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On the creation, coherence and entanglement of multi-defect quantum registers in diamond

Maarten J. Degen

Published Apr 6, 2021• 2 citations
Publisher

Abstract

Due to its long spin coherence and coherent spin-photon interface the nitrogen vacancy (NV) center in diamond has emerged as a promising platform for quantum science and technology, including quantum networks, quantum computing and quantum sensing. In recent years larger quantum systems have been demonstrated by using optical entanglement links between distant NV centers. These systems were based on high-quality NV centers that exhibit good optical coherence. State-of-the-art experiments with such systems have shown deterministic delivery of entanglement across a two-node quantum network as well as genuine multi-partite entanglement across a three-node quantum network. The additional capability to create larger quantum registers by direct magnetic coupling between high-quality NV centers and to other nearby defects would provide new opportunities for quantum memories in quantum networks but also for enhanced sensing protocols and spin chains for quantum computation architectures. In this thesis, we investigate methods to create larger quantum registers based on magnetic coupling and develop techniques to address and control individual defects in a system consisting of multiple defects. The results provide new insights for extended quantum registers based on magnetically coupled defects...

DOI
10.4233/uuid:e0b20592-a0ce-4ec4-8df0-a5aa25084301

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Due to its long spin coherence and coherent spin-photon interface the nitrogen vacancy (NV) center in diamond has emerged as a promising platform for quantum science and technology, including quantum networks, quantum computing and quantum sensing. In recent years larger quantum systems have been demonstrated by using optical entanglement links between distant NV centers. These systems were based on high-quality NV centers that exhibit good optical coherence. State-of-the-art experiments with such systems have shown deterministic delivery of entanglement across a two-node quantum network as well as genuine multi-partite entanglement across a three-node quantum network. The additional capability to create larger quantum registers by direct magnetic coupling between high-quality NV centers and to other nearby defects would provide new opportunities for quantum memories in quantum networks but also for enhanced sensing protocols and spin chains for quantum computation architectures. In this thesis, we investigate methods to create larger quantum registers based on magnetic coupling and develop techniques to address and control individual defects in a system consisting of multiple defects. The results provide new insights for extended quantum registers based on magnetically coupled defects...
Electron spin qubits associated with individual solid-state defects can exhibit exceptional coherence and bright optical interfaces. Furthermore, their magnetic interactions with nuclear spins in the host material present a resource for multi-qubit registers. They have thus emerged as powerful systems with which to develop quantum technologies. In this thesis, we develop a toolbox for the precise control of multi-qubit spin systems associated with single nitrogen-vacancy centres in diamond. We utilise this platform to explore a number of avenues in quantum science: networks, computation, sensing, and simulation. Our findings provide new insights towards the goal of distributed quantum computation, and establish a programmable solid-state-spin quantum simulator for studying many-body physics.
Single defect centers in diamond have emerged as a powerful platform for quantum optics experiments and quantum information processing tasks. Connecting spatially separated nodes via optical photons into a quantum network will enable distributed quantum computing and long-range quantum communication. Initial experiments on trapped atoms and ions as well as defects in diamond have demonstrated entanglement between two nodes over several meters. To realize multi-node networks, additional quantum bit systems that store quantum states while new entanglement links are established are highly desirable. Such memories allow for entanglement distillation, purification and quantum repeater protocols that extend the size, speed and distance of the network. However, to be effective, the memory must be robust against the entanglement generation protocol, which typically must be repeated many times. Here we evaluate the prospects of using carbon nuclear spins in diamond as quantum memories that are compatible with quantum networks based on single nitrogen vacancy (NV) defects in diamond. We present a theoretical framework to describe the dephasing of the nuclear spins under repeated generation of NV spin-photon entanglement and show that quantum states can be stored during hundreds of repetitions using typical experimental coupling parameters. This result demonstrates that nuclear spins with weak hyperfine couplings are promising quantum memories for quantum networks.
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.
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.
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.
Quantum networks promise to be the future architecture for secure communication and distributed quantum computation. This thesis describes experiments on nitrogenvacancy (NV) centres that lead towards a versatile multi-node quantum network consisting ofmulti-qubit nodes. The NV centre in diamond is a spinful optically-active crystal defect. NVs are a prime network-node candidate due to demonstrated coherence times beyond 100ms and longitudinal relaxation times exceeding 1s and their spin-selective optical interface which facilitates the generation of spin-photon entanglement. Entangling links between nodes are therefore readily created by overlapping the emission of two NVs on a beam splitter. Besides NVs, we further address individual 13C nuclear spins in the vicinity and use these spins as a quantum resource. Our goal is to propel these nuclear spins to constitute robust quantummemories which store and manipulate quantum information in an NV-based quantum network. The experiments described in this thesis are thematically separated into three groups. First, we explore the NV-nuclear interplay. We demonstrate nuclear-spin control by observing the Zeno effect on up to two logical qubits within the state space of three nuclear spins (Chapter 3). We further realize that the always-on magnetic hyperfine interaction between NV and nuclear spins will limit the nuclear spin coherence when entangling distant NV centres (Chapter 4). A systematic experimental study probes our theoretical prediction and we additionally demonstrate improved robustness for logical states within decoherence-protected state spaces (Chapter 5) and finally for individual nuclear spins (Chapter 6). Second,we use remoteNV-NV entangled states to demonstrate experimental milestones in quantumnetworks. The realization of a high-fidelity entangled link over a distance of 1.3km permits the loophole-free violation of Bell’s inequality (Chapter 7). We further increase the entangling rate by three orders of magnitude such that it exceeds the decoherence rate of an entangled state on our network. This allows us to convert our probabilistic entanglement generation into a deterministic process which delivers entangled states at prespecifiedmoments in time (Chapter 8). Third, we finally combine the concepts of nuclear-spin quantum memories and remote entanglement generation to demonstrate entanglement distillation in a network setting (Chapter 9). We subsequently generate two raw entangled input states between two remote NV centres. The first state is stored on nuclear spins to liberate both NVs for the second round of state generation. Finally, a higher-fidelity entangled state is distilled via local operations. This constitutes the first quantum-network demonstration that relies on the control of multiple fully-coherent quantum systems per network node.