It is my hope that this thesis may serve as a guide for future students wishing to build a microscope from scratch. The design and construction of a scanning, confocal fluorescence microscope equipped with shaped microwave excitation is detailed. The use of the microscope is demonstrated by coherently manipulating single Nitrogen-Vacancy centres in diamond. Further the instrument is used to investigate a dual Halbach array magnet system.

Kyoto University (京都大学) / 0048 / 新制・課程博士 / 博士(工学) / 甲第19002号 / 工博第4044号 / 新制||工||1622 / 31953 / 京都大学大学院工学研究科分子工学専攻 / (主査)教授 白川 昌宏, 教授 田中 庸裕, 教授 濵地 格 / 学位規則第4条第1項該当

Recently, developments in novel and high-purity materials allow for the presence of a single, solitary crystalline defect to define the electronic, magnetic, and optical functionality of a device. The discrete nature of the active dopant, whose properties are defined by a quantum mechanical description of its structure, enables radically new quantum investigations and applications in these arenas. Finally,there has been significant development in large-scale device engineering due to mature semiconductor manufacturing techniques. The diverse set of photonic device architectures offering light confinement, guiding, and extraction is a prime example. These three paradigms – solitary dopant photonics and optoelectronics (solotronics), quantum science and technology, and device engineering – merge in the development of novel quantum photonic devices for the next generation of information processing systems. We present in this thesis a series of investigations of optical nanostructures for single optically active spins in single crystal diamond. Chapter 1 introduces the Nitrogen-Vacancy (NV) color center, summarizes its applications, and motivates the need for their integration into photonic structures. Chapter 2 describes two prototype nanobeam photonic crystal cavities for generating strong light-matter interactions with NV centers. The first device consists of a silicon nitride photonic crystal nanobeam cavity with high quality factor \(Q \sim 10^5\) and small mode volume \(V \sim 0.5*(\lambda/n)^3\). The second device consists of a monolithic diamond nanobeam cavity fabricated with the focused ion beam (FIB) directly in a single crystal diamond sample. Chapter 3 presents a high-efficiency source of single photons consisting of a single NV center in a photonic diamond nanowire. Early FIB prototypes are described, as is the first successful realization of the device achieved via reactive ion etching nanowires in a single crystal diamond containing NV centers, and finally a variation of this approach based on incorporation of NV centers in pure diamond via ion implantation. In chapter 4 we consider the optimal design of photonic devices offering both collection efficiency and cavity-enhancements and extend the model of the NV center to include photonic effects. In chapter 5 we briefly introduce a novel optically active spin discovered in a diamond nanowire. Finally, in chapter 6 we conclude with several proposals to extend this research program. / Engineering and Applied Sciences

Magnetic imaging has been playing central roles not only in fundamental sciences but also in engineering and industry. Their numerous applications can be found in various areas, ranging from chemical analysis and biomedical imaging to magnetic data storage technology. An outstanding problem is to develope new magnetic imaging techniques with improved spatial resolutions down to nanoscale, while maintaining their magnetic sensitivities. For instance, if detecting individual electron or nuclear spins with nanomter spatial resolution is possible, it would allow for direct imaging of chemical structures of complex molecules, which then could bring termendous impacts on biological sciences. While realization of such nanoscale magnetic imaging still remains challenging, nitrogen-vacancy (NV) defects in diamond have recently considered as promising magnetic field sensors, as their electron spins show exceptionally long coherence even at room temperature. This thesis presents experimental progress in realizing a nanoscale magnetic imaging apparatus with a single nitrogen-vacancy (NV) color center diamond. We first fabricated diamond nanopillar devices hosting single NV centers at their ends, and incorporated them to a custom-built atomic force microscope (AFM). Our devices showed unprecedented combination of magnetic field sensitivity and spatial resolution for scanning NV systems. We then used these devices to magnetically image a single isolated electronic spin with nanometer resolution, for the first time under ambient condition. We also extended our study to improve and generalize the application of the scanning NV magnetometer we developed. We first introduced magnetic field gradients from a strongly magnetized tip, and demonstrated that the spatial resolution can be further improved by spectrally distinguishing identical spins at different locations. In addition, we developed a method to synchronize the periodic motion of an AFM tip and pulsed microwave sequences controlling an NV spin. This scheme enabled employment of 'AC magnetic field sensing scheme' in imaging samples with static and spatially varying magnetizations. / Engineering and Applied Sciences

Quantum mechanics, arguably one of the greatest achievements of modern physics, has not only fundamentally changed our understanding of nature but is also taking an ever increasing role in engineering. Today, the control of quantum systems has already had a far-reaching impact on time and frequency metrology. By gaining further control over a large variety of different quantum systems, many potential applications are emerging. Those applications range from the development of quantum sensors and new quantum metrological approaches to the realization of quantum information processors and quantum networks. Unfortunately most quantum systems are very fragile objects that require tremendous experimental effort to avoid dephasing. Being able to control the interaction between a quantum system with its local environment embodies therefore an important aspect for application and hence is at the focus of this thesis. / Physics

Nuclear magnetic resonance (NMR) spectroscopy and magnetic resonance imaging (MRI) are techniques widely utilized by many scientific fields, but their applications are often limited by short spin relaxation times and low sensitivity. This thesis explores two novel forms of NMR addressing these issues: nuclear spin singlet states for extending spin polarization lifetime and nitrogen-vacancy centers for sensing small samples. / Chemistry and Chemical Biology

It is my hope that this thesis may serve as a guide for future students wishing to build a microscope from scratch. The design and construction of a scanning, confocal fluorescence microscope equipped with shaped microwave excitation is detailed. The use of the microscope is demonstrated by coherently manipulating single Nitrogen-Vacancy centres in diamond. Further the instrument is used to investigate a dual Halbach array magnet system.

<div>Optical signals are a necessary tool for quantum technologies to carry information both for long-range and on-chip application. The scope of their use is determined by their ability to effectively interact with qubits. The deep-subwavelength interaction volume demands the understanding of the properties of optical fields in the near-field and light-matter interaction in this regime. Recent studies have unraveled the rich characteristics in the physical quantity known as the near-field photonic spin density (PSD). Photonic spin density is the spatial distribution of light's spin angular momentum. It is characterized by the degree of circular polarization of an optical field in deep-subwavelength volumes. In this thesis we study the properties of PSD in the near-field regime and demonstrate a platform for coherent light-spin-qubit interaction based on PSD. We show that nitrogen-vacancy (NV) centers in diamond can coherently interact with an optical beam where the interaction strength is determined by PSD in the nanoscale. To understand the near-field characteristics of PSD we study the evanescent waves and spin-momentum locking of light.</div><div><br></div><div>Evanescent electromagnetic waves possess spin-momentum locking, where the direction of propagation (momentum) is locked to the inherent polarization of the wave (transverse spin). We study the optical forces arising from this universal phenomenon and show that the fundamental origin of recently reported optical chiral forces is spin-momentum locking. For evanescent waves, we show that the direction of energy flow, direction of decay, and direction of spin follow a right hand rule for three different cases of total internal reflection, surface plasmon polaritons, and HE₁₁ mode of an optical fiber.</div><div>Furthermore, we explain how the recently reported phenomena of lateral optical force on chiral and achiral particles is caused by the transverse spin of the evanescent field and the spin-momentum locking phenomenon. Our work presents a unified view on spin-momentum locking and how it affects optical forces on chiral and achiral particles. </div><div><br></div><div>To probe the near-field properties of PSD, we propose and employ a single NV center in diamond as a nanoscale sensor. NV centers have emerged as promising room-temperature quantum sensors for probing condensed matter phenomena ranging from spin liquids, two-dimensional (2D) magnetic materials, and magnons to hydrodynamic flow of current. Here, we demonstrate that the NV center in diamond can be used as a quantum sensor for detecting the photonic spin density. We exploit a single spin qubit on an atomic force microscope tip to probe the spinning field of an incident Gaussian light beam. The spinning field of light induces an effective static magnetic field in the single spin qubit probe. We perform room-temperature sensing using Bloch sphere operations driven by a microwave field (XY8 protocol). This nanoscale quantum magnetometer can measure the local polarization of light in ultra-sub-wavelength volumes. We also put forth a rigorous theory of the experimentally measured phase change using the NV center Hamiltonian and perturbation theory involving only virtual photon transitions. </div><div><br></div><div>In order to study the wavelength dependence of the optically induced magnetic field, we demonstrate this effect for an ensemble of NV centers. We characterize the wavelength dependence of the effective static magnetic field caused by the interaction of PSD and the spin qubit. We show that the strength of the field is inversely dependent on the detuning between the frequency of the optical beam and the optical transition of the NV centers. We show an optically induced rotation of over 10 degrees in the spin qubit of NV centers at room temperature. The direct detection of the photonic spin density at the nanoscale using NV centers in diamond opens interesting quantum metrological avenues for studying exotic phases of photons, nanoscale properties of structured light as well as future on-chip applications. </div><div><br></div>

We propose an original analog method to perform instantaneous and quantitative spectral analysis of microwave signals. An ensemble of nitrogen-vacancy (NV) centers held in a diamond plate is pumped by a 532 nm laser. Its photoluminescence is imaged through an optical microscope and monitored by a digital camera. An incoming microwave signal is converted into a microwave field in the area of the NV centers by a loop shaped antenna. The resonances induced by the magnetic component of that field are detected through a decrease of the NV centers photoluminescence. A magnetic field gradient induces a Zeeman shift of the resonances and transforms the frequency information into spatial information, which allows for the simultaneous analysis of the microwave signal in the entire frequency bandwidth of the device. The time dependent spectral analysis of an amplitude modulated microwave signal is demonstrated over a bandwidth of 600 MHz, associated to a frequency resolution of 7MHz , and a refresh rate of 4 ms. With such integration time, a field of a few hundreds of lW can be detected. Since the optical properties of NV centers can be maintained even in high magnetic field, we estimate that an optimized device could allow frequency analysis in a range of 30 GHz, only limited by the amplitude of the magnetic field gradient. In addition, an increase of the NV centers quantity could lead both to an increase of the microwave sensitivity and to a decrease of the minimum refresh rate down to a few ls.

We present the controlled creation of single nitrogen-vacancy (NV) centers via ion implantation at the center of a photonic crystal cavity which is fabricated in an ultrapure, single crystal diamond membrane. High-resolution placement of NV centers is achieved using collimation of a 5 keV-nitrogen ion beam through a pierced tip of an atomic force microscope. We demonstrate coupling of the implanted NV centers’ broad band fluorescence to a cavity mode and observe Purcell enhancement of the spontaneous emission. The results are in good agreement with a master equation model for the cavity coupling.