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.
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.
This thesis describes a series of experiments on the control of the optical properties of the nitrogen-vacancy (NV) center in diamond, and on control of the electron and nuclear spin states associated with the NV center. The NV center is a fluorescing atomic defect center in diamond, consisting of a substitutional nitrogen atom adjacent to a vacancy in the diamond carbon lattice. The electron spin of the NV center can be initialized and read out optically, and coherently manipulated with high fidelity even at room temperature. This unique combination of properties has attracted much attention to the NV center in recent years for application in quantum information technologies. The experiments in this work focus on exploiting the intrinsic hybrid nature of the NV center. The NV center forms a hybrid spin register, as its electron spin is always coupled to the nuclear spin of its own nitrogen nucleus, and can furthermore be coupled to additional nuclear carbon-13 spins in the diamond. In addition, the electronic spin state can be mapped onto the state of a photon, in principle allowing long range transmission of quantum information and measurement-based entanglement of distant NV center registers. The long-term goal is to achieve a large scale quantum network where the different constituents each perform the task they are most well suited for: the stable nuclear spins store the quantum information, photons transfer quantum information over long distances, and the fast electron spin interfaces between spin and photon states. For measurement-based entanglement of distant NV centers it is of primary importance to maximize the emission and detection of coherent photons emitted by the NV center. Spontaneous emission can be controlled and enhanced by coupling an emitter to a photonic cavity. Chapters 3, 4, and 5 of this thesis describe experiments aimed at maximizing the coherent photon emission rate of an NV center by coupling the NV center to a photonic crystal cavity. One of the main challenges is to position a single NV center into the nanometer-sized cavity mode. Chapter 3 describes the development of a nanopositioning technique, which allows diamond nanocrystals ~50 nm in size containing single NV centers to be placed at arbitrary locations on a chip, with nanometer precision. By using a sharp etched tungsten tip, individual nanocrystals can be picked up, moved and placed under real-time imaging with an electron microscope. We explicitly demonstrate that the unique optical and spin properties of the NV center are conserved by the nanopositioning process. In chapter 4, we apply the nanopositioning technique to couple single NV centers contained in a diamond nanocrystals to gallium phosphide photonic crystal cavities. These cavities resonate in the visible with high quality factors, and are designed to have the lowest energy mode coincide with the zero-phonon line of the NV center. Efficient coupling is evidenced by a strong enhancement of NV center emission at the cavity wavelength. The high quality factor of a photonic crystal cavity is a result of careful design and fabrication. The introduction of a nanocrystal may therefore be expected to have a detrimental effect on the optical properties of a cavity. In chapter 5 we investigate the effect of a nanocrystal on the optical properties of photonic crystal cavities. Our simulations and measurements show that the effect of a nanocrystal is in fact only minor, a promising result for future work on cavity-QED systems in the solid state and with diamond defect centers in particular. Understanding and mitigating decoherence is a key challenge for quantum science and technology. The main source of decoherence for solid-state spin systems is the uncontrolled spin bath environment. Chapter 6 describes experiments that exploit quantum control of the NV center and recently developed dynamical decoupling techniques to study the properties of the surrounding bath of spins belonging to single substitutional nitrogen atoms. The coherence properties of a single NV center are affected by changes in the state of the bath spins, allowing a single NV center to be used as a probe to detect bath spin resonances and study the quantum dynamics of the spin bath. We use quantum control of the spin bath to extend the dephasing time of the NV center, important for the application of the NV center in DC magnetometry. In chapter 7 we describe the development and implementation of decoherence protected quantum gates for the hybrid spin register formed by the NV center electron spin that is coupled to the nuclear spin of its own nitrogen atom. Electron and nuclear spins evolve and decohere at vastly different rates, making it challenging to use such a hybrid system as a fully functional quantum register. We create a universal set of two-qubit quantum gates by integrating dynamical decoupling techniques into the gate operation. We demonstrate the power of our gate design by implementing for the first time Grover's quantum search algorithm on a solid-state spin register.
The NV defect center in diamond forms a pseudo-atomic quantum system with discreet optically excitable transitions between ground and excited states in the gap between valence and conduction bands, making the NV center a deep-level defect center in diamond. For the negatively charged NV center (NV-), both the ground and excited states are spin triplets (S=1) and coupling between optical and spin states provides unique opportunities for optical detection of magnetic resonance (ODMR) and quantum metrology under ambient conditions. As an atomically sized point defect that is stable in single nanodiamonds as small as a few nanometers, the NV center enables spin based imaging of temperature, electric fields, magnetic fields and mechanical strain with nanoscale spatial resolution. Made of carbon, nanodiamonds are also ideal nanoparticles for use in biological systems, exhibiting extremely low cytotoxicity, no photo bleaching and exceptional contrast in transmission electron and light microscopy. With the ability to act as both a passive, non perturbing sensor (e.g. a diamagnetic material used for sensing magnetic fields) and a connection point for two way, direct coupling of far field optics to NV− spins and indirectly to the highly localized neighborhood of atoms, electronic states and phonon modes in the local vicinity, NV diamond provides a route to nanoscale field sensing and spin based optical microscopy. These sensors are also stable in nanodiamonds. For nanoparticles, the reduction in particle diameter dramatically enhances the proportion of the material that is surface exposed, enhancing any surface related properties. Nitrogen Vacancy centers in nanodiamonds provide another example of material properties that vary with particle size. In chapter 5, evidence that modulation of nanodiamonds fluorescent emissions by electrical perturbations in their surrouding environment allows transduction of local electrodynamics into a far field optical signal capable of mapping action potentials in cardiomyocytes in presented. The unifying theme for all of the work presented in this dissertation is to enable the use of magnetic resonance signals and interactions for imaging and sensing in previously inaccessible regimes. The specific focus is on methods and techniques to enable nanoscale physical sensing and functional imaging in live tissues, with the ultimate aim to lay the predicate for the combination of both without compromise.
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.
In this thesis, quantum states of single spin systems in solid state are investigated for potential applications in quantum information processing. The studied system is the nitrogen-vacancy defect in diamond, which can be thought of as a molecule trapped inside the diamond crystal. An issue for high-fidelity state preparation is the intitialization of the system. The photo-induced charge state dynamics of the nitrogen-vacancy defect is determined, and methods for charge state initialization are beeing developed. The electron spin state of single nitrogen-vacancy defects can be read out optically. Here, we focus on nearby nuclear spins coupled to the electron spin. We investigate the quantum evolution of a single nuclear spin, measurement of non-orthogonal quantum states and improved magnetic field sensing. Based on three nuclear spins, a small quantum register is realized. We prepare and measure the GHZ and the W state in this register, and implement an algorithm for quantum error correction.
Nitrogen-vacancy centers in diamond are sensitive probes of time-varying magnetic fields that can be used to identify unknown spin defects in their nearby environment. Performing spectral quantum measurements on such single quantum probes enables gaining information about the internal structure and dynamics of nearby spin defects that would otherwise be inaccessible through direct or indirect measurements with classical probes. Here, we identify a system composed of two electron-nuclear spin defects in a diamond crystal by performing a series of spectral identification measurements using a single nitrogen-vacancy center in diamond. Besides enabling the identification of new spin defects and studies of their formation mechanisms, these techniques will be useful for scaling up quantum systems by converting environmental spin defects into quantum resources.
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.