Nanostructures are promising building blocks for quantum technologies due to their reproducible nature and ability to self-assemble into complex structures. However, the need to control these nanostructures represents a key challenge. Hence, this thesis investigates the manipulation and creation of quantum states in certain nanostructures. The results of this thesis can be applied to quantum information processing and to extremely sensitive magnetic-field measurements.In the first research chapter, we propose and examine methods for entangling two (remote) nuclear spins through their mutual coupling to a transient optically excited electron spin. From our calculations we identify the specific molecular properties that permit high entangling power gates for different protocols.In the next research chapter, we investigate another method to create entanglement; this time between two remote electronic spins. This method uses a very sensitive magnetic-field sensor based on a crystal defect that allows the detection of single magnetic moments. The act of sensing the local field constitutes a two-qubit projective measurement. This entangling operation is remarkably robust to imperfections occurring in an experiment.The third research chapter presents an augmented sensor consisting of a nitrogen-vacancy centre for readout and an `amplifier' spin system that directly senses tiny local magnetic fields. Our calculations show that this hybrid structure has the potential to detect magnetic moments with a sensitivity and spatial resolution far beyond that of a sensor based on only a nitrogen-vacancy centre, and indeed this may be the physical limit for sensors of this class.Finally, the last research chapter investigates measurements of magnetic-field strength using an ensemble of spin-active molecules. Here, we describe a quantum strategy that can beat the common standard strategy. We identify the conditions for which this is possible and find that this crucially depends on the decoherence present in the system.
Nanostructures are promising building blocks for quantum technologies due to their reproducible nature and ability to self-assemble into complex structures. However, the need to control these nanostructures represents a key challenge. Hence, this thesis investigates the manipulation and creation of quantum states in certain nanostructures. The results of this thesis can be applied to quantum information processing and to extremely sensitive magnetic-field measurements.In the first research chapter, we propose and examine methods for entangling two (remote) nuclear spins through their mutual coupling to a transient optically excited electron spin. From our calculations we identify the specific molecular properties that permit high entangling power gates for different protocols.In the next research chapter, we investigate another method to create entanglement; this time between two remote electronic spins. This method uses a very sensitive magnetic-field sensor based on a crystal defect that allows the detection of single magnetic moments. The act of sensing the local field constitutes a two-qubit projective measurement. This entangling operation is remarkably robust to imperfections occurring in an experiment.The third research chapter presents an augmented sensor consisting of a nitrogen-vacancy centre for readout and an `amplifier' spin system that directly senses tiny local magnetic fields. Our calculations show that this hybrid structure has the potential to detect magnetic moments with a sensitivity and spatial resolution far beyond that of a sensor based on only a nitrogen-vacancy centre, and indeed this may be the physical limit for sensors of this class.Finally, the last research chapter investigates measurements of magnetic-field strength using an ensemble of spin-active molecules. Here, we describe a quantum strategy that can beat the common standard strategy. We identify the conditions for which this is possible and find that this crucially depends on the decoherence present in the system.
Nanostructures are promising building blocks for quantum technologies due to their reproducible nature and ability to self-assemble into complex structures. However, the need to control these nanostructures represents a key challenge. Hence, this thesis investigates the manipulation and creation of quantum states in certain nanostructures. The results of this thesis can be applied to quantum information processing and to extremely sensitive magnetic-field measurements.In the first research chapter, we propose and examine methods for entangling two (remote) nuclear spins through their mutual coupling to a transient optically excited electron spin. From our calculations we identify the specific molecular properties that permit high entangling power gates for different protocols.In the next research chapter, we investigate another method to create entanglement; this time between two remote electronic spins. This method uses a very sensitive magnetic-field sensor based on a crystal defect that allows the detection of single magnetic moments. The act of sensing the local field constitutes a two-qubit projective measurement. This entangling operation is remarkably robust to imperfections occurring in an experiment.The third research chapter presents an augmented sensor consisting of a nitrogen-vacancy centre for readout and an `amplifier' spin system that directly senses tiny local magnetic fields. Our calculations show that this hybrid structure has the potential to detect magnetic moments with a sensitivity and spatial resolution far beyond that of a sensor based on only a nitrogen-vacancy centre, and indeed this may be the physical limit for sensors of this class.Finally, the last research chapter investigates measurements of magnetic-field strength using an ensemble of spin-active molecules. Here, we describe a quantum strategy that can beat the common standard strategy. We identify the conditions for which this is possible and find that this crucially depends on the decoherence present in the system.
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 ability to measure and manipulate the quantum state of a single spin in a solid state system opens up a broad range of powerful applications ranging from nano probes to quantum information processing. Over the past few years, a number of ground breaking experiments have been conducted on paramagnetic nitrogen vacancy defect centers in diamond, including up to 3-qubit entanglement, single-shot-readout of a nuclear spin, selective access of two coupled centers and magnetic, electric and thermographic sensing at the nanoscale with promising properties in some cases exceeding most currently known techniques. Yet, almost all of the experiments conducted so far focus on centers deeply buried in the diamond, which is undesirable especially for sensing applications, but also in terms of scalability and electronic access to the information. In this work we focus on the spin physics of centers only few nanometers below the surface, where the unique properties of the center are strongly influenced by the external environment. We coherently manipulated and detected single spins at ambient temperature by combining optically detected magnetic resonance with single molecule spectroscopy using a confocal microscope. We measured the spin dephasing behavior and the phase relaxation time and examined the primary sources of decoherence. Furthermore, we observed effects of water, atmosphere and paramagnetic molecules on the coherence and readability of spins in nanodiamonds and demonstrated ways to preserve the coherence using external magnetic fields and a number of different dynamic decoupling pulse sequences. In addition, we measured couplings to proximal nuclear spins by continuous wave spectroscopy and to molecules on the surface by double electron electron resonance. Also, we demonstrate execution of the refined Deutsch-Jozsa algorithm on a nitrogen vacancy center in a nanodiamond. Finally, we propose new technological approach for realtime measurements of magnetic fields using a single spin in diamond. In test measurements using external fields and spatially resolved measurements of the field from a magnetic microwire a sensitivity of a few uT / sqrt(Hz) was achieved.
TThis thesis presents works not only to understand the spin degree of freedom present in the nitrogen-vacancy defect in diamond: its internal structure and its relation to its environment, but also to find novel applications of it in metrology. First, a mathematical model is develop to understand how this defect couples to a nuclear spin bath of Carbon 13 which constitutes the main dephasing mechanism in pure natural diamond. Next, we demonstrate the use of this defect to sense external oscillating magnetic fields. The high sensitivity and the small sensing volume achieved when a defect is placed in a nanocrystal of few tents of nanometers in diameter, allows this sensor to detect single electronic spins and even single nuclear spins. This sensitivity, proportional to the signal to noise per readout, can be improve by the help of the environment of this defect. We show that strongly interacting nearby nuclei can enable repetitive readout schemes to improve the signal to noise of the electronic spin signal. We also combine ideas from the microscopy community such as stimulated emission depletion to enable high spatial resolution magnetometry. Finally, we develop a formalism based on group theory to understand the internal structure of defects in solids such as their selection rules and the effect of spin-spin and spin-orbit interactions even when perturbations reduce the symmetry group of the system.
Sensors based on crystal defects, especially nitrogen vacancy (NV) centres in nanodiamond, can achieve detection of single magnetic moments. Here, we show that this exquisite control can be utilized to entangle remote electronic spins for applications in quantum computing; the mobile sensor provides a 'flying' qubit while the act of sensing the local field constitutes a two-qubit projective measurement. Thus, the NV centre mediates entanglement between an array of well-separated (and thus well-controlled) qubits. Our calculations establish that such a device would be remarkably robust against realistic issues such as dephasing, inaccurate timing and both positioning errors and multimodal vibrations in the sensor tip. Interestingly, the fact that this form of flying qubit is readily measurable allows one to convert certain classes of unknown errors into heralded failures, which are relatively easy to deal with using established quantum information processing techniques. We also provide calculations establishing the feasibility of performing a demonstrator experiment with a fixed sensor in the immediate future.
The highly parallel nature of the fundamental principles of quantum mechanics means that certain key resource-intensive tasks --- including searching, code decryption and medical, chemical and material simulations --- can be computed polynomially or even exponentially faster with a quantum computer. In spite of its remarkably fast development, the field of quantum computing is still young, and a large-scale prototype using any one of the candidate quantum bits (or 'qubits') under investigation has yet to be developed. Spin-based qubits in condensed matter systems are excellent candidates. Spins controlled using magnetic resonance have provided the first, most advanced, and highest fidelity experimental demonstrations of quantum algorithms to date. Despite having highly promising control characteristics, most physical ensembles investigated using magnetic resonance are unable to produce entanglement, a critical missing ingredient for a pure-state quantum computer. Quantum objects are said to be entangled if they cannot be described individually: they remain fundamentally linked regardless of their physical separation. Such highly non-classical states can be exploited for a host of quantum technologies including teleportation, metrology, and quantum computation. Here I describe how to experimentally create, control and characterise entangled quantum ensembles using magnetic resonance. I first explore the relationship between entanglement and quantum metrology and demonstrate a sensitivity enhancement over classical resources using molecular sensors controlled with liquid-state nuclear magnetic resonance. I then examine the computational potential of irreversible relaxation processes in combination with traditional reversible magnetic resonance control techniques. I show how irreversible processes can polarise both nuclear and electronic spins, which improves the quality of qubit initialisation. I discuss the process of quantum state tomography, where an arbitrary quantum state can be accurately measured and characterised, including components which go undetected using traditional magnetic resonance techniques. Lastly, I combine the above findings to initialise, create and characterise entanglement between an ensemble of electron and nuclear spin defects in silicon. I further this by generating pseudo-entanglement between an ensemble of nuclear spins mediated by a transient electron spin in a molecular system. These findings help pave the way towards a particular architecture for a scalable, spin-based quantum computer.