Abstract Hybrid quantum devices, in which disparate quantum elements are combined in order to achieve enhanced functionality, have received much attention in recent years due to their exciting potential to address key problems in quantum information processing, communication, and control. Specifically, significant progress has been made in the field of hybrid mechanical devices, in which a qubit is coupled to a mechanical oscillator. High cooperativity in such devices has been demonstrated with superconducting qubits, and coupling defect qubits to mechanical elements via crystal strain has enabled novel methods of qubit measurement and control. In this paper we demonstrate the fabrication of diamond optomechanical crystals (OMCs) with embedded nitrogen-vacancy (NV) centers, a preliminary step toward reaching the quantum regime with defect qubit hybrid mechanical devices. We measure optical and mechanical resonances of diamond OMCs as well as the spin coherence of single embedded NV centers. We find that the spin has long coherence times T 2 * = 1.5 μ s and T 2 = 72 μ s despite its proximity to nanofabricated surfaces. Finally, we discuss potential improvements of these devices and prospects for future experiments in the quantum regime.
A fully functional quantum computer must contain at least two important components: a quantum memory for storing and manipulating quantum information and a quantum data bus to securely transfer information between quantum memories. Typically, a quantum memory is composed of a matter system, such as an atom or an electron spin, due to their prolonged quantum coherence. Alternatively, a quantum data bus is typically composed of some propagating degree of freedom, such as a photon, which can retain quantum information over long distances. Therefore, a quantum computer will likely be a hybrid quantum device, consisting of two or more disparate quantum systems. However, there must be a reliable and controllable quantum interface between the memory and bus in order to faithfully interconvert quantum information. The current engineering challenge for quantum computers is scaling the device to large numbers of controllable quantum systems, which will ultimately depend on the choice of the quantum elements and interfaces utilized in the device. In this thesis, we present and characterize a hybrid quantum device comprised of single nitrogen-vacancy (NV) centers embedded in a high quality factor diamond mechanical oscillator. The electron spin of the NV center is a leading candidate for the realization of a quantum memory due to its exceptional quantum coherence times. On the other hand, mechanical oscillators are highly sensitive to a wide variety of external forces, and have the potential to serve as a long-range quantum bus between quantum systems of disparate energy scales. These two elements are interfaced through crystal strain generated by vibrations of the mechanical oscillator. Importantly, a strain interface allows for a scalable architecture, and furthermore, opens the door to integration into a larger quantum network through coupling to an optical interface.There are a few important engineering challenges associated with this device. First, there have been no previous demonstrations of a strain-mediated spin-mechanical interface and hence the system is largely uncharacterized. Second, fabricating high quality diamond mechanical oscillators is difficult due to the robust and chemically inert nature of diamond. Finally, engineering highly coherent NV centers with a coherent optical interface in nanostructured diamond remains an outstanding challenge. In this thesis, we theoretically and experimentally address each of these challenges, and show that with future improvements, this device is suitable for future quantum-enabled applications. First, we theoretically and experimentally demonstrate a dynamic, strain-mediated coupling between the spin and orbital degrees of freedom of the NV center and the driven mechanical motion of a single-crystal diamond cantilever. We employ Ramsey interferometry to demonstrate coherent, mechanical driving of the NV spin evolution. Using this interferometry technique, we present the first demonstration of nanoscale strain imaging, and quantitatively characterize the previously unknown spin-strain coupling constants. Next, we use the driven motion of the cantilever to perform deterministic control of the frequency and polarization dependence of the optical transitions of the NV center. Importantly, this experiment constitutes the first demonstration of on-chip control of both the frequency and polarization state of a single photon produced by a quantum emitter. In the final experiment, we use mechanical driving to engineer a series of spin ``clock" states and demonstrate a significant increase in the spin coherence time of the NV center. We conclude this thesis with a theoretical discussion of prospective applications for this device, including generation of non-classical mechanical states and spin-spin entanglement, as well as an evaluation of the current limitations of our devices, including a possible avenues for improvement to reach the regime of strong spin-phonon coupling.
Trapping of a nanodiamond/microdiamond containing Nitrogen-Vacancy centers in the vacuum is an ideal platform to develop a hybrid mechanical system. In such a system, the coupling between the Nitrogen-Vacancy centers and the mechanical motion of a trapped diamond provides pathways for generating a quantum superposition state of the mechanical motion with long coherence time. In this work, I demonstrate our preliminary data in the detection of Nitrogen-Vacancy spin signals from trapped diamonds using optical and magneto-gravitational trapping technologies. I compared the advantages and drawbacks of both techniques and improvements need to be made. I also explored the charge dynamics of Nitrogen-Vacancy centers in diamonds under near-IR laser illumination and first demonstrate low energy (0.95 to 1.18 eV or 1050 to 1300 nm) Multi-photon Photoluminescence Excitation (PLE) spectrum of NV centers in a sub-millimeter diamond crystal.
Defect based qubit systems like the nitrogen vacancy center in diamond have recently emerged as promising candidates for quantum technologies due to their combination of long coherence times, room temperature operation, and robust optical interface. In order to realize many of their proposed applications, defect qubits must be incorporated into scalable devices architectures consisting of photonic, mechanical, or electrical degrees of freedom. Despite much recent progress, many challenges remain for diamond growth and device fabrication. As an alternate approach, we engaged in a search for nitrogen vacancy center analogues in alternative materials with the hope of obtaining a greater degree of control over defect and material properties. Ultimately, we discovered that divacancy-related point defects in all three of the most common forms of silicon carbide- termed 4H, 6H, and 3C- act as analogues to the nitrogen vacancy center in diamond. We chose to focus our research primarily on defects in 3C silicon carbide (termed 'Ky5' defects) because of its availability as a single crystal heteroepitaxial thin film grown on silicon, an advantage that greatly facilitates the fabrication of functional devices. We characterized the spin and optical properties of Ky5 defects in thin film geometries and observed many similarities to the nitrogen vacancy center. We performed the first measurements of spin dynamics in 3C silicon carbide and demonstrate coherent control of defect spins up to room temperature and observe coherence times of up to 22 microseconds. To demonstrate their use in real devices, we designed, fabricated, and characterized photonic crystal cavities in 3C silicon carbide thin films with mode volumes of less than (lambda/n)^3 and Q's as high as 1,500 with integrated Ky5 defects. Additionally, we performed simulations and analysis of the fabricated structures using observed structural imperfections to determine that the Q's are likely limited primarily by the non-vertical structure sidewall angle. Despite the modest Q's of these structures, they can be utilized to generate large local field intensities to enhance optical interactions with Ky5 qubit states within the cavities. We accomplish this by performing cavity enhanced photoluminescence excitation spectroscopy on cavity modes tuned to the zero phonon line of the defects and observe large (as high as 30 times) increases in the luminescence and optically detected magnetic resonance signals originating from the defect states and approximately 2x faster rates of ground state spin initialization. In addition, we use these techniques to probe the photoluminescence dynamics of the Ky5 defects' optical pumping cycle, perform excitation wavelength dependent studies of spin and spectral inhomogeneity, and use the small mode volume and narrowband photoluminescence enhancements of the cavities to observe spectrally distinct subensembles of defects with linewidths as narrow as 25 GHz within the inhomogeneously broadened zero phonon line. Although much is still unknown regarding the properties of these defects, they show great promise as a candidate system for defect qubit based quantum devices and technologies.
Silicon has turned from a niche laboratory-scale material into the backbone of modern electronics. Diamond functionalized with color centers could follow a similar path and grow from proof-of-concepts experiments to application-oriented quantum technologies. Quantum sensing, communication, and information processing with color centers has been proven to work in scientific experiments and enhanced sensitivities as well as novel functionalities have been reported. While the first generation of diamond quantum devices relied on color centers formed uncontrolled in natural diamond with a high statistical variation in composition and crystallinity, the situation has changed nowadays. With the emergence of high purity monocrystals and the option for isotopic purification of the carbon matrix, technological progress in materials science on the atomic-scale enabled tailoring the spin properties in diamond. But, since many color centers typically require vacancies to combine with impurities in the carbon lattice via diffusion, the generation of color centers underlies a statistical process providing only little control on the center's final position in the crystal lattice. The negatively charged nitrogen-vacancy (NV
−) center is the most studied optically active defect in diamond and exhibits remarkable spin properties and sensing capabilities, even on the nanoscale and at room temperature. The spin properties of NV
− centers close to the surface (1\,nm - 30\,nm) have been thoroughly studied and the deeper the spins are located in diamond the less decoherence from surface defects is observed. Creating NV
− centers at the surface by nitrogen ion implantation and burying them beneath a thin diamond layer via chemical vapor deposition (CVD) of diamond is reported to enhance the coherence times significantly. By separating the color center generation from controlling the resulting depth by an additional diamond layer, narrow depth profiles can be achieved by reducing the ion energy during implantation. Although the coherence properties improve, many of the implanted NV
− center are reported to vanish in the hydrogen-rich plasma of growth CVD chambers. The mechanism responsible for the instability of NV
− centers towards the plasma remains unclear, though. One hypothesis is the formation of nitrogen-vacancy-hydrogen centers from diffusing hydrogen and implanted NV
− centers but is has not been proven, yet. Here, we demonstrate the fabrication of depth confined NV
− centers by combining low energy (1\,keV - 5\,keV) ion implantation and CVD overgrowth. By increasing the thickness of the overgrown layer (6\,nm - 100\,nm) the influence of surface noise is shown to decrease leading to bulk-like coherence properties of up to $450\,\upmu$s (Hahn-echo) and
T2∗ dephasing times around $20\,\upmu$s. Monitoring the NV
− density as a function of the overgrowth time, we analyze the kinetics of the passivation in case of implanting ion doses of 10
11 15N
+/cm
2 and 10
12 15N
+/cm
2. The passivation turns out to occur faster for lower doses offering insights into sub-surface hydrogen diffusion in diamond. Analyzing the spin bath before and after overgrowth reveals a drastic reduction in paramagnetic spins after the CVD process but no NVH
− is found around the surviving NV
− centers. Checking the chemical composition in overgrown implantation sites with secondary-ion-mass-specrometry (SIMS), however, confirms significant amounts of hydrogen in the
15N-implanted layers. Since the concentration found for hydrogen exceeds the one for nitrogen by far, we suggest that diffusing hydrogen interacts also with vacancies forming probably mostly diamagnetic defects. In the last part of this dissertation, NV
− centers are generated with sub-nanometer precision below a thin
13C-enriched layer for quantum simulation. For fabricating the spin architecture starting from a
12C base layer, we overgrow implanted nitrogen with a
13C layer and bury the spins beneath a 30\,nm-thick
12C capping layer. By measuring the coupling strength between the electron and nuclear spins, we deduce a NV
− placement accuracy reaching below one nanometer with respect to the
13C-layer. Regarding the spin properties of the electron spins, no reduction in
T2 is observed despite of the proximity to the dense
13C-bath. As a consequence, the overgrowth of NV
− centers is demonstrated as a bottom-up approach to produce buried spin architectures with sharp isotopic transitions and efficient
13C-NV
− coupling. Together with the potential for bulk-like coherence properties the synergy of implantation and overgrowth is a powerful tool to fabricate reproducible quantum systems with tailored properties and high depth confinement.
Nitrogen-vacancy (NV) centers in diamond have recently emerged as a unique platform for fundamental studies in quantum information and nanoscience. The special properties of these impurity centers allow robust, room-temperature operation of solid-state qubits and have enabled several remarkable demonstrations in quantum information processing and precision nanoscale sensing. This article reviews the recent advances in magnetic and optical manipulation of the NV center’s quantum spin and their importance for prospective applications. We discuss how quantum control of individual centers can be harnessed for the protection of NV-center spin coherence, for multiqubit quantum operations in the presence of decoherence, and for high-fidelity initialization and readout. We also discuss the progress in resonant optical control, which has led to interfaces between spin and photonic qubits and may lead to spin networks based on diamond photonics. Many of these recently developed diamond-based technologies constitute critical components for the future leap toward practical multiqubit devices.