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Coherent dynamics of a hybrid quantum spin-mechanical oscillator system

Kenneth William Lee

Published Jan 1, 2017• 1 citation
OpenAlex

Abstract

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.

Related papers

Diamond optomechanical crystals with embedded nitrogen-vacancy centers

Jeffrey V. Cady, Ohad Michel, Kenneth W. Lee +4 more

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. Strong coupling 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 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 optomechanical crystals as well as the spin coherence of single embedded NV centers. We find that the spin has long coherence times $T_2^* = 1.5 μs$ and $T_2 = 72 μs$ despite its proximity to nanofabricated surfaces. Finally, we discuss potential improvements of these devices and prospects for future experiments in the quantum regime.

arXiv:1811.04275•APS•Nov 10, 2018•0 citations

Diamond optomechanical crystals with embedded nitrogen-vacancy centers

Jeffrey V. Cady, Ohad Michel, Kenneth W. Lee +4 more

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.

Quantum Science and Technology•Feb 4, 2019•41 citations

Quantum control of single spins and single photons in diamond

Toeno van der Sar

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.

•Mar 27, 2012•0 citations

Quantum acoustics with diamond color centers

Srujan Meesala

Realization of physical systems for quantum information processing fundamentally rests on the ability to generate entanglement among many quantum bits. To this end, solid state quantum systems are often considered a scalable approach due to the relative ease of generating of a large number of individual qubits. However, realizing strong coherent interactions that dominate decoherence processes in the solid state environment is a formidable challenge that has continued to motivate the investigation of new physical systems to store quantum information and new mechanisms to achieve controllable interactions. This thesis takes steps in these directions with diamond color centers, which can store optically accessible quantum information in their electronic spin. We study color center spins as acoustic two level systems, and consider whether their interaction with single phonons in diamond can be engineered to be coherent. Through spectroscopy of color centers in diamond nanomechanical devices and follow-up theoretical work, we identify the negatively charged silicon vacancy (SiV) color center as a promising candidate for phonon-mediated quantum information processing. In the process, an electromechanical device platform capable of tuning the strain environment of color centers is developed. It is used to mitigate thermal decoherence of the SiV spin and demonstrate photon-mediated quantum interference between two SiV centers on a diamond chip, highlighting the utility of nanomechanical devices for photonic quantum networks. Finally, we present high quality factor, wavelength scale acoustic resonators in diamond using phononic crystals towards a coherent interface between SiV centers and single phonons.

•May 16, 2019•0 citations

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The nitrogen vacancy (NV) center in diamond is a unique quantum system that combines solid state spin qubits with coherent optical transitions. The spin states of the NV center can be initialized, read out, and controlled with RF fields at room temperature. It can be coupled to other spin systems in the environment while at the same time maintaining an extraordinary degree of quantum coherence. Experiments utilizing the NV center's spin states have led to a wide range of demonstrations from quantum error correction to high-sensitivity magnetometry. This thesis, however, focuses on creating an interface between NV centers and light in the visible domain by making use of its optical transitions. Such an interface connects the quantum system consisting of NV centers and nuclear spins to photons, which can then be used to both manipulate the spin qubits themselves or transport quantum information over large distances.

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Quantum Optical Control of Single Spins in Diamond

Christopher G. Yale

The nitrogen-vacancy (NV) center in diamond has garnered great interest over the past decade as its electronic spin shows promise as a quantum bit (qubit) and nanoscale sensor. Consisting of a substitutional nitrogen adjacent to a vacant site within the carbon lattice of diamond, this defect exhibits millisecond-long spin coherence times extending beyond room temperature, spin-dependent optical addressability, coupling to intrinsic and nearby nuclear spins, and it can be controlled and manipulated through electrical, magnetic, and optical means. In particular, at cryogenic temperatures (T < 25 K), the NV center's excited state becomes sharp and optically resolvable, providing a solid-state quantum optical testbed. In this thesis, I describe several experiments that explore this quantum optical interface to facilitate the development of a photonic network of single spins linked and controlled by light. We begin by exploring how electric fields tune the orbital levels within the NV center through the DC Stark effect, finding a surprising photo-induced field that aids in the ability to tune multiple NV centers' optical transitions to degeneracy. We then develop techniques to fully control the spin state of the NV center by coupling through a lambda system, an energy configuration consisting of two lower levels coupled to one of higher energy. When a lambda system is optically driven, the spin becomes trapped in a dark state, or the eigenstate of the system that is not coupled to the light fields through destructive interference, forming the basis for the various types of control demonstrated. We demonstrate arbitrary-basis initialization and readout of the spin state through coherent population trapping, as well as the ability to rotate about any arbitrary basis through stimulated Raman transitions. Combining these techniques, we measure the NV center's spin coherence through a completely optical measurement. We then extend these lambda system techniques to adiabatically move the dark state in trajectories around the Bloch sphere. Such trajectories accumulate a quantum mechanical phase that depends only on the geometry of the path enclosed, not on the energetics or time of the interaction. We characterize the interaction, measure this phase, known as Berry phase, and explore the limits of its control and resilience to noise. Finally, we demonstrate another all-optical control technique that uses strong ultrafast pulses of light to transfer the spin between the ground and excited states, deriving spin manipulation from the excited state dynamics. This technique also provides time-resolved spectroscopy of the excited state and its various decay and decoherence mechanisms. These experiments advance the progress toward the development of photonic networks coupling and controlling defects through light-matter interactions.

•Jan 1, 2015•0 citations
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.
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. Strong coupling 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 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 optomechanical crystals as well as the spin coherence of single embedded NV centers. We find that the spin has long coherence times T2∗=1.5μsT_2^* = 1.5 μsT2∗​=1.5μs and T2=72μsT_2 = 72 μsT2​=72μs despite its proximity to nanofabricated surfaces. Finally, we discuss potential improvements of these devices and prospects for future experiments in the quantum regime.
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.
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.
Realization of physical systems for quantum information processing fundamentally rests on the ability to generate entanglement among many quantum bits. To this end, solid state quantum systems are often considered a scalable approach due to the relative ease of generating of a large number of individual qubits. However, realizing strong coherent interactions that dominate decoherence processes in the solid state environment is a formidable challenge that has continued to motivate the investigation of new physical systems to store quantum information and new mechanisms to achieve controllable interactions. This thesis takes steps in these directions with diamond color centers, which can store optically accessible quantum information in their electronic spin. We study color center spins as acoustic two level systems, and consider whether their interaction with single phonons in diamond can be engineered to be coherent. Through spectroscopy of color centers in diamond nanomechanical devices and follow-up theoretical work, we identify the negatively charged silicon vacancy (SiV) color center as a promising candidate for phonon-mediated quantum information processing. In the process, an electromechanical device platform capable of tuning the strain environment of color centers is developed. It is used to mitigate thermal decoherence of the SiV spin and demonstrate photon-mediated quantum interference between two SiV centers on a diamond chip, highlighting the utility of nanomechanical devices for photonic quantum networks. Finally, we present high quality factor, wavelength scale acoustic resonators in diamond using phononic crystals towards a coherent interface between SiV centers and single phonons.
The nitrogen vacancy (NV) center in diamond is a unique quantum system that combines solid state spin qubits with coherent optical transitions. The spin states of the NV center can be initialized, read out, and controlled with RF fields at room temperature. It can be coupled to other spin systems in the environment while at the same time maintaining an extraordinary degree of quantum coherence. Experiments utilizing the NV center's spin states have led to a wide range of demonstrations from quantum error correction to high-sensitivity magnetometry. This thesis, however, focuses on creating an interface between NV centers and light in the visible domain by making use of its optical transitions. Such an interface connects the quantum system consisting of NV centers and nuclear spins to photons, which can then be used to both manipulate the spin qubits themselves or transport quantum information over large distances.
The nitrogen-vacancy (NV) center in diamond has garnered great interest over the past decade as its electronic spin shows promise as a quantum bit (qubit) and nanoscale sensor. Consisting of a substitutional nitrogen adjacent to a vacant site within the carbon lattice of diamond, this defect exhibits millisecond-long spin coherence times extending beyond room temperature, spin-dependent optical addressability, coupling to intrinsic and nearby nuclear spins, and it can be controlled and manipulated through electrical, magnetic, and optical means. In particular, at cryogenic temperatures (T < 25 K), the NV center's excited state becomes sharp and optically resolvable, providing a solid-state quantum optical testbed. In this thesis, I describe several experiments that explore this quantum optical interface to facilitate the development of a photonic network of single spins linked and controlled by light. We begin by exploring how electric fields tune the orbital levels within the NV center through the DC Stark effect, finding a surprising photo-induced field that aids in the ability to tune multiple NV centers' optical transitions to degeneracy. We then develop techniques to fully control the spin state of the NV center by coupling through a lambda system, an energy configuration consisting of two lower levels coupled to one of higher energy. When a lambda system is optically driven, the spin becomes trapped in a dark state, or the eigenstate of the system that is not coupled to the light fields through destructive interference, forming the basis for the various types of control demonstrated. We demonstrate arbitrary-basis initialization and readout of the spin state through coherent population trapping, as well as the ability to rotate about any arbitrary basis through stimulated Raman transitions. Combining these techniques, we measure the NV center's spin coherence through a completely optical measurement. We then extend these lambda system techniques to adiabatically move the dark state in trajectories around the Bloch sphere. Such trajectories accumulate a quantum mechanical phase that depends only on the geometry of the path enclosed, not on the energetics or time of the interaction. We characterize the interaction, measure this phase, known as Berry phase, and explore the limits of its control and resilience to noise. Finally, we demonstrate another all-optical control technique that uses strong ultrafast pulses of light to transfer the spin between the ground and excited states, deriving spin manipulation from the excited state dynamics. This technique also provides time-resolved spectroscopy of the excited state and its various decay and decoherence mechanisms. These experiments advance the progress toward the development of photonic networks coupling and controlling defects through light-matter interactions.