the NV centers indicated the presence of 6.1 × 1015–3.1 × 1016 cm−3 NV centers, which suggested the formation of an ensemble of NV centers. The optically detected magnetic resonance (ODMR) spectrum confirmed perfect alignment (more than 99%) for all the samples fabricated by step-flow growth via CVD. Perfectly aligned shallow ensemble NV centers indicated a high Rabi contrast of approximately 30% which is comparable to the values reported for a single NV center. Nanoscale nuclear magnetic resonance demonstrated surface-sensitive nuclear spin detection and provided a confirmation of the NV centers' depth. Single NV center approximation indicated that the depth of the NV centers was approximately 9–10.7 nm from the surface with error of less than ±0.8 nm. Thus, a route for material control of shallow NV centers has been developed by step-flow growth using a CVD system. Our finding pioneers on the atomic level control of NV center alignment for large area quantum magnetometry.
Abstract A nitrogen-vacancy (NV) center in a diamond enables the access to an electron spin, which is expected to present highly sensitive quantum sensors. Although exploiting a nitrogen nuclear spin improves the sensitivity, manipulating it using a resonant pulse requires a long gate time owing to its small gyromagnetic ratio. Another technique to control nuclear spins is a conditional rotation gate based on dynamical decoupling, which is faster but unavailable for nitrogen spins owing to the lack of transverse hyperfine coupling with the electron spin. In this study, we generated effective transverse coupling by applying a weak off-axis magnetic field. An effective coupling depends on the off-axis field; the conditional rotation gate on the nitrogen-14 spins of an NV center was demonstrated within 4.2 μs under an 1.8% off-axis field and a longitudinal field of approximately 280 mT. We estimated that a population transfer from the electron to nitrogen spins can be implemented with 8.7 μs. Our method is applicable to an ensemble of NV centers, in addition to a single NV center.
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 chemical-vapor-deposition (CVD) diamond can form preferentially oriented ensembles with high sensing performance and low densities of lattice defects. Thin films of this material are a cornerstone of various imaging modalities. However, nitrogen injection needed to produce such films can transiently drive growth out of equilibrium, generating interfacial strain and spin defects that degrade NV coherence. Here, we investigate this disorder in 12C^{12}\text{C}12C-enriched, preferentially oriented NV layers grown on (111) diamond using two nitrogen-injection procedures, combined with nanometer-scale selective plasma etching and NV spin-coherence measurements. Pulsed nitrogen injection produces a pronounced nitrogen overshoot within a 60--80 nm interfacial region, generating excessive amounts of defects. By contrast, smooth nitrogen delivery through mass flow controllers substantially suppresses interfacial disorder, yielding coherence properties close to the theoretical limit imposed by spin-bath noise. A 50-nm NV layer is used to demonstrate proton nuclear magnetic resonance detection. This work reveals the role of interfacial disorder associated with the nitrogen-doping procedure and provides a route to growing high-quality, thin NV-doped layers for quantum-sensing applications.