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arXiv:2305.06269 · Physical Review Applied

Sensitive ac and dc magnetometry with nitrogen-vacancy-center ensembles in diamond

John F. Barry, Matthew Steinecker, Scott T. Alsid, Jonah A. Majumder, Linh Pham, Michael F. O’Keeffe, Danielle Braje

Published Oct 25, 2024• 87 citations
arXivHTMLPDF

Abstract

Quantum sensing with solid-state spins offers the promise of high spatial resolution, bandwidth, and dynamic range at sensitivities comparable to more mature quantum sensing technologies, such as atomic vapor cells and superconducting devices. However, despite comparable theoretical sensitivity limits, the performance of bulk solid-state quantum sensors has so far lagged behind these more mature alternatives. A recent review [Barry et al., Rev. Mod. Phys. 92, 015004 (2020)] suggests several paths to improve performance of magnetometers employing nitrogen-vacancy defects in diamond, the most-studied solid-state quantum sensing platform. Implementing several suggested techniques, we demonstrate the most sensitive nitrogen-vacancy-based bulk magnetometer reported to date. Our approach combines tailored diamond growth to achieve low strain and long intrinsic dephasing times, the use of double-quantum Ramsey and Hahn-echo magnetometry sequences for broadband and narrowband magnetometry, respectively, and P1 driving to further extend dephasing time. Notably, the device does not include a flux concentrator, preserving the fixed response of the nitrogen vacancies to magnetic field. The magnetometer realizes a minimum sensitivity of $460\phantom{\rule{0.2em}{0ex}}\mathrm{fT}\phantom{\rule{0.2em}{0ex}}{\mathrm{s}}^{1/2}$ in a broadband dc-sensitive mode and $210\phantom{\rule{0.2em}{0ex}}\mathrm{fT}\phantom{\rule{0.2em}{0ex}}{\mathrm{s}}^{1/2}$ in a narrowband ac mode. We describe the experimental setup in detail and highlight potential paths for future improvement.

DOI
10.1103/physrevapplied.22.044069

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Quantum sensing with solid-state spins offers the promise of high spatial resolution, bandwidth, and dynamic range at sensitivities comparable to more mature quantum sensing technologies, such as atomic vapor cells and superconducting devices. However, despite comparable theoretical sensitivity limits, the performance of bulk solid-state quantum sensors has so far lagged behind these more mature alternatives. A recent review [Barry et al., Rev. Mod. Phys. 92, 015004 (2020)] suggests several paths to improve performance of magnetometers employing nitrogen-vacancy defects in diamond, the most-studied solid-state quantum sensing platform. Implementing several suggested techniques, we demonstrate the most sensitive nitrogen-vacancy-based bulk magnetometer reported to date. Our approach combines tailored diamond growth to achieve low strain and long intrinsic dephasing times, the use of double-quantum Ramsey and Hahn-echo magnetometry sequences for broadband and narrowband magnetometry, respectively, and P1 driving to further extend dephasing time. Notably, the device does not include a flux concentrator, preserving the fixed response of the nitrogen vacancies to magnetic field. The magnetometer realizes a minimum sensitivity of 460fTs1/2460\phantom{\rule{0.2em}{0ex}}\mathrm{fT}\phantom{\rule{0.2em}{0ex}}{\mathrm{s}}^{1/2}460fTs1/2 in a broadband dc-sensitive mode and 210fTs1/2210\phantom{\rule{0.2em}{0ex}}\mathrm{fT}\phantom{\rule{0.2em}{0ex}}{\mathrm{s}}^{1/2}210fTs1/2 in a narrowband ac mode. We describe the experimental setup in detail and highlight potential paths for future improvement.
In modern-day quantum metrology, quantum sensors are widely employed to detect weak magnetic fields or nanoscale signals. Quantum devices, exploiting quantum coherence, are inevitably connected to physical constants and can achieve accuracy, repeatability, and precision approaching fundamental limits. As a result, these sensors have shown utility in a wide range of research domains spanning both science and technology. A rapidly emerging quantum sensing platform employs atomic-scale defects in crystals. In particular, magnetometry using nitrogen-vacancy (NV) color centers in diamond has garnered increasing interest. NV systems possess a combination of remarkable properties, optical addressability, long coherence times, and biocompatibility. Sensors based on NV centers excel in spatial resolution and magnetic sensitivity. These diamond-based sensors promise comparable combination of high spatial resolution and magnetic sensitivity without cryogenic operation. The above properties of NV magnetometers promise increasingly integrated quantum measurement technology, as a result, they have been extensively developed with various protocols and find use in numerous applications spanning materials characterization, nuclear magnetic resonance (NMR), condensed matter physics, paleomagnetism, neuroscience and living systems biology, and industrial vector magnetometry. In this chapter, NV centers are explored for magnetic sensing in a number of contexts. In general, we introduce novel regimes for magnetic-field probes with NV ensembles. Specifically, NV centers are developed for sensitive magnetometers for applications where microwaves (MWs) are prohibitively invasive and operations need to be carried out under zero ambient magnetic field. The primary goal of our discussion is to improve the utility of these NV center-based magnetometers.
Diamond-based quantum magnetometers are more sensitive to oscillating (ac) magnetic fields than static (dc) fields because the crystal impurity-induced ensemble dephasing time T2∗{T}_{2}^{*}T2∗​, the relevant sensing time for a dc field, is much shorter than the spin coherence time T2{T}_{2}T2​, which determines the sensitivity to ac fields. Here we demonstrate measurement of dc magnetic fields using a physically rotating ensemble of nitrogen-vacancy centers at a precision ultimately limited by T2{T}_{2}T2​ rather than T2∗{T}_{2}^{*}T2∗​. The rotation period of the diamond is comparable to T2{T}_{2}T2​ and the angle between the nitrogen-vacancy (NV) axis and the target magnetic field changes as a function of time, thus upconverting the static magnetic field to an oscillating field in the physically rotating frame. Using spin-echo interferometry of the rotating NV centers, we are able to perform measurements for over 100 times longer compared to a conventional Ramsey experiment. With modifications our scheme could realize dc sensitivities equivalent to demonstrated NV center ac magnetic field sensitivities of order $0.1\phantom{\rule{0.28em}{0ex}}\mathrm{nT}\phantom{\rule{0.16em}{0ex}}{\mathrm{Hz}}^{\ensuremath{-}1/2}$.
Ensembles of nitrogen-vacancy (NV) centers in diamond are versatile quantum sensors with broad applications in the physical and life sciences. The concentration of neutral substitutional nitrogen ( [ N s 0 ]) strongly influences NV electronic spin coherence times, sensitivity, and optimal sensing strategies. Diamonds with [ N s 0 ] ∼ 1–10 ppm are a focus of recent material engineering efforts, with higher concentrations being favorable for continuous-wave optically detected magnetic resonance (CW-ODMR) and lower concentrations expected to benefit pulsed magnetometry techniques through extended NV spin coherence times and improved sensing duty cycles. In this work, we synthesize and characterize low- [ N s 0 ] ( ∼ 0.8 ppm), NV-enriched diamond material, engineered through low-strain chemical vapor deposition (CVD) growth on high-quality substrates, 12 C isotopic purification, and controlled electron irradiation and annealing. Our results demonstrate good strain homogeneity in diamonds grown on CVD substrates and spin-bath-limited NV dephasing times. By measuring NV spin and charge properties across a wide range of optical NV excitation intensity, we provide direct comparisons of photon-shot-noise-limited magnetic field sensitivity between the current low- [ N s 0 ] and previously studied higher- [ N s 0 ] ( ∼ 14 ppm) NV-diamond sensors. We show that low- [ N s 0 ] diamond can outperform higher- [ N s 0 ] diamond at moderate and low optical NV excitation intensity. Our results provide practical benchmarks and guidance for selecting NV-diamond sensors tailored to specific experimental constraints and sensing requirements.
We demonstrate quantum sensing of dc magnetic fields that exceeds the sensitivity of conventional ${T}_{2}^{\ensuremath{\ast}}$-limited dc magnetometry by more than an order of magnitude. We use nitrogen-vacancy centers in a diamond rotating at periods comparable to the spin coherence time, and characterize the dependence of magnetic sensitivity on measurement time and rotation speed. Our method up-converts only the dc field of interest and preserves the quantum coherence of the sensor. These results definitively improve the sensitivity of a quantum magnetometer to dc fields, demonstrating that sensitivity below the ${T}_{2}^{\ensuremath{\ast}}$ limit is possible and can be applied to any diamond magnetometer where ${T}_{2}\ensuremath{\gg}{T}_{2}^{\ensuremath{\ast}}$ to yield an order-of-magnitude sensitivity improvement.
Abstract Nitrogen-vacancy (NV) center ensembles in diamond are one of the most promising solid-state quantum platforms for various sensing applications. Achieving ultimate sensitivity requires simultaneously long spin dephasing times ( T2∗{T}_{2}^{* }T2∗​ T 2 * ) and high NV center concentrations. In this work, we propose a systematic measurement approach to quantify the electron spin dephasing in NV center ensembles and analyze the contributions of various sources to the dephasing time, including NV-NV interactions, strain and electric field distributions, 13 C nuclear spins, and P1 electron spins. Our method is validated using a series of high-performance diamond samples, providing a comprehensive understanding of dephasing mechanisms and revealing correlations between NV concentration and different dephasing sources. Building on these insights, we outline strategies to further enhance the achievable sensitivity for DC magnetic field measurements.
We demonstrate an absolute magnetometer based on quantum beats in the ground state of nitrogen-vacancy centers in diamond. We show that, by eliminating the dependence of spin evolution on the zero-field splitting D, the magnetometer is immune to temperature fluctuation and strain inhomogeneity. We apply this technique to measure low-frequency magnetic field noise by using a single nitrogen-vacancy center located within 500 nm of the surface of an isotopically pure (99.99% 12C) diamond. The photon-shot-noise limited sensitivity achieves 38 nT/sqrt[Hz] for 4.45 s acquisition time, a factor of sqrt[2] better than the implementation which uses only two spin levels. For long acquisition times (>10 s), we realize up to a factor of 15 improvement in magnetic sensitivity, which demonstrates the robustness of our technique against thermal drifts. Applying our technique to nitrogen-vacancy center ensembles, we eliminate dephasing from longitudinal strain inhomogeneity, resulting in a factor of 2.3 improvement in sensitivity.