Characterization of HPHT Diamonds with NV Centers for High-Sensitivity Bulk-Ensemble Magnetometer
T. Sekiguchi, Y. Kamitsubo, T. Tsuji, Y. Aoki, Masuyama Yuta, T. Taniguchi, M. Miyakawa, C. Shinei, Onoda Shinobu, Abe Hiroshi, Saiki Seiichi, Ishii Shuya, T. Teraji, Ohshima Takeshi, T. Iwasaki, M. Hatano
Quantum sensors utilize quantized energy levels, quan- tum superposition states, and eventually quantum entan- glement, which are also key elements in quantum comput- ing. Electronic and nuclear spins in semiconductors may serve as quantum sensing elements or qubits. The phos- phorus donor in silicon is an ideal qubit in terms of coherence time because of highest chemical purity of host material with isotopic 28Si enrichment and a very low den- sity of structural defects. However, it requires a cryogenic temperature to avoid ionization of the donor. In contrast in diamond, due to the wide band gap, the nitrogen-vacancy (NV) center exhibits optical initialization and readout of its spin state and a long coherence time even above room temperature, promoting its research and development as quantum sensors or qubits. Nevertheless, the syn- thesized diamond crystals with NV centers are not so per- fect as silicon. Therefore, the host material characteriza- tion is essential to improve the bulk-ensemble sensi- tivity to the magnetic field. The present study shows how to measure the spin properties of the diamond as a sens- ing host via the NV centers themselves and how to utilize such information to improve the sensor performance.
Quantum sensors utilize quantized energy levels, quan- tum superposition states, and eventually quantum entan- glement, which are also key elements in quantum comput- ing. Electronic and nuclear spins in semiconductors may serve as quantum sensing elements or qubits. The phos- phorus donor in silicon is an ideal qubit in terms of coherence time because of highest chemical purity of host material with isotopic 28Si enrichment and a very low den- sity of structural defects. However, it requires a cryogenic temperature to avoid ionization of the donor. In contrast in diamond, due to the wide band gap, the nitrogen-vacancy (NV) center exhibits optical initialization and readout of its spin state and a long coherence time even above room temperature, promoting its research and development as quantum sensors or qubits. Nevertheless, the syn- thesized diamond crystals with NV centers are not so per- fect as silicon. Therefore, the host material characteriza- tion is essential to improve the bulk-ensemble sensi- tivity to the magnetic field. The present study shows how to measure the spin properties of the diamond as a sens- ing host via the NV centers themselves and how to utilize such information to improve the sensor performance.
Quantum sensors encompass a diverse class of devices that exploit quantum coherence to detect weak or nanoscale signals. As their behavior is tied to physical constants, quantum sensors can achieve accuracy, repeatability, and precision approaching fundamental limits [1, 2]. As a result, these sensors have shown utility in a wide range of applications in both science and engineering leading to innovations. Among many solid-state spin systems, nitrogen-vacancy (NV) centers in diamonds have attracted considerable attention as a leading platform in many fields of quantum technologies, from quantum sensing to information processing and communication applications. They have superior physical properties, and their quantum coherence is preserved even at room temperature. The energy levels of NV centers are sensitive to magnetic fields, electric fields, strain, and temperature, and the spatial resolution is scalable from nanometers to millimeters. Therefore, diamond quantum sensors are distinctive sensors with multimodality and span scalable application fields. To realize an ideal quantum sensor for applications, the technical challenges in the sensor materials and the quantum control techniques, such as coherent microwave spin manipulation, effective optical spin-state initialization, and readout, have been developed. This chapter briefly explains the sensing principle using NV centers and then introduces sensor systems for biomedical applications, and monitoring of batteries for electric vehicles and internal power devices.
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.
One of the biggest challenges to implement quantum protocols and quantum information processing (QIP) is achieving long coherence times, usually requiring systems at ultra-low temperatures. The nitrogen-vacancy (NV) center in diamond is a promising alternative to this problem. Due to its spin properties, easy manipulation, and the possibility of doing optical state initialization and readout, it quickly became one of the best solid-state spin systems for QIP at room temperature. Here, we present the characterization of the spin-coherence of an ensemble of NV centers in an engineered sample of ultrapure diamond as a testbed for quantum protocols for quantum metrology.
This thesis investigates the theoretical foundations, material properties, and experimental realization of quantum sensors based on the Nitrogen-Vacancy (NV) centers in diamond, a solid-state system that combines quantum coherence with room-temperature operability. The first chapter introduces the principles of quantum sensing, outlining the fundamental definitions, operating protocols, and physical processes underlying the quantum measurement paradigm. Emphasis is placed on the quantum sensing Hamiltonian and the distinction between various classes of quantum sensors. The second chapter focuses on diamond as a host material and on the NV center as a quantum defect. The electronic structure, optical transitions, and spin properties of the NV center are analyzed in detail. Several techniques of NV-based magnetometry are presented, including continuouswave and pulsed optically detected magnetic resonance (ODMR). The discussion also addresses coherence times (T1, T2, and T∗2 ) and methods of diamond synthesis together with NV-center generation through irradiation and annealing. Chapter three develops the physical theory describing the NV center. The Hamiltonian formalism includes spin-spin, hyperfine, and quadrupolar interactions, as well as couplings to external magnetic fields. The chapter further introduces the Bloch sphere representation, magnetic resonance phenomena, and models of lightmatter interaction, ranging from the semiclassical to the fully quantum Rabi framework. A seven-level rate-equation model is proposed to capture the spin dynamics and optical cycling processes of the NV center. The fourth chapter reports the experimental results. After describing materials and methods, several ODMR-based vector magnetometry experiments are presented, highlighting different spectral regimes and the dependence of resonance features on the external magnetic field geometry. Additional studies demonstrate temperature sensing and microwave-free magnetometry techniques for mapping magnetic field distributions. Sensitivity analysis and calibration procedures are also discussed.
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.
Because of their high sensitivity, quantum materials are extremely promising for new technologies. The main challenge lies in maintaining a sufficiently quantum coherence times for quantum computation or quantum sensing systems. NV centers in diamond which are point defects consisting of a substitutional nitrogen atom neighboring an atomic vacancy, where an electron pair can reside in a triplet state – are ideal candidates for the development of industrial-scale quantum systems. These spin states exhibit ms-long coherence times at room temperature and can be manipulated optically, hence opening interesting perspectives for sending magnetic fields with high sensitivity1.At HiQuTe Diamond, we take up the challenge of mastering the entire nitrogen-doped diamond production chain synthesized by Microwave Plasma-Assisted Chemical Vapor Deposition (MPACVD). We aim at creating affordable diamonds specially engineered to achieve long coherence times with high NV density and high doping uniformity. This quest require to overcome the impact of several external factors that contribute to electron spin decoherence. First, the chemical composition of the diamond, specifically the types and concentrations of impurities within the diamond matrix (such as substitutional nitrogen NS, NV centres, mono-vacancies and clusters, hydrogen, etc.), as well as their electrical charge states (NS⁰, NS⁺, NV⁰, NV⁻) should be carefully controlled. Thanks to extensive scientific research conducted over the past decade, combined with our own R&D efforts, we are now able to quantify these parameters using experimental techniques compatible with industrial applications (Raman and UV-Vis spectroscopy) and compare our results with key performance indicators2. Second, we study the relationship between coherence (T2*) and strain inhomogeneities in our diamond layers, which we analyse using birefringence measurements. Our findings demonstrate our capability to produce CVD diamond layers with reduced strain and extended defect and confirm that strain could be a critical limiting factor for T2*.In this poster, I will review the efforts carried out at HiQuTe Diamond to develop specific material that is well suited for quantum sensing applications.References1.Barry, J. F., Schloss, J. M., Bauch, E., Turner, M. J., Hart, C. A., Pham, L. M., & Walsworth, R. L. (2020). Sensitivity optimization for NV-diamond magnetometry. Reviews of Modern Physics, 92(1), 015004.2.Langer, J. (2022). Quantum-grade diamond for cavity-based solutions. Fraunhofer Verlag.