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International Conference on Optical Fiber Sensors (OFS)

NV centres in diamond for magnetic field quantum sensing

Matthew Green, Matthias Fabian, Tong Sheng Sun, K. T. V. Grattan

Published May 22, 2025• 1 citation
Publisher

Abstract

Nitrogen-Vacancy (NV) centres in diamond have been shown to possess a quantised energy structure that allows for a number of macroscopic parameters to be measured with a high level of sensitivity. The process of sensing magnetic fields can be achieved through the behaviour of the NV centre’s electron spin triplet states using the separation of field-dependent and independent states, inferred by applying a microwave frequency to drive transitions. Observation of the states is achieved through optical pumping and stimulated emission, where the intensity of the fluorescent emission and frequency of the applied microwaves relates to the magnitude of the magnetic field the NV centre experiences. The optical method of sensing can be facilitated using optical fibres in which NV diamond particles are embedded between the core and outer fibre layers, leading to a robust platform for further practical applications with strong resistance to external interference.

DOI
10.1117/12.3062857

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This protocol predicts a theoretical magnetic field sensitivity <10µT/√Hz in the range 0.3 - 30mT and I will demonstrate it experimentally with a maximum sensitivity of 3.6mT/Hz. Following, I will focus on exploring techniques to increase the magnetic field sensitivity by improving the material properties of the diamond samples. I will demonstrate that the simultaneous electron irradiation and annealing improves the creation efficiency of an ensemble of NV centres by up to 117%. Finally, I will investigate how substitutional nitrogen defects in the surrounding lattice affects the charge state of the NV centre, its emission intensity, its lifetime and its magnetic field sensitivity. I will study a sample characterised by multiple regions across its volume, with nitrogen concentration changing between 10ppm and 100ppm in each region. 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Nitrogen-Vacancy (NV) centres in diamond have been shown to possess a quantised energy structure that allows for a number of macroscopic parameters to be measured with a high level of sensitivity. The process of sensing magnetic fields can be achieved through the behaviour of the NV centre’s electron spin triplet states using the separation of field-dependent and independent states, inferred by applying a microwave frequency to drive transitions. Observation of the states is achieved through optical pumping and stimulated emission, where the intensity of the fluorescent emission and frequency of the applied microwaves relates to the magnitude of the magnetic field the NV centre experiences. The optical method of sensing can be facilitated using optical fibres in which NV diamond particles are embedded between the core and outer fibre layers, leading to a robust platform for further practical applications with strong resistance to external interference.
The fluorescence of the nitrogen-vacancy (NV) centre in artificial diamond has been widely studied for applications such as quantum communication protocols, quantum computation, fluorescence-based biolabelling, and optical sensing. Optical sensing by itself encompasses a wide range of possible applications: from magnetic and electric field sensing to temperature sensing and enabling, for example, the detection of paramagnetic ions and the identification of molecules by nuclear magnetic resonance. Compared to many other systems capable of optical sensing, the NV centre works at room temperature, and its spin-dependent fluorescence emission is the key property to achieve a high sensitivity to the surrounding environment. Additionally, the NV centre emission is highly photostable, has a relatively short lifetime (~ 12ns) and spans a broad wavelength range, from the red to the near-infrared region of the electromagnetic spectrum (600 - 800nm). While the common denominator of all mentioned applications is the NV centre, the properties of the artificial diamond surrounding the NV centre have a significant impact on its sensing performance. At present, the processing of artificial diamond has not been fully optimised, and research and development towards the realisation of the `best¿ diamond sample for optical sensing is far from over. Specifically, the role of other defects in diamond and their effects on the photo-physical properties of the NV centres are not entirely understood. In this thesis, I will discuss the potential benefits of a novel processing technique to create ensembles of NV centres, and the importance that surrounding nitrogen defects has on the achievable magnetic field sensitivity. Additionally, I will show both theoretical and experimental investigations of the NV centres photo-physical processes, with focus on magnetic field sensing. I will initially explore a protocol for microwave-free magnetometry. This protocol predicts a theoretical magnetic field sensitivity <10µT/√Hz in the range 0.3 - 30mT and I will demonstrate it experimentally with a maximum sensitivity of 3.6mT/Hz. Following, I will focus on exploring techniques to increase the magnetic field sensitivity by improving the material properties of the diamond samples. I will demonstrate that the simultaneous electron irradiation and annealing improves the creation efficiency of an ensemble of NV centres by up to 117%. Finally, I will investigate how substitutional nitrogen defects in the surrounding lattice affects the charge state of the NV centre, its emission intensity, its lifetime and its magnetic field sensitivity. I will study a sample characterised by multiple regions across its volume, with nitrogen concentration changing between 10ppm and 100ppm in each region. There si an optimal region with ~ 40ppm of substitutional nitrogen which demonstrates the highest fluorescence emission, mainly from the negatively-charged NV centre, and the highest magnetic field sensitivity of 1.6 ± 0.2µT/√Hz. However, both the regions with lower and higher substitutional nitrogen concentration than the optimal region show lower emission intensity and worse magnetic field sensitivity. Following is a summary of the content in each chapter: Chapter 1 will present an introduction to the diamond material and the classification of artificial diamond samples. It will introduce the NV centre, its fluorescence properties and the process to create NV centres in diamond. The chapter will also introduce the concepts around optical magnetometry and the working principle that allows the NV centre to sense magnetic fields as well as other external quantities, such as temperature or pressure. Finally, it will include a brief overview of the defects that are found in artificial diamond or are created during the sample processing. Chapter 2 will describe the working principle of the instruments utilised in this work. I will list the details of each instrument and describe the methods used for the analysis of the data. Chapter 3 will introduce the background of modelling the fluorescence emission from NV centres. I will discuss the implementation of a computational model based on the Lindblad master equation to simulate the photo-physical dynamics of the NV centre. I will demonstrate the successful simulation of the saturation emission, fluorescence lifetime and optically detected magnetic resonance using the theoretical model. Finally, I will explore the theoretically predicted sensitivity of microwave-free magnetometry, based on the NV centre emission intensity change under an external magnetic field. Chapter 4 will demonstrate experimentally the microwave-free magnetometry technique. In relation to the study of microwave-free magnetometry, this chapter will explore an unexpected increase in emission intensity at high magnetic fields > 100mT. Combining the experimental observations and the theoretical simulation developed in the previous chapter, I will identify and discuss a phenomenological decrease in the NV centre transition rate from the triplet state to the singlet state. The chapter will conclude comparing the experimental and theoretical sensitivities associated with the microwave-free magnetometry technique. Chapter 5 will show the characterisation of a diamond sample at each step of the process to create NV centres. I will study the electron irradiation followed by separate annealing on a high-pressure high-temperature diamond sample. I will then characterise the sample employing visible and infrared absorption spectroscopy, as well as measure the fluorescence spectra and lifetime of the defects identified at each step. Chapter 6 will examine an alternative method to create NV centres in diamond. I will compare diamond samples irradiated and annealed separately with samples simultaneously irradiated and annealed (referred to as 'annealing in situ'). To compare the two processes, I will estimate the concentration of nitrogen defects and NV centres and calculate their N-to-NV conversion efficiency. Chapter 7 will discuss the effects of substitutional nitrogen on the properties of the NV centres in diamond. For this discussion, I will use a single-crystal diamond that shows the presence of 4 growth sectors. Each growth sector is characterised by a different nitrogen concentration, as I will demonstrate at the beginning of the chapter. I will focus on 4 main properties affected by the concentration of nitrogen in the different sectors: the balance between the charge states of the NV centre, the overall fluorescence intensity from each sector, the fluorescence lifetime and its relation to non-radiative processes, and the magnetic field sensitivity obtained with the optically detected magnetic resonance technique. Chapter 8 will gather the results and conclusions of the entire body of work. It will also discuss future avenues of research in the topic of diamond processing and characterisations, to improve the existing optical sensing applications.
Nitrogen vacancy (NV) centres are a type of defect in diamond that exhibit a number of interesting properties. NV centres can be optically excited around 450-650 nm and emit fluorescence at around 550-800 nm [1]. The optical excitation also spin polarises the negatively charged NV centres, permitting optical detection of magnetic resonance [2]. This allows nanotesla scale sensitive magnetometry to be performed with nanometre scale spatial resolution [3].To date, a direct measurement of stimulated emission from ensembles of NV centres in diamond has yet to be demonstrated experimentally. Despite this, stimulated emission depletion microscopy has been utilised in superresolution imaging that relies on the stimulated emission of single NV centres to quench fluorescence [4]. Recently, there has also been similar indirect experimental evidence of stimulated emission in NV ensembles [5]. We thus aimed to show both optical gain of a probe beam in a pumped NV-rich diamond sample and a modulation of this gain via microwave excitation of its ground level spin transitions. The experimental set-up consisted of a pump (532 nm) and probe (723-950 nm) laser beam combined with a dichroic mirror and focused into a bulk diamond specimen to a spot-size of around 90 microns. Pump excitation powers of up to 3 W and probe powers up to 0.5 W were used. The beams were then collimated and separated with a prism and the probe power measured with a photodiode. The diamond specimen was placed on an antenna to allow simultaneous excitation with microwaves. A double modulation scheme was employed to measure either the change in probe power due to the pump laser or the microwave excitation during any one experiment.
The physical properties of diamond crystals, such as color or electrical conductivity, can be controlled via impurities. In particular, when doped with nitrogen, optically active nitrogen-vacancy centers (NV), can be induced. The center is an outstanding quantum spin system that enables, under ambient conditions, optical initialization, readout, and coherent microwave control with applications in sensing and quantum information. Under optical and radio frequency excitation, the Zeeman splitting of the degenerate states allows the quantitative measurement of external magnetic fields with high sensitivity. This study provides a pedagogical introduction to the properties of the NV centers as well as a step-by-step process to develop and test a simple magnetic quantum sensor based on color centers with significant potential for the development of highly compact multisensor systems.
Negatively charged nitrogen-vacancy centres in diamond are promising quantum magnetic field sensors. Laser threshold magnetometry has been a theoretical approach for the improvement of NV-centre ensemble sensitivity via increased signal strength and magnetic field contrast. In this work we experimentally demonstrate laser threshold magnetometry. We use a macroscopic high-finesse laser cavity containing a highly NV-doped and low absorbing diamond gain medium that is pumped at 532nm and resonantly seeded at 710nm. This enables amplification of the signal power by stimulated emission of 64%. We show the magnetic-field dependency of the amplification and thus, demonstrate magnetic-field dependent stimulated emission from an NV-centre ensemble. This emission shows a record contrast of 33% and a maximum output power in the mW regime. These advantages of coherent read-out of NV-centres pave the way for novel cavity and laser applications of quantum defects as well as diamond NV magnetic field sensors with significantly improved sensitivity for the health, research and mining sectors.
The nitrogen-vacancy (NV) centre in diamond is a perfect candidate for quantum sensing applications applied to numerous fields of science. Past studies improved the sensitivity of diamonds containing NV centres by increasing their density or prolonging their coherence time. However, few studies discussed the effects of other defects inside the diamond crystal on the sensitivity of the NV centres. In this study, we demonstrated the implication of single substitutional nitrogen defects on the fluorescence emission, charge state stability, coherence time and sensitivity of the NV centres. We found that there is an optimal concentration of nitrogen defects that allows diamond samples to have a high-density of NV centres and high fluorescence without significantly affecting the coherence time. This results will inform the correct choice of diamond characteristics for current and future quantum sensing applications with the NV centres.
The nitrogen-vacancy (NV) centre in diamond is a perfect candidate for quantum sensing applications applied to numerous fields of science. Past studies improved the sensitivity of diamonds containing NV centres by increasing their density or prolonging their coherence time. However, few studies discussed the effects of other defects inside the diamond crystal on the sensitivity of the NV centres. In this study, we demonstrated the implication of single substitutional nitrogen defects on the fluorescence emission, charge state stability, coherence time and sensitivity of the NV centres. We found that there is an optimal concentration of nitrogen defects that allows diamond samples to have a high-density of NV centres and high fluorescence without significantly affecting the coherence time. This results will inform the correct choice of diamond characteristics for current and future quantum sensing applications with the NV centres.