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Controlled quantum dynamics of Nitrogen vacancy centers in diamond

Albrecht, Andreas

Published Jan 1, 2015• 1 citation
Publisher

Abstract

Color centers in diamond, and in particular the nitrogen-vacancy center (NV center), have proven promising for the emerging field of quantum technologies. In this thesis, new concepts for the manipulation of the NV center dynamics will be addressed, along with the proposal of novel fields of application. It comprises: (i) A study of the NV coupling to intrinsic acoustical phonons in nanocrystals, and concepts to exploit that mechanism for conditional quantum operations. (ii) The proposal for the bottom-up creation of NV arrangements on the nanoscale by the ordered arrangement of nanodiamonds directed by biological scaffold structures. A framework is developed for coherently addressing and manipulating NV centers in such structures along with studies of noise and imperfections. (iii) The interferometry with nanodiamonds in search of signatures of quantum gravity. (iv) The creation of an illustrative (filter-based) framework for the analysis and design of hybrid NV-nuclear spin couplings.

DOI
10.18725/oparu-3319

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Color centers in diamond, and in particular the nitrogen-vacancy center (NV center), have proven promising for the emerging field of quantum technologies. In this thesis, new concepts for the manipulation of the NV center dynamics will be addressed, along with the proposal of novel fields of application. It comprises: (i) A study of the NV coupling to intrinsic acoustical phonons in nanocrystals, and concepts to exploit that mechanism for conditional quantum operations. (ii) The proposal for the bottom-up creation of NV arrangements on the nanoscale by the ordered arrangement of nanodiamonds directed by biological scaffold structures. A framework is developed for coherently addressing and manipulating NV centers in such structures along with studies of noise and imperfections. (iii) The interferometry with nanodiamonds in search of signatures of quantum gravity. (iv) The creation of an illustrative (filter-based) framework for the analysis and design of hybrid NV-nuclear spin couplings.
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.
The Nitrogen-Vacancy (NV) color center is a defect of diamond which behaves as an artificial atom hosted in a solid-state matrix. Due to its electron spin properties which can be read-out and manipulated as an elementary quantum system, the NV center has found a wide panel of applications as a qubit for quantum information and as a magnetic field sensor. However these applications require to control the properties of the NV centers and their localization. This doctoral thesis investigates methods allowing us to tailor the properties of NV centers by combining techniques for the implantation of nitrogen atoms and the plasma-assisted (CVD) synthesis of diamond.The manuscript is divided into six chapters. The first chapter summarizes the properties of the NV center which will set our objectives for the NV engineering. The second chapter will describe how arrays of NV centers can be created using Focused Ion Beam implantation. The results open a wide range of applications for the targeted creation of NV centers in diamond structures such as photonic crystals and tips. However the low kinetic energy which is required for achieving implantation within a spot of 10-nm diameter leads to shallow defects which properties are strongly affected by the sample surface. The third chapter investigates how the overgrowth of a diamond layer over implanted NV centers can remove the detrimental influence of the surface. The fourth and fifth chapters describe effective methods for NV center fabrication through the control of the CVD growth conditions of the hosting crystal. Thin layers with high NV doping can be grown and almost perfect control of the orientation of the NV axis can be achieved. With the goal to optimize the spin coherence properties, the sixth chapter investigates how the electron spin of the NV center can be protected from decoherence effects induced by magnetic noise due to the unpolarized spins in the diamond lattice.
During the last decade, nitrogen-vacancy (NV) centers in diamond have gained a prominent role within the field of quantum technologies. These color defects inside the diamond lattice have been proved to be an extraordinary platform that assists in many of the current challenges that cutting-edge research is facing. The application of these novel tools exceeds the borders of quantum physics and reaches fields such as medicine, biology or chemistry. This thesis is focused on the development of novel theoretical schemes that intend to open new ways of understanding the NV centers as a quantum tool and sensor with direct applications. The manipulation of NV centers has become relatively easy in these last years. Moreover, via a proper control, the environment of an NV center may be overridden. In this thesis, we treat the NV center as a tool for enhancing the performance of nuclear magnetic resonance (NMR). Since the resolution of NMR is largely limited by the poor polarization of certain organic molecules, we here create and develop a theoretical frame that uses the NV center as a tool to transfer polarization toward organic samples in an efficient and controllable manner. In addition, this theoretical effort is supported by extensive numerical simulations and, moreover, all the predictions are confirmed by experimental evidence. Therefore, we demonstrate polarization transfer to external molecules at room-temperature paving the way for high-resolution NMR. Motivated by the success of the NV center as a polarization tool, we have further extended our analysis aiming to develop a phase transition sensor. In particular, we propose the NV center as a tool to assist current research on chemical reactions and molecular dynamics occurring at solid-liquid interfaces. These processes occur at a nanometric scale and thus, a nanometric sensor is desirable. In this context, the NV center is introduced as an ideal platform to investigate exotic phases of water when deposited onto diamond surface at room-temperature. In fact, recent studies predict that ultra-thin layers of water behave differently from bulk water due to interactions between water molecules and carbon atoms in the diamond surface. Through this thesis, we provide a theoretical and numerical work that predict how the NV center spin will behave in the presence of different phases of water, and hence, we reveal the NV center as a high-resolution sensor able to determine internal structures.
Nitrogen-vacancy centers (NVs) are an atomic defect in diamond which possess remarkable fluorescence and spin properties which can be used for multiple metrological applications, particularly when the NV is hosted in nanodiamond, which can be easily integrated with a variety of nanoscale systems. A new class of nanodiamond hybrid nanostructures was developed using bottom-up synthesis methods. In this work, coupling between NV centers and plasmonic, excitonic and magnetic nanoparticles in these nanodiamond hybrid nanostructures is investigated using fluorescence lifetime measurements, spin relaxometry measurements and modeled using finite element method (FEM) and Monte Carlo simulations. This work not only characterizes the properties of these nanodiamond-hybrid nanostructures but also facilitates design guidelines for future hybrid structures with enhanced metrological and imaging capabilities.
This thesis represents several steps in the development of Nitrogen-Vacancy Nanodiamond as an effective optical label for biological measurements and as a tool for nanometry and quantum information techniques. In this thesis I cover concrete progress in many areas of nanodiamond research, demonstrating that optical interactions alone can be used to control NV spin polarisation and measure NV temperature. I develop a method for high-contrast imaging of NV centres using magnetic modulation, and also show a method for measuring the Raman scattering of water to an unprecedented level of accuracy. This thesis also contains the outlines of two more experiments: one aimed at measuring NV concentration in aqueous nanodiamond suspensions, and another whose aim is to use multiple NV centres in a single nanodiamond to measure the orientation and strength of an external magnetic field.