Color centers are optically active point defects in semiconductor materials, many of them carrying a spin degree of freedom that couples coherently to emitted photons. This makes them a leading candidate for building quantum computers, networks, and sensors, but realizing that promise depends on the interface between the emitter and light. Color centers must be integrated into nanophotonic structures, such as nanopillars that collect their emission efficiently and optical cavities that couple them to a single mode. This dissertation studies the physics of quantum emitters inside such structures along two complementary threads: the direct cryogenic spectroscopy of color centers integrated into silicon carbide nanostructures, and the study of the physics of many-body cavity quantum electrodynamics (CQED) through simulation on superconducting and trapped-ion quantum hardware. The first thread concerns the nitrogen-vacancy (NV) center in 4H silicon carbide integrated into nanopillars. We show that the sub-wavelength geometry of a nanopillar reshapes the local electromagnetic environment, granting optical access to transitions that selection rules forbid in bulk material: emission from the PL3 divacancy, nearly absent in planar devices, becomes pronounced in nanopillars through a polarization transformation of the excitation field, and the orientation-dependent collection of the pillar resolves the previously ambiguous NV4′ line, establishing nanophotonic integration as a symmetry-sensitive probe of defect structure. We then take up the complementary problem of quantifying how many emitters a device contains, adapting the number-and-brightness technique from fluorescence microscopy to solid-state emitters. This calibration-free method counts dense NV ensembles in silicon carbide nanopillars, a regime beyond the reach of existing optical techniques, and extracts their areal density and formation yield. The second thread turns to many-body cavity QED, in which placing N emitters in a common cavity enhances the light-matter coupling by √N and gives rise to collective effects that are central to strong-coupling applications yet difficult to achieve in solid-state devices based on defects. We realize one such effect on a superconducting circuit, demonstrating photon blockade, the conversion of a coherent drive into a stream of single photons, in a Tavis–Cummings system of N = 1, 2, 3 transmon qubits coupled to a common resonator. To study the open-system dynamics that govern these systems, we digitally simulate the dissipative Tavis–Cummings model on both a superconducting and a trapped-ion processor. Platform-specific compilation and error mitigation yield population dynamics in close agreement with exact solutions, providing a recipe for simulating cavity-emitter systems on contemporary quantum computers. Together, the two threads connect the fabrication and characterization of color-center devices to the many-body cavity-QED physics that will ultimately govern their performance.
Color centers are optically active point defects in semiconductor materials, many of them carrying a spin degree of freedom that couples coherently to emitted photons. This makes them a leading candidate for building quantum computers, networks, and sensors, but realizing that promise depends on the interface between the emitter and light. Color centers must be integrated into nanophotonic structures, such as nanopillars that collect their emission efficiently and optical cavities that couple them to a single mode. This dissertation studies the physics of quantum emitters inside such structures along two complementary threads: the direct cryogenic spectroscopy of color centers integrated into silicon carbide nanostructures, and the study of the physics of many-body cavity quantum electrodynamics (CQED) through simulation on superconducting and trapped-ion quantum hardware. The first thread concerns the nitrogen-vacancy (NV) center in 4H silicon carbide integrated into nanopillars. We show that the sub-wavelength geometry of a nanopillar reshapes the local electromagnetic environment, granting optical access to transitions that selection rules forbid in bulk material: emission from the PL3 divacancy, nearly absent in planar devices, becomes pronounced in nanopillars through a polarization transformation of the excitation field, and the orientation-dependent collection of the pillar resolves the previously ambiguous NV4′ line, establishing nanophotonic integration as a symmetry-sensitive probe of defect structure. We then take up the complementary problem of quantifying how many emitters a device contains, adapting the number-and-brightness technique from fluorescence microscopy to solid-state emitters. This calibration-free method counts dense NV ensembles in silicon carbide nanopillars, a regime beyond the reach of existing optical techniques, and extracts their areal density and formation yield. The second thread turns to many-body cavity QED, in which placing N emitters in a common cavity enhances the light-matter coupling by √N and gives rise to collective effects that are central to strong-coupling applications yet difficult to achieve in solid-state devices based on defects. We realize one such effect on a superconducting circuit, demonstrating photon blockade, the conversion of a coherent drive into a stream of single photons, in a Tavis–Cummings system of N = 1, 2, 3 transmon qubits coupled to a common resonator. To study the open-system dynamics that govern these systems, we digitally simulate the dissipative Tavis–Cummings model on both a superconducting and a trapped-ion processor. Platform-specific compilation and error mitigation yield population dynamics in close agreement with exact solutions, providing a recipe for simulating cavity-emitter systems on contemporary quantum computers. Together, the two threads connect the fabrication and characterization of color-center devices to the many-body cavity-QED physics that will ultimately govern their performance.
Efficient interfaces between optical photons and quantum bits are fundamental building blocks for quantum networks and large-scale quantum computers. We demonstrate an integrated platform for scalable quantum optics based on color centers coupled to diamond nanodevices. First, we incorporate nitrogen-vacancy (NV) centers in diamond into hybrid nanophotonic crystal cavities. Despite our progress towards coupling the NV to cavity photons, we find that the NV-cavity interface is limited by the imperfections of the color center's properties and its local environment. We approach this challenge first by characterizing and modifying the diamond surface to reduce the environmental noise affecting the NV optical transition. Subsequently, we develop a new approach that makes use of a quantum emitter with intrinsic protection from this noise: the silicon-vacancy (SiV) center in diamond. We demonstrate that SiV centers introduced through ion implantation feature highly coherent optical transitions, even inside nanostructures. By placing SiV centers inside all-diamond photonic crystal cavities, we achieve strong SiV-photon coupling with a cooperativity of greater than 20. Using this platform, we realize a quantum-optical switch controlled by the spin degree of freedom of a single SiV. By measuring intensity correlations of indistinguishable Raman photons emitted into a single waveguide, we observe a quantum interference effect resulting from the superradiant emission of two probabilistically entangled SiV centers. Finally, we demonstrate controllable photon-mediated interactions between the spin degrees of freedom of two cavity-coupled SiV centers. When the optical transitions of the two SiV centers are tuned into resonance, the coupling of each SiV to the common cavity mode results in a coherent interaction between the two SiVs, leading to the observation of super- and sub-radiant two-SiV states.
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.
Quantum networking is a crucial technology towards constructing large-scale distributed quantum systems. The structure of photonic link and distributed network nodes allows high-speed and high-fidelity interconnect, enabling various applications such as distributed quantum computing and sensing, as well as secure quantum communications. Optically interfaced solid-sate spins are promising candidates for building a quantum network due to their active spin-photon interfaces, compatibility, and scalability for device integration. Especially for defect spins in silicon, the platform benefits from mature silicon photonic industry, and can access to the integration techniques developed over the past decades. T center in silicon particularly holds great expectations because of the telecom-O band optical interface, ground state doublet spin manifold, and long-lived nuclear spin coherence. Their telecom spin-photon interface provides a direct link between stationary quantum memory and flying qubits that are compatible with the existing telecommunication fiber network infrastructure. This work focuses on investigating cavity quantum electrodynamics (cQED) for cavity-coupled single T centers, its applications in quantum optical control of T center optical properties, and in realizing single-shot spin state readout. The cavity enhanced light-matter interaction mitigates the caveats of T center, such as long radiative lifetime, low Debye-Waller factor, and lack of polarization selection rule for the optical transitions. In this work, by integrating single T centers with a low-loss, small mode volume silicon photonic cavity, we have achieved the Purcell enhancement for boosting the T center fluorescence rate with a factor of 6.89. We build up the theoretical framework based on the Jaynes-Cummings model and Lindblad master equation to explain experimental observations and reveal cQED parameters. The further study on the electronic spin state readout is carried out as the fast, high-fidelity single-shot readout is critical for quantum information processing. Two methods are proposed based on realistic cQED parameters: resonant fluorescence readout in the low-cooperativity regime and spin-dependent cavity-reflection readout for intermediate- and high-cooperativity regimes. Both approaches demonstrate feasibility of high-fidelity (F > 0.95) readout, particularly the reflection readout allows F > 0.99 within a short readout time of 50 μs. This work demonstrates a promising telecom spin-photon interface with high-fidelity readout based on cavity-coupled single T centers in silicon, which are promising candidates for building future large-scale quantum networks.
With their ability to process and transfer quantum information, large-scale entanglement-based quantum networks could be at the heart of a new age of quantum information, enabling fundamentally new applications such as distributed quantum computation, quantum communication, and quantum enhanced sensing. Due to their long spin coherence, controllable local qubit registers and optically active spins, color centers in diamond are prime candidates for nodes of such a network, and have enabled some of the most advanced quantum network demonstrations to date. These demonstrations include the distribution of a 3-node GHZ state across a quantum network, entanglement swapping, entanglement distillation, and memory-enhanced quantum communication. To move beyond current proof-of-principle networks, a further increase of entanglement generation rates is crucial. This thesis presents theoretical and experimental work on enhancing the spin-photon interface of color centers in diamond to achieve this goal, making use of the Purcell effect. The discussed work follows two main directions: embedding of color centers in open, tuneable Fabry-Perot micro-cavities, and in all-diamond photonic crystal cavities. First, we describe theoretical and experimental progress towards cavity-enhanced quantum networks based on nitrogen-vacancy (NV) centers in diamond. Due to their first order sensitivity to electric fields, we choose to embed NV centers in microns-thin diamond membranes that can be integrated into open fiber-based micro-cavities. We develop analytical methods to optimize the design of such open cavity systems for maximum Purcell enhancement of embedded color centers. We demonstrate a method to fabricate optically coherent NV centers in microns-thin diamond membranes, and use such structures to demonstrate the resonant excitation and detection of coherent, Purcell enhanced NV emission. A theoretical model in excellent agreement with our results suggests our system can improve entanglement rates between distant NV centers by two orders of magnitude with near-term improvements to the setup. Second, we describe progress towards an efficient spin-photon interface of group-IV color centers in diamond by coupling them to photonic nanostructures, allowing for large-scale integration. Due to their first-order insensitivity to electric fields, group-IV color centers can be brought in close proximity to surfaces (~ 100 nm), allowing for sub-wavelength mode volumes and thus very high Purcell factors. We numerically optimize photonic crystal cavity designs to maximize the Purcell enhancement of embedded emitters, test the robustness of our designs to real-world fabrication imperfections, and devise a method to efficiently interface nanophotonic structures. We then proceed to fabricate all-diamond photonic crystal cavities, making use of a dry etching technique that is selective to different crystallographic directions, and characterize the resulting optical quality factors. Finally, we marry the developed fabrication methods to fabricate microns-sized diamond platelets that can be transferred from a holding frame in a controlled fashion. This capability could be crucial for the realization of hybrid photonic circuits that we expect to be at the heart of future large-scale quantum networks.
Photons are excellent carriers of quantum information. The generation, manipulation and read-out of photonic quantum states have enabled pioneering investigations in quantum physics, paving the way to groundbreaking technologies. Integrated quantum photonics, that is the processing of photons on-chip, is at the forefront of this revolution. In particular, silicon integrated circuits have emerged as the dominant material platform for large-scale quantum photonics. However, the difficulty to inject single photons on-demand in a silicon chip is a major obstacle to the level of complexity of current systems. In this context, the isolation of individual fluorescent defects in silicon, called color centers, opens an avenue toward the integration of atomic sources of single photons. While several color centers have demonstrated an ability to generate antibunched photons, practical applications require tailoring of their emission through quantum electrodynamics effects in optical cavities.This PhD thesis is devoted to cavity quantum electrodynamics with color centers in silicon optical cavities, in view of building an efficient source of single photons. The efforts are first focused on ensembles of G centers in microring cavities. The optical properties of cavity-coupled G centers are studied using microphotoluminescence spectroscopy, and an enhancement of their zero-phonon emission rate by Purcell effect is demonstrated. However, a quantitative analysis reveals a poor quantum efficiency, motivating the choice of another emitter for further experiments. Subsequently, the efforts are focused on the W center. Purcell enhancement of the overall recombination rate is observed for an ensemble of W centers in a circular Bragg grating cavity. Using a quantitative analysis based on finite-difference time-domain calculation, a high quantum efficiency is estimated. The results being encouraging for the purpose of single photon emission, an optical setup is developed for single-emitter spectroscopy and a strategy is devised to fabricate individually-adressable emitters, leading to the isolation of single W centers in unpatterned silicon-on-insulator. Using a nanofabrication process allowing for deterministic positionning, the emitters are embedded into circular Bragg grating cavities, resulting in an increase of the photoluminescence intensity by orders of magnitude by Purcell effect. This work leads to the demonstration of a source of triggered single photons.A next milestone will be the demonstration of a single photon source for integrated photonic circuits, based on a color center in a waveguide-coupled optical cavity. Beyond the interest for integrated quantum photonics, the observation of bright photoluminescence from single color centers opens perspectives for further experiments, allowing to probe fundamental questions relative to their photophysics.
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\tand 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.