The recent decade has witnessed exciting developments in quantum science and technology. Quantum sensing is a rapidly growing branch, which exploits the fragility of quantum systems to detect small external signals. The extreme control at the single-atom level and the remarkably long coherence time of engineered quantum systems enable unprecedented sensitivity and precision, beating the performance of classical techniques. The nitrogen-vacancy (NV) center in diamond is one of the most promising quantum sensors. Its unique advantages have attracted considerable attention, including a long spin coherence time throughout a broad temperature range, nanoscale resolution limited by the sensor-sample distance, convenient optical control of its spin states and remarkably versatile sensing capabilities. Its properties are well studied under a bias magnetic field oriented along its quantization axis. However, its sensing capabilities in the presence of an off-axis magnetic field are much less explored. My research aims to unlock the full potential of NV quantum sensor by developing new sensing modalities under a magnetic field acting perpendicular to the NV axis, and furthermore, integrating them into a scanning probe microscope. In this dissertation, I will report our progress toward building a scanning NV multimodal quantum imaging platform, which will open up exciting opportunities in measuring nanoscale phenomena. The first chapter provides an introduction to the background of quantum sensing with NV centers, followed by a discussion on its basic properties and established sensing techniques. The second and third chapters are dedicated to two experiments performed under a perpendicular magnetic field where traditional NV magnetometry based on the Zeeman effect fails. In the second chapter, I will introduce a new sensing strategy that uses the entanglement between the electron and nuclear spins to restore the magnetic field sensitivity under this unfavored condition. This allows us to sense small changes in the magnetic field angle relative to the NV axis, and to detect anisotropic magnetic noise in the local environment. In the third chapter, I will present our latest development of scanning NV electrometry, where a single NV at the apex of a diamond scanning probe images external alternating (AC) and direct (DC) electric fields with sub-100 nm resolution. In the last chapter, I will discuss our efforts on four experiments that were left unfinished. I will present the results we have achieved, analyze the challenges that we faced and propose potential solutions to overcome them.
The recent decade has witnessed exciting developments in quantum science and technology. Quantum sensing is a rapidly growing branch, which exploits the fragility of quantum systems to detect small external signals. The extreme control at the single-atom level and the remarkably long coherence time of engineered quantum systems enable unprecedented sensitivity and precision, beating the performance of classical techniques. The nitrogen-vacancy (NV) center in diamond is one of the most promising quantum sensors. Its unique advantages have attracted considerable attention, including a long spin coherence time throughout a broad temperature range, nanoscale resolution limited by the sensor-sample distance, convenient optical control of its spin states and remarkably versatile sensing capabilities. Its properties are well studied under a bias magnetic field oriented along its quantization axis. However, its sensing capabilities in the presence of an off-axis magnetic field are much less explored. My research aims to unlock the full potential of NV quantum sensor by developing new sensing modalities under a magnetic field acting perpendicular to the NV axis, and furthermore, integrating them into a scanning probe microscope. In this dissertation, I will report our progress toward building a scanning NV multimodal quantum imaging platform, which will open up exciting opportunities in measuring nanoscale phenomena. The first chapter provides an introduction to the background of quantum sensing with NV centers, followed by a discussion on its basic properties and established sensing techniques. The second and third chapters are dedicated to two experiments performed under a perpendicular magnetic field where traditional NV magnetometry based on the Zeeman effect fails. In the second chapter, I will introduce a new sensing strategy that uses the entanglement between the electron and nuclear spins to restore the magnetic field sensitivity under this unfavored condition. This allows us to sense small changes in the magnetic field angle relative to the NV axis, and to detect anisotropic magnetic noise in the local environment. In the third chapter, I will present our latest development of scanning NV electrometry, where a single NV at the apex of a diamond scanning probe images external alternating (AC) and direct (DC) electric fields with sub-100 nm resolution. In the last chapter, I will discuss our efforts on four experiments that were left unfinished. I will present the results we have achieved, analyze the challenges that we faced and propose potential solutions to overcome them.
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 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.
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.
Quantum sensing has witnessed rapid development and transition from laboratories to practical applications in the past decade. Applications of quantum sensors, ranging from nanotechnologies to biosensing, are expected to benefit from quantum sensors' unprecedented spatial resolution and sensitivity. Solid-state spin systems are particularly attractive platforms for quantum sensing technologies because room temperature operation is viable while reaching the quantum limits of sensitivity. Among various solid-state spin systems, nitrogen-vacancy (NV) centers in diamond demonstrated high-fidelity initialization, coherent control, and high contrast readout of the electron spin state. However, electron spin coherence due to noise from the surrounding spin bath and this environment effect limits the sensitivity of NV centers. Thus, a critical task in NV center-based quantum sensing is sensitivity enhancement through coherence protection. Several strategies, such as dynamical decoupling techniques, feedback control, and nuclear spin-assisted sensing protocols, have been developed and realized for this task. Among these strategies, nuclear spin-assisted protocols have demonstrated greater enhancement of electron spin coherence. In addition, the electron and nuclear spin pair of an NV center in diamond naturally allows the application of the nuclear spin-assisted sensitivity enhancement protocol. Owing to long nuclear coherence times, further enhancement of sensitivity can be achieved by exploiting active nuclear spins (e.g., 14N, 13C) in the proximity of an NV center as memory ancillas when coupled with the NV center. Here, we review the spin properties of NV centers, mechanisms of the nuclear spin-assisted protocol and its gate variation, and the status of quantum sensing applications in high-resolution nuclear spin spectroscopy, atomic imaging, and magnetic field sensing. We discuss the potential for commercialization, current challenges in sensitivity enhancement, and conclude with future research directions for promoting the development of nuclear spin-assisted protocol and its integration into industrial applications.
This dissertation investigates applications of the Nitrogen vacancy in diamond (NV). The NV is a unique quantum system allowing for optical polarization and read out even at ambient conditions. Its electron spin (S=1) has coherence times in the order of milliseconds and is therefore an ideal candidate to investigate the foundations of quantum mechanics as well as exploiting quantum effects in metrology and information processing applications. To utilize the NV for quantum technologies, first the interaction of the NV with its surroundings has to be investigated and controlled. Here dynamical decoupling sequences (CPMG) could be utilized to extend the NV coherence time to a few milliseconds by decoupling the NV from its surrounding spin bath (given by the 13C isotope, natural abundance 1.1%). But not only decoupling sequences can be used to suppress the spin bath interaction, also eigen state tailoring can suppress the bath interaction. As long as strain is the dominant interaction, the NV eigen energies are not susceptible to small magnetic field changes. Therefore the magnetic dipole interaction with the spin bath is suppressed. But the spin bath is not only a nuisance limiting NV coherence times, but also a potential resource for quantum technologies. In order to harness the individual 13C nuclear spins, their interaction with the NV and among themselves has to be investigated. To not be limited by the NV coherence times, a new spectroscopy method, only limited by the NV lifetime, was developed. This can in principle be extended to the second range by using a nuclear spin memory. First advances in quantum technology were demonstrated in the field of metrology, where the Zeeman effect of the NV center allowed for precise nanoscale measurement of magnetic fields. Here this concept was extended to us the Stark effect to detect electric fields. A sensitivity of η=142.6±3.6 V/(cmHz1/2) was demonstrated. This is equivalent to the detection of a single elemental charge at a distance of 150 nm in one second. By using two NVs with a distance of less then 20 nm, a demonstration of nanoscale single fundamental charge detection was feasible. Here one NV was used as a controllable fundamental charge while the other NV was used as sensor NV, detecting the electric field of the fundamental charge. This allowed for the detection of a single electronic charge at ambient conditions. Another keystone of quantum technology is the reliable on demand or heralded creation of entanglement. In this dissertation, the successful entanglement of two electron spins in solid state at ambient conditions is demonstrated. The fundamental interaction used to create an entangled state was dipolar coupling between the two electron spins. In order to be able to harness weaker coupling strengths, an entanglement protocol based on dynamical decoupling was developed. A fidelity of F=0.67±0.04 was demonstrated. By using the intrinsic nuclear spins of the nitrogen it was possible to store the entangled state on the millisecond time scale. However, the theoretical limit for the fidelity given by the polarization and the coherence times is F=0.849. The discrepancy can be explained by pulse errors. These can be avoided by using optimal control yielding a fidelity of F=0.824±0.015. Also optimal control allowed for nuclear spin entanglement by storing the electron spin entanglement on the nitrogen nuclear spins. These experiments are first steps towards a room temperature quantum register, where the electron spins are used as bus to transport information and the nuclear spins act as a memory.
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.