School of Physics - Theses

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    Developing and applying quantum sensors based on optically addressable spin defects
    Healey, Alexander Joseph ( 2023-04)
    Quantum sensing aims to further our understanding of the natural world and support an upcoming technological revolution by exploiting quantum properties or systems to exceed the performance of classical sensing. Owing to their convenient modes of operation and strong room temperature quantum properties, optically active spin defects hosted within solid state materials have come to prominence as one of the foremost tools of choice in this landscape. Many applications now aim to leverage dense ensembles of such defects to boost measurement sensitivity or scale up, which places greater emphasis on the quality of the host material and sensor production methods since cherry-picking individual defects is no longer an option. The prototypical example of such a defect is the nitrogen-vacancy (NV) centre in diamond, which exhibits remarkable room temperature spin coherence, bestowed upon it by diamond's material properties. In this thesis, we first look at optimising the production of NV ensembles for quantum sensing, aiming to efficiently and cost-effectively produce sensors capable of performing high sensitivity measurements in two key regimes that will be central to the experimental applications explored later. The topics examined are hyperpolarisation of a nuclear spin ensemble on the diamond surface through coupling to an ultra-near-surface NV layer, and investigating the properties of a van der Waals antiferromagnet through widefield NV microscopy. The demands placed on the NV layer for these applications are diverse from one another, with charge stability and quantum coherence properties being vital for the former, and the ability to scalably and reproducibly create layers of known thickness crucial to the latter. In light of these studies, we finally consider whether a different spin system housed within an entirely separate materials system, the boron-vacancy defect in hexagonal boron nitride, may be a suitable alternative to the well-established NV diamond system. We find that the distinct properties of the new host material provide both advantages and disadvantages compared to diamond, and that this system could allow quantum sensing to find even broader scope in the future. By investigating the link between host material properties and the suitability of a quantum sensor for given applications, this thesis provides a unique perspective on the future of the field, which will likely demand more highly specialised and varied sensors.
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    Principles and applications of quantum decoherence in biological, chemical, and condensed matter systems
    Hall, Liam Terres ( 2013)
    This thesis focuses on the use of the Nitrogen-Vacancy (NV) defect centre in diamond as a single spin sensor of nanoscale magnetic fields. The NV system has attracted considerable interest in recent years due to its unique combination of sensitivity, nanoscale resolution, room temperature operation, and stable fluorescence, together with the inherent biocompatibility of diamond; making it ideal for measuring coherent quantum processes in biological, chemical and condensed matter systems. Existing NV-based sensing techniques, however, are ultimately limited by sources of magnetic noise that act to destroy the very resource required for their operation: the quantum phase coherence between NV spin levels. We address this problem by showing that this noise is a rich source of information about the dynamics of the environment we wish to measure. We develop protocols by which to extract dynamical environmental parameters from decoherence measurements of the NV spin, and a detailed experimental verification is conducted using diamond nanocrystals immersed in a MnCl2 electrolyte. We then detail how sensitivities can be improved by employing sophisticated dynamic decoupling techniques to remove the decoherence effects of the intrinsic noise, whilst preserving that of the target sample. To characterise the effects of pulse errors, we describe the full coherent evolution of the NV spin under pulse-based microwave control, including microwave driven and free precession intervals. This analysis explains the origin of many experimental artifacts overlooked in the literature, and is applied to three experimentally relevant cases, demonstrating remarkable agreement between theoretical and experimental results. We then analyse and discuss two important future applications of decoherence sensing to biological imaging. The first involves using a single NV centre in close proximity to an ion channel in a cell membrane to monitor its switch-on/switch-off activity. This technique is expected to have wide ranging implications for nanoscale biology and drug discovery. The second involves using an array of NV centres to image neuronal network dynamics. This technique is expected to yield significant insight into the way information is processed in the brain. In both cases, we find the temporal resolution to be of millisecond timescales, effectively allowing for real time imaging of these systems with micrometre spatial resolution. We analyse cases in which environmental frequencies are sufficiently high to result in a mutual exchange of energy with the NV spin, and discuss how this may be used to reconstruct the corresponding frequency spectrum. This analysis is then applied to two ground-breaking experiments, showing remarkable agreement. Protocols for in-situ monitoring of mobile nanodiamonds in biological systems are developed. In addition to obtaining information about the local magnetic environment, these protocols allow for the determination of both the position and orientation of the nanocrystal, yielding information about the mechanical forces to which it is subjected. These techniques are applied in analysing a set of experiments in which diamond nanocrystals are taken up endosomally by human cervical cancer cells. Finally, we focus our attention on understanding the microscopic dynamics of the spin bath and its effect on the NV spin. Many existing analytic approaches are based on simplified phenomenological models in which it is difficult to capture the complex physics associated with this system. Conversely, numerical approaches reproduce this complex behaviour, but are limited in the amount of theoretical insight they can provide. Using a systematic approach based on the spatial statistics of the spin bath constituents, we develop a purely analytic theory for the NV central spin decoherence problem that reproduces the experimental and numerical results found in the literature, whilst correcting the limitations and inaccuracies associated with existing analytical approaches.
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    Nanoscale quantum sensing using nitrogen-vacancy centres in diamond
    McGuinness, Liam Paul ( 2012)
    Devices that detect and spatially image magnetic fields are important in many areas of study including chemistry, electronics, materials science and biology. By extending the boundaries of what is currently achievable we may begin to explore areas previously inaccessible to science, such as wide-field imaging of neuron signaling or structural determination of single molecules. Here we present experimental progress towards the development of a nanoscale magnetic sensor operating under ambient conditions using the nitrogen-vacancy (NV) centre in diamond. This thesis describes the construction of a lab-built, confocal microscope capable of detecting single NV centres, with additional microwave control for coherent manipulation of the NV spin. The feasibility of using NV-diamond for real-time detection of the action potential generated by a neuron, and with high spatial resolution is experimentally demonstrated. The quantum coherence of single NV spins is monitored in various chemical solutions, and detection of nanoscale magnetic environments external to the diamond are demonstrated. This work sets the experimental foundation for using manufactured single quantum systems as sensitive probes of external chemical environments. In addition, the first measurements of single quantum coherent spins inside living cells are performed with NV centres in nanodiamonds. These studies on NV centres inside living cells demonstrate their promise as magnetic sensors for biology. Furthermore, alternative quantum sensing technologies emerge including rotational tracking of nanodiamonds and enhanced identification of fluorescent nanoparticles.
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    From geometric phases to intracellular sensing: new applications of the diamond nitrogen-vacancy centre
    MACLAURIN, DOUGAL ( 2010)
    This thesis consists of two parts, each of which proposes a new application of the diamond nitrogen-vacancy (NV) centre. We first consider the NV centre as a device to detect geometric phases. We show that the Aharonov-Casher phase and Berry’s phase may be produced in the NV centre’s spin sublevels and observed using existing experimental techniques. We give the background theory to geometric phases, then show how these phases apply to the NV system. Finally, we outline a number of realistic experiments to detect these phases. The second part considers the behaviour of an NV centre within a diamond nanocrystal which rotates, in a Brownian sense, in a fluid. Our aim is to understand the effect of rotational motion on the initialisation, evolution and readout of an NV centre, motivated by the idea of using colloidal nanodiamonds for biological imaging. We first develop a model to describe the quantum evolution of a rotationally diffusing nanocrystal. The model uses theory developed in NV magnetometry and also the geometric phase theory developed in the first part of this thesis. We then explore the consequences of this model for nanoscale sensing. We show that the tumbling NV system may be used as a sensitive magnetometer with nanoscale resolution and also as a probe of its own rotational motion.