The thesis focuses on one of the most promising experimental platforms for quantum technologies: Single nitrogen-vacancy (NV) centers in diamond. This quantum system is composed by the spins of the valence electrons of the crystalline point defects and their nearby nuclei. Quite generally, a fundamental requirement to exploit the potentialities of the quantum nature of a system is its precise control. However, this always involves new challenges, related to the need to protect the quantum system from the environment (i.e. preserving the quantum nature of the system itself) and the desire to develop measurement protocols that can enhance its performance for quantum applications. Therefore, I focused my Ph.D. work to find novel solutions to these challenges.
The thesis focuses on one of the most promising experimental platforms for quantum technologies: Single nitrogen-vacancy (NV) centers in diamond. This quantum system is composed by the spins of the valence electrons of the crystalline point defects and their nearby nuclei. Quite generally, a fundamental requirement to exploit the potentialities of the quantum nature of a system is its precise control. However, this always involves new challenges, related to the need to protect the quantum system from the environment (i.e. preserving the quantum nature of the system itself) and the desire to develop measurement protocols that can enhance its performance for quantum applications. Therefore, I focused my Ph.D. work to find novel solutions to these challenges.
The field of quantum science and technology has generated many ideas for new revolutionary devices that exploit the quantum mechanical properties of small-scale systems. Isolated solid state spins play a large role in quantum technologies. They can be used as basic building blocks for a quantum computer or as ultra-sensitive magnetic-field probes which can detect the extremely weak magnetic field generated by a single proton. A major hurdle for realizing these applications is the loss of quantum coherence resulting from uncontrolled interactions with spins in the environment. In the experiments described in my thesis we studied spins associated with defect centers in diamond and used new strategies for mitigating decoherence involving advanced quantum control techniques and for fundamental studies of decoherence. We show that we can prolong the coherence time of a single spin associated with a Nitrogen-Vacancy (NV) defect center in diamond with dynamical decoupling techniques. Our experiments are accurately reproduced theoretically and from this theory we conclude that, with dynamically decoupling, the spin environment can in principle be made irrelevant for the decoherence of a single spin. This removes a major obstacle for using solid-state spins in quantum science and technology. Furthermore, the dynamics in the spin environment and its influence on the NV spin is thoroughly experimentally studied. By better understanding the mechanisms behind decoherence we may one day find the answer to unresolved fundamental issues in quantum physics such as the quantum measurement problem.
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.
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 work investigates the applicability of the nitrogen-vacancy (NV) defect center in diamond for quantum computation and metrology purposes. The NV center is a molecule like defect in the diamond lattice which is optically active and possesses an electron spin in its ground state. The spin can be used as a quantum bit and as a field sensor. The NV center has three major properties enabling individual control of single defects. Its optical properties depend on the spin state, the spin can be polarized optically and the spin state has an exceptionally long lifetime. Single NV centers can be controlled by optical and microwave radiation. Generally, the research on individually controllable quantum systems is not only motivated by quantum computation and communication. With the ongoing miniaturization nowadays electronic and electro-optic devices will soon reach the limit of single quantum building blocks. While in these applications the full complexity of single quantum systems might not be needed, small sensors based on single atoms or molecules might very well take advantage of the susceptibility of quantum coherences to environmental conditions. Major challenges for all approaches towards single quantum system control are the individual addressing, the measurement of the quantum state and the protection of quantum coherence from environmental noise. Today, there is a variety of systems (including the NV center) that allow control on the single quantum level. These are for example single photons, single ions and atoms in traps, single spins in semiconductors or single molecules in solid state systems. Rather mesoscopic examples are superconducting devices, nanomechanical oscillators or surface plasmon polaritons. Regarding the NV center it has been shown that the magnetic moment of its electron spin allows individual sensing and coupling to other surrounding electron and nuclear spins. Especially single nuclear spins were shown to be exceptional quantum memories. In this work small quantum registers of up to 5 spins have been used to test major requirements for a feasible quantum processor. Therefore, mainly artificially created high purity diamond samples with controlled spin and impurity concentration were used. The NV centers were either grown in or created via ion implantation techniques in a controlled fashion. As a first requirement for quantum computation entanglement among up to three spins has been generated and was verified by quantum state tomography. This proves the access of the full Hilbert space. Especially, entanglement among nuclear spins was very long-living. In further experiments this processor was used for first quantum algorithms like super-dense coding and the Deutsch algorithm. In addition, this work demonstrates new methods to initialize nuclear spin qubits into a desired quantum state. This is particularly important as improper initialization inhibits quantum computation. One of these methods is related to dynamic nuclear spin polarization and the other to measurement based state preparation. Nuclear spins in the diamond lattice originate mainly from the C-13 isotope. By artificially altering its content the influence on the NV center spin was investigated. The coherence times of the NV center were increasing inversely with the nuclear spin density. Even increasing nuclear spin density to offer more nuclear spin qubits to an operational quantum register was possible. As an alternative route of scaling up the quantum register pairs of closely spaced NV centers were investigated. For the first time two qubit gates among two NV centers mediated by magnetic dipolar coupling have been realized. Furthermore the sensing ability was demonstrated by measuring the relative distance of the two centers (10 nm) with sub-nm precision. Eventually, this work contains new insight into the electronically excited state of the NV center which allowed a more advanced control of the electron and nuclear spins. A comparably high magnetic field was used to decouple electron and nuclear spins. Finally, this allowed quantum nondemolition measurements on single nuclear spins which manifests in the observation of quantum jumps. The new insight was used to drastically improve the performance of quantum state readout. Summarizing, it was shown that single NV centers and proximal nuclear spins form versatile small quantum registers which can be interconnected with neighboring such NV quantum registers. Although the number of qubits used in this work is still small the experimental results propose a way of how to proceed when building a quantum computer. Regarding quantum metrology, however, the use of such a small register which can sense fields and store and process the results would already outperform a single NV electron spin by orders of magnitude.
Quantum technologies are transitioning from proof-of-principle experiments to practical everyday applications. As this transition unfolds, it remains unclear which quantum system will offer the most suitable platform for specific tasks. While many candidate systems offer excellent control and demonstrate rapid progress, they often require demanding operating conditions such as cryogenic temperatures down to the millikelvin range. The nitrogen-vacancy (N-V) center in diamond is a notable exception. This optically active defect allows full control of its electronic spin state at room temperature and maintains long coherence times under ambient conditions, a prerequisite for many applications. This accessibility makes the N-V center uniquely suited for translating fundamental quantum concepts into deployable technologies. The applicability of N-V centers in quantum sensing, quantum control, and quantum simulation is the central focus of this thesis. After an introductory overview of the field, the thesis introduces the experimental and theoretical concepts that are necessary to understand the presented results. It proceeds to show how the operating regime of N-V centers as sensors for AC magnetic fields and nuclear spins can be extended to low and zero magnetic bias fields. Many commonly used sensing protocols require a magnetic bias field, which can alter the investigated dynamics or may be infeasible to apply due to experimental constraints. This work describes how established sensing protocols can be adjusted for operation under these conditions, and presents novel sensing protocols that enable the detection of AC magnetic fields and nuclear spins in a regime where conventional protocols fail. These results highlight that precise control of the underlying quantum system is a must. Such control can be optimized using quantum optimal control, which allows one to improve the underlying gate operations in a closed-loop, black-box manner, provided a figure of merit can be found which reliably evaluates the gate-set's performance. As this performance can depend on the specific application, the following part of this thesis defines and benchmarks several figures of merit for closed-loop optimal control using an ensemble of N-V centers. The strengths and limitations of these figures of merit are discussed, and the dependence of the optimization performance on several control and experimental parameters is analyzed. The achieved results are applicable to a broad range of other physical platforms, and can serve as a reference for experimental groups that aim to optimize their gate operations using optimal control. Building upon these insights into quantum control, the next part of this thesis presents the fabrication, control, and application of a room-temperature quantum simulator based on thin nuclear spin layers in diamond. A detailed assessment of the growth process is provided, and the dynamics that allow nearby N-V centers to initialize and read out the nuclear spins are thoroughly investigated. Furthermore, the nuclear spin layer is employed to create and study discrete time-crystalline order. The results demonstrate a scalable route for exploring quantum many-body phenomena under ambient conditions. The thesis concludes with a summary and discussion of all results and provides an outlook on future work based on these findings. In conclusion, this thesis demonstrates and expands the versatile use of N-V centers in diamond for quantum sensing, control, and simulation, highlighting their potential as a practical platform for future quantum technologies.
The recent decade has witnessed exciting developments in quantum science and technology. Quantum sensing is a rapidly growing branch, which exploits the fragility of quantum systems to detect small external signals. The extreme control at the single-atom level and the remarkably long coherence time of engineered quantum systems enable unprecedented sensitivity and precision, beating the performance of classical techniques. The nitrogen-vacancy (NV) center in diamond is one of the most promising quantum sensors. Its unique advantages have attracted considerable attention, including a long spin coherence time throughout a broad temperature range, nanoscale resolution limited by the sensor-sample distance, convenient optical control of its spin states and remarkably versatile sensing capabilities. Its properties are well studied under a bias magnetic field oriented along its quantization axis. However, its sensing capabilities in the presence of an off-axis magnetic field are much less explored. My research aims to unlock the full potential of NV quantum sensor by developing new sensing modalities under a magnetic field acting perpendicular to the NV axis, and furthermore, integrating them into a scanning probe microscope. In this dissertation, I will report our progress toward building a scanning NV multimodal quantum imaging platform, which will open up exciting opportunities in measuring nanoscale phenomena. The first chapter provides an introduction to the background of quantum sensing with NV centers, followed by a discussion on its basic properties and established sensing techniques. The second and third chapters are dedicated to two experiments performed under a perpendicular magnetic field where traditional NV magnetometry based on the Zeeman effect fails. In the second chapter, I will introduce a new sensing strategy that uses the entanglement between the electron and nuclear spins to restore the magnetic field sensitivity under this unfavored condition. This allows us to sense small changes in the magnetic field angle relative to the NV axis, and to detect anisotropic magnetic noise in the local environment. In the third chapter, I will present our latest development of scanning NV electrometry, where a single NV at the apex of a diamond scanning probe images external alternating (AC) and direct (DC) electric fields with sub-100 nm resolution. In the last chapter, I will discuss our efforts on four experiments that were left unfinished. I will present the results we have achieved, analyze the challenges that we faced and propose potential solutions to overcome them.