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arXiv:1304.1407

Effect of fluorinated diamond surface on charge state of nitrogen-vacancy centers

Shanying Cui, Evelyn L. Hu

Published Apr 4, 2013• 2 citations
arXivHTMLPDF

Abstract

We investigated the effect of fluorine-terminated diamond surface on the charged state of shallow nitrogen vacancy defect centers (NVs). Fluorination is achieved with CF4 plasma and the surface chemistry is confirmed with x-ray photoemission spectroscopy. Photoluminescence of these ensemble NVs reveal that fluorine-treated surfaces lead to a higher negatively charged nitrogen vacancy (NV-) population than oxygen-terminated surfaces. Using surface chemistry to control NV charges, in particular increasing the density of NV- centers, is an important step towards improving the optical and spin properties of NVs for quantum information processing and magnetic sensing.

DOI
10.48550/arxiv.1304.1407

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We investigated the effect of fluorine-terminated diamond surface on the charged state of shallow nitrogen vacancy defect centers (NVs). Fluorination is achieved with CF4 plasma and the surface chemistry is confirmed with x-ray photoemission spectroscopy. Photoluminescence of these ensemble NVs reveal that fluorine-treated surfaces lead to a higher negatively charged nitrogen vacancy (NV-) population than oxygen-terminated surfaces. Using surface chemistry to control NV charges, in particular increasing the density of NV- centers, is an important step towards improving the optical and spin properties of NVs for quantum information processing and magnetic sensing.
We investigated the effect of fluorine-terminated diamond surface on the charged state of shallow nitrogen vacancy defect centers (NVs). Fluorination is achieved with CF4 plasma, and the surface chemistry is confirmed with x-ray photoemission spectroscopy. Photoluminescence of these ensemble NVs reveals that fluorine-treated surfaces lead to a higher and more stable negatively charged nitrogen vacancy (NV−) population than oxygen-terminated surfaces. NV− population is estimated by the ratio of negative to neutral charged NV zero-phonon lines. Surface chemistry control of NV− density is an important step towards improving the optical and spin properties of NVs for quantum information processing and magnetic sensing.
Abstract The nitrogen-vacancy (NV) center in diamond is the most promising candidate for quantum sensing because of its beneficial properties. For quantum-sensing applications, a shallow NV center is critical for approximating the sensing target on a diamond surface. Such shallow NV centers are strongly affected by the diamond surface termination. The properties of shallow NV centers in hydrogen-, oxygen-, and fluorine-terminated diamond have been well studied. In recent years, silicon-terminated diamond has also been investigated; however, the effect of silicon-terminated diamond on the properties of shallow NV centers remains unclear. Recently, the suitability of nitrogen-terminated diamond for shallow NV centers has been theoretically and experimentally examined; however, quantum sensing has not yet been performed. In this work, we evaluated the effect of silicon and nitrogen termination on shallow NV centers. The negatively charged state of shallow NV centers was unstable below silicon termination. In contrast, the properties of shallow NV centers in nitrogen-terminated diamond were satisfactory for quantum sensing and enabled 1H NMR detection. Our results are in good agreement with previous reports on silicon and nitrogen terminations and provide the perspective that the stability of shallow NV centers highly depends on the polarity of electron affinity of the diamond surface.
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.
Abstract We investigated the charge state stability and coherence properties of near-surface single nitrogen vacancy (NV) centers in 12 C-enriched diamond for potential use in nanoscale magnetic field sensing applications. The stability of charge states in negatively charged NV centers (NV − ) was evaluated using one of the pulsed optically detected magnetic resonance measurements, Rabi oscillation measurements. During the accumulation of Rabi oscillations, an unstable shallow NV − was converted to a neutral state. As a result, the contrast of Rabi oscillations degraded, depending on charge state stability. We stabilized the NV − state of very shallow NV centers (∼2.6 ± 1.1 nm from the surface) created by 1.2 keV nitrogen ion implantation by diamond surface modification, UV/ozone exposure, and oxygen annealing. This improvement indicates that we can suppress the upward surface band bending and surface potential fluctuations through Fermi level pinning originating from oxygen-terminated diamond surfaces.
The ability to control the charge and spin states of nitrogen-vacancy (NV) centers near the diamond surface is of pivotal importance for quantum applications. Hydrogen-terminated diamond is promising for long spin coherence times and ease of controlling the charge states due to the low density of surface defects. However, it has so far been challenging to create negatively charged single NV centers with controllable spin states beneath a hydrogen-terminated surface because atmospheric adsorbates that act as acceptors induce surface holes. In this study, we optically detected the magnetic resonance of shallow single NV centers in hydrogen-terminated diamond through precise control of the nitrogen implantation fluence. Furthermore, we found that the probability of detecting the resonance was enhanced by reducing the surface acceptor density through passivation of the hydrogen-terminated surface with hexagonal boron nitride without air exposure. This control method opens up new opportunities for using NV centers in quantum applications.
A nitridation process of a diamond surface with nitrogen radical exposure far from the radio-frequency plasma for the stabilization of a negatively charged nitrogen-vacancy (NV − ) centers near the surface is presented. At a nitrogen coverage of as high as 0.9 monolayers, high average Rabi contrasts of 0.40 ± 0.06 and 0.46 ± 0.03 have been obtained for single NV − centers formed by shallow nitrogen implantation with acceleration voltages of 1 and 2 keV, respectively. This indicates that nitrogen termination by a radical exposure process produces an electric charge state suitable for single NV − centers near the surface compared with the states obtained for alternatively terminated surfaces.