For quantum information applications, nitrogen-vacancy (NV) centers in diamond combine many of the advantages of atomic systems (optical access, millisecond spin-coherence times) with the engineering flexibility of solid-state devices. Recent demonstrations of coherent coupling between photons and individual NV-center spins [1,2] provide a route to integrating NV-center qubits within photonic networks and for on-demand generation of entangled single-spin/single-photon pairs. Such applications require the ability to tune the NV-center zero-phonon optical transitions, to compensate for natural sample inhomogeneities which perturb the electronic orbital states. Here we demonstrate the ability to electrically control the orbitals of individual NV centers by applying voltages to micron-scale surface gates [3]. Surprisingly, the local electric field experienced by an NV center is significantly enhanced by a photoinduced space charge resulting from photoionization of deep donor impurities within the diamond, even in high-purity single-crystal material (< 5 ppb nitrogen content). Since the photoinduced electric fields are reproducible as a function of gate voltage and are predominantly directed perpendicular to the diamond surface, we can harness them to obtain three-dimensional control of the local electric field vector with surface gates alone. To demonstrate this technique, we tune the excited-state orbital doublet of a strained NV center to degeneracy, as required for some spin-photon entanglement protocols [2], and then adjust the optical transition frequency, showing that we can tune multiple NV centers to have the same degenerate transition energy. This method should enable the coherent coupling of multiple NV center spins to indistinguishable photons within a scalable photonic network.
For quantum information applications, nitrogen-vacancy (NV) centers in diamond combine many of the advantages of atomic systems (optical access, millisecond spin-coherence times) with the engineering flexibility of solid-state devices. Recent demonstrations of coherent coupling between photons and individual NV-center spins [1,2] provide a route to integrating NV-center qubits within photonic networks and for on-demand generation of entangled single-spin/single-photon pairs. Such applications require the ability to tune the NV-center zero-phonon optical transitions, to compensate for natural sample inhomogeneities which perturb the electronic orbital states. Here we demonstrate the ability to electrically control the orbitals of individual NV centers by applying voltages to micron-scale surface gates [3]. Surprisingly, the local electric field experienced by an NV center is significantly enhanced by a photoinduced space charge resulting from photoionization of deep donor impurities within the diamond, even in high-purity single-crystal material (< 5 ppb nitrogen content). Since the photoinduced electric fields are reproducible as a function of gate voltage and are predominantly directed perpendicular to the diamond surface, we can harness them to obtain three-dimensional control of the local electric field vector with surface gates alone. To demonstrate this technique, we tune the excited-state orbital doublet of a strained NV center to degeneracy, as required for some spin-photon entanglement protocols [2], and then adjust the optical transition frequency, showing that we can tune multiple NV centers to have the same degenerate transition energy. This method should enable the coherent coupling of multiple NV center spins to indistinguishable photons within a scalable photonic network.
We demonstrate precise control over the zero-phonon optical transition energies of individual nitrogen-vacancy (NV) centers in diamond by applying multiaxis electric fields, via the dc Stark effect. The Stark shifts display surprising asymmetries that we attribute to an enhancement and rectification of the local electric field by photoionized charge traps in the diamond. Using this effect, we tune the excited-state orbitals of strained NV centers to degeneracy and vary the resulting degenerate optical transition frequency by >10 GHz, a scale comparable to the inhomogeneous frequency distribution. This technique will facilitate the integration of NV-center spins within photonic networks.
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.
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.
Abstract Nitrogen vacancy (NV) centers, optically active atomic defects in diamond, have attracted tremendous interest for quantum sensing, network, and computing applications due to their excellent quantum coherence and remarkable versatility in a real, ambient environment. One of the critical challenges to develop NV-based quantum operation platforms results from the difficulty in locally addressing the quantum spin states of individual NV spins in a scalable, energy-efficient manner. Here, we report electrical control of the coherent spin rotation rate of a single-spin qubit in NV-magnet based hybrid quantum systems. By utilizing electrically generated spin currents, we are able to achieve efficient tuning of magnetic damping and the amplitude of the dipole fields generated by a micrometer-sized resonant magnet, enabling electrical control of the Rabi oscillation frequency of NV spins. Our results highlight the potential of NV centers in designing functional hybrid solid-state systems for next-generation quantum-information technologies. The demonstrated coupling between the NV centers and the propagating spin waves harbored by a magnetic insulator further points to the possibility to establish macroscale entanglement between distant spin qubits.
A key requirement for many applications in solid-state quantum sciences is a high fluence of indistinguishable photons. The spontaneous emission of these photons is governed by the coupling of an excited quantum system to electromagnetic vacuum fluctuations. In our experiment, we enhance this coupling by engineering a tunable Fabry-Perot microcavity. The quantum system we study is the nitrogen-vacancy (NV) center in diamond, a workhorse for quantum science and engineering, due to its optical transitions and the coherent electron spin system it hosts. Our device consists of a high-quality, nano-fabricated, single-crystalline diamond membrane bonded to a planar mirror; the cavity is completed by a second, concave mirror. Using piezo positioners, we achieve full spectral and spatial tunability and freedom in selecting NVs with favorable emission properties in our low-temperature (4 Kelvin) experiments. Upon tuning of the cavity into resonance, we find significant enhancement of the 637 nm zero phonon line for several individual NVs which is accompanied by a strong reduction of the overall photoluminescence (PL) lifetime. We infer a 30-fold enhancement of the zero-phonon transition rate at best. The fraction of the PL emission associated to this resonant transition is thereby increased from 3% to 46%. Our results constitute a significant leap on the route towards the implementation of fast long-distance quantum networks, which are currently limited by the photon emission rate in their nodes. Furthermore, our versatile design is readily applicable to other solid-state quantum emitters like color centers in silicon carbide.
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.