This thesis presents a set of experiments that explore the possible realisation of a macroscopic quantum network based on solid-state quantum bits. Such a quantum network would allow for studying quantum mechanics on large scales (meters, or even kilometers), and can open new possibilities for applications in quantum information processing. A promising candidate platform for such a network is the nitrogen-vacancy (NV) center in diamond. The NV center is a lattice defect in diamond that has excellent quantum properties and allows optical access to a quantum register of individual electronic and nuclear spins. We use optical spectroscopy and magnetic resonance techniques at liquid helium temperature to manipulate individual spins, and perform projective quantum measurements on them. We first show an experiment in which we create entanglement between two non-interacting nuclear spins by a projective quantum measurement. Second, we demonstrate the creation of an entangled state between two NV electronic spins located in different setups at a distance of three meters. Finally, we demonstrate the deterministic teleportation of the quantum state of a nuclear spin onto an electronic spin over three meters. Our results demonstrate the great potential of the NV center for the realization of a large-scale quantum network.
This thesis presents a set of experiments that explore the possible realisation of a macroscopic quantum network based on solid-state quantum bits. Such a quantum network would allow for studying quantum mechanics on large scales (meters, or even kilometers), and can open new possibilities for applications in quantum information processing. A promising candidate platform for such a network is the nitrogen-vacancy (NV) center in diamond. The NV center is a lattice defect in diamond that has excellent quantum properties and allows optical access to a quantum register of individual electronic and nuclear spins. We use optical spectroscopy and magnetic resonance techniques at liquid helium temperature to manipulate individual spins, and perform projective quantum measurements on them. We first show an experiment in which we create entanglement between two non-interacting nuclear spins by a projective quantum measurement. Second, we demonstrate the creation of an entangled state between two NV electronic spins located in different setups at a distance of three meters. Finally, we demonstrate the deterministic teleportation of the quantum state of a nuclear spin onto an electronic spin over three meters. Our results demonstrate the great potential of the NV center for the realization of a large-scale quantum network.
In this thesis we experimentally investigate quantum nonlocality: entangled states of spatially separated objects. Entanglement is one of the most striking consequences of the quantum formalism developed in the 1920's; the predicted outcomes of independent measurements on entangled objects reveal strong correlations that cannot be explained by classical physics. Early on, such predictions led physicists to doubt the validity and completeness of quantum theory. At the same time, entanglement is a key resource for applications in quantum information processing and a pre-requisite for many tasks in quantum communication and computation. This thesis attempts to answer two application driven questions: Firstly, can we generate useful entangled states of solid state spins for applications in quantum information processing? Secondly, can we use such entangled states as a resource to teleport an unknown quantum state? Finally, we ask a foundational question: Are our entangled states indeed inconsistent with the classical notions of free choice, locality and realism? Can we prove this experimentally, under the minimal assumptions of a loophole-free Bell test? To answer these questions we use single spins in ultra-pure diamonds. In particular, we use the electronic and nuclear spins associated with single nitrogen-vacancy (NV) defects. The NV centre is a point defect in diamond, consisting of a substitutional nitrogen (N) atom and a neighbouring missing carbon atom (vacancy, V). The NV centre possesses bound electronic states, whose energy levels lie well within the bandgap of the diamond host and whose spin degree of freedom can be used as a quantum bit (qubit). Because of the large diamond bandgap and the 99% spin free carbon-12 environment, the electronic spin qubit has exceptional coherence properties even at room temperature. Optical and microwave fields allow control of the electronic spin, which in turn allows control of nearby nuclear spins (the host nitrogen nuclear spin, and nearby carbon-13 spins). At liquid helium temperatures, spin-preserving optical transitions provide a powerful optical interface to the electronic spin, allowing, for example, projective readout of the spin state. By employing a protocol where entanglement is heralded by the detection of a single photon from each of two NV centres in diamonds separated by three metres, we find we can answer the first question in the affirmative. We show for the first time heralded entanglement between solid state quantum systems separated by a human-scale distance. Then, by combining the heralded entanglement with a deterministic local Bell state measurement and fast feed-forward, we show for the first time unconditional quantum teleportation over human-scale distances. We teleport an unknown quantum state from a nuclear spin in one diamond to an electronic spin in a diamond three meters away. Finally, by employing techniques from the previous experiments, we implement the first loophole-free Bell test. We separate two diamonds by 1.3 kilometres and optimize all operational fidelities, collection efficiencies and rates. This allows us to generate heralded entanglement between them approximately once an hour. The distance provides us with time to read out the electronic spin state in each diamond, faster than any lightlike signal could travel between them. The high-fidelity entangled state preparation and spin readout are sufficient to violate the Clauser-Horne-Shimony-Holt Bell-inequality. Combined with fast random number generators and a robust statistical analysis, we find a significant rejection of the local-realist hypothesis, without requiring additional experimental assumptions. The results in this thesis open the door to various applications in quantum information processing. In particular, a remote photonic entangling operation may enable future quantum networks. In such a network the nodes would be formed by the NV centre's combined electronic and nuclear spin register. The nodes would be linked by photonic entanglement operations. Such a network could be used for long distance secure communication, provide a connection between separated quantum computers, or form the basis of a fault tolerant quantum computer by itself. Furthermore, a loophole-free Bell test demonstrates the possibility to do device independent randomness generation and key distribution, that could form the basis for future secure communication channels.
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.
Individual nitrogen vacancy (NV) centers in diamond have recently emerged as a leading candidate for a building block for quantum information processing systems. Individual NV centers have many properties that are desirable for qubits. For example their spin states can be manipulated, initialized and measured even at room temperature. In order to build a quantum information processing system that consists of more than a single NV center, these individual NV centers have to be connected via quantum channels that distribute entanglement and allow quantum state transfer between NV centers. This thesis explores how the optical properties of the NV center can be used and manipulated to form these quantum channels. Likewise we show how the same properties can be used to better control the nuclear spin environment surrounding the NV center. We first introduce, review and experimentally study the relevant optical properties of the NV center. These quantum optical techniques are then used to experimentally demonstrate spin-photon entanglement between the electronic spin of an individual NV center and a single photon. We next demonstrate quantum interference of two photons produced by NV centers in distinct diamond samples separated by two meters. These two demonstrations pave the way for entanglement generation, leading to quantum channels, between remote NV centers. Finally we demonstrate optical cooling, real-time measurement and conditional preparation of the nuclear spin environment around an NV center using all-optical manipulation of its electronic spin. This technique can lead to better control of individual NV centers and thus more robust quantum information processing systems.
Digital information based on the laws of quantum mechanics promisses powerful new ways of computation and communication. However, quantum information is very fragile; inevitable errors continuously build up and eventually all information is lost. Therefore, realistic large-scale quantum information processing requires the protection of quantum bits (qubits) against errors. In this thesis we present the experimental implementation of quantum error correction protocols based on spins in diamond. In such protocols, a quantum state is protected against errors by encoding in multiple qubits. Errors can be detected and corrected by measurement of correlations, so-called stabilizer-measurements, on these qubits.The experimental work presented in this thesis employs multiple spins in diamond as qubits to explore and implement error correction protocols. The nitrogen-vacancy (NV) centre in diamond is a lattice defect consisting of a nitrogen atom (N) and a vacancy (V) on two adjacent diamond lattice sites. This defect effectively results in an electronic spin that can be addressed as a qubit. The spin state can be manipulated by microwave fields and optically read out. At liquid helium temperatures (cryogenic temperature, ~4 K = -269 C), the NV electron spin provides high-fidelity single-shot readout and long coherence times.The NV centre is surrounded by naturally available (1.1% abundance) nuclear C13 spins. As the number of spins that are close enough to the NV centre to be strongly coupled is limited, we employ the weakly coupled nuclear spins in the spin bath of the NV centre. Using dynamical decoupling techniques these nuclear spins can be detected via the NV electron spin through the hyperfine interaction. The nuclear spins are long-lived and robust against optical excitation of the NV electron spin, which can make these spins a robust quantum register for quantum error correction.In Ch. 4 we demonstrate universal control over multiple of such weakly coupled nuclear C13 spins in the environment of the NV centre at ambient temperatures. We demonstrate initialization, control and read-out of individual nuclear spins. Finally, we implement a quantum error correction protocol by encoding a quantum state in the NV electron spin and two nuclear spins. Errors are detected by un-encoding the quantum state back to the electron spin and correction via a double controlled operation.For universal fault-tolerant quantum computations it is essential that the quantum information remains encoded at all times. In Ch. 5 we present multiple rounds of quantum error correction and active feedback on a continuously encoded qubit at cryogenic temperatures. A quantum state is protected by encoding in three weakly coupled spins. Errors are detected via high-fidelity non-demolition readout of the NV electron spin and actively corrected using fast classical electronics. We demonstrate that an actively error-corrected qubit is robust against phase flip errors and show that a superposition state can live longer than the best physical qubit in the encoding.The presented methods and results can be extended to a range of future experiments. In Ch. 6 we propose the implementation of five-qubit quantum error correction, the smallest code to correct for general single-qubit errors on the physical qubits in the encoding, by extending the experimental methods as developed in Chs. 4&5. Besides the exploration and development of larger error correction protocols and fault-tolerant quantum computing, the presented quantum register based in spins in diamond can be employed as a quantum node and combined with recent advances in the realization of quantum entanglement over large distances to form quantum networks. These networks can be used to study both fundamental questions as well as future applications in quantum information technology.
Gaining precise control over quantum systems is crucial for applications in quantum information processing and quantum sensing and to perform experimental tests of quantum mechanics. The experiments presented in this thesis implement quantum measurements and real-time feedback protocols that can help to achieve these goals using single electron and nuclear spins associated with the Nitrogen Vacancy (NV) center in diamond. Here we demonstrate that adaptive measurements allow for the manipulation of a quantum system using only measurement backaction and that they can enhance the performance of a single spin magnetometer. Furthermore, by creating entanglement and performing teleportation between two distant NV centers, we implement two elementary operations between two nodes of a quantum network.
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.