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arXiv:2311.14129 · ACS Photonics

Stability of Near-Surface Nitrogen Vacancy Centers Using Dielectric Surface Passivation

Ravi Kumar, Saksham Mahajan, Felix Donaldson, Siddharth Dhomkar, Hector J. Lancaster, Curran Kalha, Aysha A. Riaz, Yujiang Zhu, Christopher A. Howard, Anna Regoutz, John J. L. Morton

Published Feb 14, 2024• 26 citations
arXivHTMLPDF

Abstract

High Resolution Image Download MS PowerPoint Slide We study the photophysical stability of ensemble near-surface nitrogen vacancy (NV) centers in diamond under vacuum and air. The optically detected magnetic resonance contrast of the NV centers was measured following exposure to laser illumination, showing opposing trends in air compared to vacuum (increasing by up to 9% and dropping by up to 25%, respectively). Characterization using X-ray photoelectron spectroscopy (XPS) suggests a surface reconstruction: In air, atmospheric oxygen adsorption on a surface leads to an increase in NV – fraction, whereas in vacuum, net oxygen desorption increases the NV 0 fraction. NV charge state switching is confirmed by photoluminescence spectroscopy. Deposition of ∼2 nm alumina (Al 2 O 3 ) over the diamond surface was shown to stabilize the NV charge state under illumination in either environment, attributed to a more stable surface electronegativity. The use of an alumina coating on diamond is therefore a promising approach to improve the resilience of NV sensors.

DOI
10.1021/acsphotonics.3c01773

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High Resolution Image Download MS PowerPoint Slide We study the photophysical stability of ensemble near-surface nitrogen vacancy (NV) centers in diamond under vacuum and air. The optically detected magnetic resonance contrast of the NV centers was measured following exposure to laser illumination, showing opposing trends in air compared to vacuum (increasing by up to 9% and dropping by up to 25%, respectively). Characterization using X-ray photoelectron spectroscopy (XPS) suggests a surface reconstruction: In air, atmospheric oxygen adsorption on a surface leads to an increase in NV – fraction, whereas in vacuum, net oxygen desorption increases the NV 0 fraction. NV charge state switching is confirmed by photoluminescence spectroscopy. Deposition of ∼2 nm alumina (Al 2 O 3 ) over the diamond surface was shown to stabilize the NV charge state under illumination in either environment, attributed to a more stable surface electronegativity. The use of an alumina coating on diamond is therefore a promising approach to improve the resilience of NV sensors.
Degradation of near surface nitrogen vacancy (NV) centers in diamond under optical illumination has restricted their deployment in applications such as scanning NV magnetomety, particularly under harsh environment such as low temperatures and vacuum. Previously, alumina passivation of planar diamond samples has been shown to reduce the degradation of near surface ensemble NV centers in vacuum. Here, we expand this study to incorporate photonic nanostructures by analyzing the single photon emission characteristics of NV centers embedded in an array of alumina-coated diamond nanopillars in high vacuum and low temperature (6K, high vacuum) environments under non-resonant (522 nm) laser exposure. We find that, in contrast to the oxygen-terminated diamond nanopillars, NV centers in the alumina-coated nanopillars demonstrate negligible change in the single photon purity and brightness over the course of laser exposure in vacuum. At low temperature, NV centers under alumina termination demonstrate stable single photon emission, whereas under oxygen termination the single photon purity degrades under high intensity laser exposure. Alumina surface passivation is therefore shown as a viable path toward the realization of robust NV-diamond based nanoscale sensing under non-ambient atmospheric environments, including using diamond scanning probes.
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.
Control of charge-state stability in near-surface quantum defects is critical for nanoscale sensing, yet remains particularly challenging under ultra-high vacuum (UHV), where surface-induced band bending destabilizes the metrologically relevant charge-state. Here, we present a robust and reproducible approach for stabilizing shallowly implanted (< 10 nm deep) nitrogen-vacancy (NV) centers in near-UHV conditions (P = 3×10−93 \times 10^{-9}3×10−9 mbar) based on dielectric interface engineering. Through measurements on individually addressable NV centers, we demonstrate that a TiO2 coating on the diamond suppresses surface-induced electrostatic fields, yielding a 79% increase n NV- population and a 45% enhancement in NV-spin resonance contrast at room temperature. Coherent control measurements further reveal suppressed charge-state conversion dynamics. These results establish dielectric screening as a powerful and reproducible strategy to engineer charge transition energetics of NV centers in scanning-probe-compatible geometries under extreme conditions.
High Resolution Image Download MS PowerPoint Slide Near-surface negatively charged nitrogen vacancy (NV) centers hold excellent promise for nanoscale magnetic imaging and quantum sensing. However, they often experience charge-state instabilities, leading to strongly reduced fluorescence and NV coherence time, which negatively impact magnetic imaging sensitivity. This occurs even more severely at 4 K and ultrahigh vacuum (UHV, p = 2 × 10 –10 mbar). We demonstrate that in situ adsorption of H 2 O on the diamond surface allows the partial recovery of the shallow NV sensors. Combining these with band-bending calculations, we conclude that controlled surface treatments are essential for implementing NV-based quantum sensing protocols under cryogenic UHV conditions.
Abstract The nitrogen-vacancy (NV) color center in diamond has demonstrated great promise in a wide range of quantum sensing. Recently, there have been a series of proposals and experiments using NV centers to detect spin noise of quantum materials near the diamond surface. This is a rich complex area of study with novel nano-magnetism and electronic behavior, that the NV center would be ideal for sensing. However, due to the electronic properties of the NV itself and its host material, getting high quality NV centers within nanometers of such systems is challenging. Band bending caused by space charges formed at the metal-semiconductor interface force the NV center into its insensitive charge states. Here, we investigate optimizing this interface by depositing thin metal films and thin insulating layers on a series of NV ensembles at different depths to characterize the impact of metal films on different ensemble depths. We find an improvement of coherence and dephasing times we attribute to ionization of other paramagnetic defects. The insulating layer of alumina between the metal and diamond provide improved photoluminescence and higher sensitivity in all modes of sensing as compared to direct contact with the metal, providing as much as a factor of 2 increase in sensitivity, decrease of integration time by a factor of 4, for NV T 1 relaxometry measurements.
The nitrogen-vacancy (NV) color center in diamond has demonstrated great promise in a wide range of quantum sensing. Recently, there have been a series of proposals and experiments using NV centers to detect spin noise of quantum materials near the diamond surface. This is a rich complex area of study with novel nano-magnetism and electronic behavior, that the NV center would be ideal for sensing. However, due to the electronic properties of the NV itself and its host material, getting high quality NV centers within nanometers of such systems is challenging. Band bending caused by space charges formed at the metal-semiconductor interface force the NV center into its insensitive charge states. Here, we investigate optimizing this interface by depositing thin metal films and thin insulating layers on a series of NV ensembles at different depths to characterize the impact of metal films on different ensemble depths. We find an improvement of coherence and dephasing times we attribute to ionization of other paramagnetic defects. The insulating layer of alumina between the metal and diamond provide improved photoluminescence and higher sensitivity in all modes of sensing as compared to direct contact with the metal, providing as much as a factor of 2 increase in sensitivity, decrease of integration time by a factor of 4, for NV T1T_1T1​ relaxometry measurements.