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arXiv:1807.04444 · AIP Advances

Wide-field diamond magnetometry with millihertz frequency resolution and nanotesla sensitivity

Kosuke Mizuno, Makoto Nakajima, Hitoshi Ishiwata, Yuta Masuyama, Takayuki Iwasaki, Mutsuko Hatano

Published Dec 1, 2018• 20 citations
arXivHTMLPDF

Abstract

Wide-field quantum magnetometry using nitrogen-vacancy (NV) center in diamond can be a breakthrough for a nuclear magnetic resonance (NMR) in a small volume, which is important for biological applications. Although the coherence time of the electron spin of the NV center results in a limited frequency resolution for diamond magnetometry in the range 10–100 kHz, recent studies have shown that a phase-sensitive protocol can circumvent this limit using a confocal setup. We proposed a new measurement protocol, “iQdyne,” which facilitates an improved frequency resolution of wide-field imaging, unencumbered by the coherence limit imposed by the NV center. We demonstrated wide-field magnetometry with a frequency resolution of 238 mHz and a magnetic sensitivity of 65 nT/Hz1/2, which are superior to those obtained using a conventional XY8-based technique, and showed the potential of the iQdyne protocol for the wide-field NMR imaging.

DOI
10.1063/1.5048265

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•Jun 4, 2019•0 citations
Wide-field quantum magnetometry using nitrogen-vacancy (NV) center in diamond can be a breakthrough for a nuclear magnetic resonance (NMR) in a small volume, which is important for biological applications. Although the coherence time of the electron spin of the NV center results in a limited frequency resolution for diamond magnetometry in the range 10–100 kHz, recent studies have shown that a phase-sensitive protocol can circumvent this limit using a confocal setup. We proposed a new measurement protocol, “iQdyne,” which facilitates an improved frequency resolution of wide-field imaging, unencumbered by the coherence limit imposed by the NV center. We demonstrated wide-field magnetometry with a frequency resolution of 238 mHz and a magnetic sensitivity of 65 nT/Hz1/2, which are superior to those obtained using a conventional XY8-based technique, and showed the potential of the iQdyne protocol for the wide-field NMR imaging.
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.
Quantum systems composed of solid-state electronic spins can be sensitive detectors of narrowband magnetic fields. A prominent example is the nitrogen-vacancy (NV) center in diamond, which has been employed for magnetic spectroscopy with high spatial and spectral resolution. However, NV-diamond spectroscopy protocols are typically based on dynamical decoupling sequences, which are limited to low-frequency signals ( ≲ 20 MHz) due to the technical requirements on microwave (MW) pulses used to manipulate NV electronic spins. In this work, we experimentally demonstrate a high-resolution magnetic spectroscopy protocol that integrates a quantum frequency mixing (QFM) effect in a dense NV ensemble with coherently averaged synchronized readout (CASR) to provide both a wide range of signal frequency detection and sub-Hz spectral resolution. We assess the sensitivity of this QFM-CASR protocol across a frequency range of 10 MHz to 4 GHz. By measuring the spectra of multi-frequency signals near 0.6, 2.4 and 4 GHz, we demonstrate sub-Hz spectral resolution with a nT-scale noise floor for the target signal, and precise phase measurement with error < 1 ∘ . Compared to state-of-the-art NV-diamond techniques for high-resolution magnetic spectroscopy, the QFM-CASR protocol extends the signal frequency range by more than an order of magnitude, enabling applications in radio frequency (RF) and MW signal microscopy and analysis, as well as tesla-scale nuclear magnetic resonance (NMR) spectroscopy of small samples.
Abstract Quantum systems composed of solid-state electronic spins can be sensitive detectors of narrowband magnetic fields. A prominent example is the nitrogen-vacancy (NV) center in diamond, which has been employed for magnetic spectroscopy with high spatial and spectral resolution. However, NV-diamond spectroscopy protocols are typically based on dynamical decoupling sequences, which are limited to low-frequency signals (≲ 20 MHz) due to the technical requirements on microwave (MW) pulses used to manipulate NV electronic spins. In this work, we experimentally demonstrate a high-resolution magnetic spectroscopy protocol that integrates a quantum frequency mixing (QFM) effect in a dense NV ensemble with coherently averaged synchronized readout (CASR) to provide both a wide range of signal frequency detection and sub-Hz spectral resolution. We assess the sensitivity of this QFM-CASR protocol across a frequency range of 10 MHz to 4 GHz. By measuring the spectra of multi-frequency signals near 0.6, 2.4 and 4 GHz, we demonstrate sub-Hz spectral resolution with a nT-scale noise floor for the target signal, and precise phase measurement with error <1°. Compared to state-of-the-art NV-diamond techniques for narrowband magnetic spectroscopy, the QFM-CASR protocol greatly extends the detectable frequency range, enabling applications in high-frequency radio frequency (RF) and MW signal microscopy and analysis, as well as tesla-scale nuclear magnetic resonance (NMR) spectroscopy of small samples.
High-resolution wide-spectrum measurement techniques have important applications in fields such as astronomy, wireless communication, and medical imaging. Nitrogen-vacancy (NV) center in diamond is well known for its high stability, high sensitivity, real-time monitoring, single-point detection, and suitability for long-term measurement, and has an outstanding choice for spectrum analyzers. Currently, spectrum analyzers based on NV centers as detectors can perform real-time spectrum analysis in the range of several tens of gigahertz, but their frequency resolution is limited to a MHz level. In this study, we construct a quantum diamond microwave spectrum imaging system by combining continuous wave-mixing techniques. According to the spin-related properties of the NV center in diamond, we implement optical pumping by 532 nm green laser light illuminating the diamond NV center. A spherical magnet is used to produce a magnetic field gradient along the direction of the diamond crystal. By adjusting the size and direction of the magnetic field gradient, spatial encoding of the resonance frequency of the NV center is achieved. The magnetic field gradient induces the Zeeman effect on the diamond surface at different positions, generating corresponding ODMR signals. Through accurate programming, we coordinate the frequency scanning step size of the microwave source with the camera exposure and image storage time, and synchronize them circularly according to the order of image acquisition. Ultimately, after algorithmic processing, we successfully obtain comprehensive spectrum data in a range from 900 MHz to 6.0 GHz. Within the measurable spectrum range, the system employs continuous wave-mixing, simultaneously applying resonant microwaves and slightly detuning auxiliary microwaves to effectively excite the NV center. This method triggers off microwave interference effects, disrupting the balance between laser-induced polarization and microwave-induced spontaneous relaxation. Specifically, microwave interference causes the phase and amplitude of the fluorescence signal to change, leading to the generation of alternating current fluorescence signals. This further enhances the response of the NV magnetometer to weak microwave signals. The method enables the system to achieve a frequency resolution of 1 Hz in the measurable spectrum range, and it can separately measure the frequency resolution of multiple frequency points with a frequency step size of 1 MHz. The research results indicate that the wide-spectrum measurement based on NV centers can achieve sub-hertz frequency resolution, providing robust technical support for future spectrum analysis and applications.
Quantum sensing using nitrogen-vacancy (NV) centers in diamond has emerged as a powerful platform for detecting ultra-low magnetic fields under ambient conditions. Owing to their long spin coherence times, optical addressability, and compatibility with aqueous environments, it has found widespread applications in biosensing and bio-imaging. This review presents the fundamental principles and recent advances in NV-based quantum magnetometry for biosensing applications, with a particular focus on measurements in aqueous medium and at cellular and molecular length scales. We discuss the underlying spin physics of NV centers and highlight two primary detection modalities: optically detected magnetic resonance (ODMR) and T1 relaxometry-based sensing and how these approaches aids in the detection of both static magnetic fields and dynamic magnetic noise arising from biological processes. The review explores key application areas, including nanoscale nuclear magnetic resonance (NMR), monitoring of neural activity, detection of abnormal or rogue cells using NV-based platforms etc. In addition, strategies for enhancing sensitivity, such as surface functionalization of nanodiamonds, femtosecond (fs) laser-written photonic structures, and integration with microfluidic and lab-on-chip systems have also been discussed in depth. We also address the critical challenges, including surface-induced decoherence, charge-state instability, and signal-to-noise limitations in biofluids associated with NV-based biosensing applications. Finally, we outline future prospects, highlighting how NV-based magnetic biosensing provides a promising pathway for translating quantum sensing technologies into practical biomedical applications.
Nitrogen—Vacancy (NV) center in diamond can detect tiny magnetic field due to relative long coherence time even at room temperature. Its optical accessibility and capability of thin-film formation provide us an interesting sensing modality such as wide field imaging. We have reported phase sensitive protocol for ac magnetic field designed for wide field setup.[1] In this study we demonstrate an application of phase sensitive protocol; measuring distribution of ac magnetic field strength by phase sensing. Previous methods of multi-pulse quantum sensing such as XY8 realize quite high sensitivity of ac magnetic field. Since XY8 has dependencies on strength and phase of ac magnetic field, it is necessary to adjust ac phase to an optimal point in order to obtain a best sensitivity, and we cannot distinguish the effect of amplitude and phase. Recent studies have showed utilizing time-domain information is effective for improving frequency resolution of quantum sensing,[2,3] and we found same technique is also effective for simultaneous measurement of strength and phase. Here we propose a robust method for amplitude estimation by phase sensing. We added another signal for reference, then sensing phase difference between target signal and reference can be converted into amplitude. Conventional XY8 sensing is based upon fluorescence measurement which can be affected easily by many obstacles such as stray light, autofluorescence, and fringes of excitation laser. In the other hand, our method can be more robust because it is based on phase measurement. Nothing can change the phase except absorption of ac signal. This work was supported by MEXT Q-LEAP, CAO PRISM, Japan. [1] Mizuno et al., AIP advances 2018 [2][3] Boss, Schmitt