Guiding Diamond Spin Qubit Growth with Computational Methods
Jonathan C. Marcks, Mykyta Onizhuk, Nazar Delegan, Yuxin Wang, Masaya Fukami, Watts, Maya, Aashish A. Clerk, F. Joseph Heremans, Giulia Galli, D. D. Awschalom
The nitrogen vacancy (NV) center in diamond, a well-studied, optically active spin defect, is the prototypical system in many state of the art quantum sensing and communication applications. In addition to the enticing properties intrinsic to the NV center, its diamond host's nuclear and electronic spin baths can be leveraged as resources for quantum information, rather than considered solely as sources of decoherence. However, current synthesis approaches result in stochastic defect spin positions, reducing the technology's potential for deterministic control and yield of NV-spin bath systems, as well as scalability and integration with other technologies. Here, we demonstrate the use of theoretical calculations of electronic central spin decoherence as an integral part of an NV-spin bath synthesis workflow, providing a path forward for the quantitative design of NV center-based quantum sensing systems. We use computationally generated coherence data to characterize the properties of single NV center qubits across relevant growth parameters to find general trends in coherence time distributions dependent on spin bath dimensionality and density. We then build a maximum likelihood estimator with our theoretical model, enabling the characterization of a test sample through NV T2* measurements. Finally, we explore the impact of dimensionality on the yield of strongly coupled electron spin systems. The methods presented herein are general and applicable to other qubit platforms that can be appropriately simulated.
The nitrogen vacancy (NV) center in diamond, a well-studied, optically active spin defect, is the prototypical system in many state of the art quantum sensing and communication applications. In addition to the enticing properties intrinsic to the NV center, its diamond host's nuclear and electronic spin baths can be leveraged as resources for quantum information, rather than considered solely as sources of decoherence. However, current synthesis approaches result in stochastic defect spin positions, reducing the technology's potential for deterministic control and yield of NV-spin bath systems, as well as scalability and integration with other technologies. Here, we demonstrate the use of theoretical calculations of electronic central spin decoherence as an integral part of an NV-spin bath synthesis workflow, providing a path forward for the quantitative design of NV center-based quantum sensing systems. We use computationally generated coherence data to characterize the properties of single NV center qubits across relevant growth parameters to find general trends in coherence time distributions dependent on spin bath dimensionality and density. We then build a maximum likelihood estimator with our theoretical model, enabling the characterization of a test sample through NV T2* measurements. Finally, we explore the impact of dimensionality on the yield of strongly coupled electron spin systems. The methods presented herein are general and applicable to other qubit platforms that can be appropriately simulated.
Abstract Nitrogen-vacancy (NV) centers in diamond have been developed into essential hardware units for a wide range of solid-state-based quantum technology applications. While such applications require the long spin coherence times of the NV centers, they are often limited due to decoherence. In this study, we theoretically investigate the decoherence of NV-spin ensembles induced by nitrogen impurities (P1 centers), which are one of the most dominant and inevitable magnetic field noise sources in diamond. We combined cluster correlation expansion and density functional theory to compute the Hahn-echo spin-coherence time of the NV centers for a broad range of P1 concentrations. Results indicate a clear linear dependence of T2 on P1 concentrations on a log scale with a slope of −1.06, which is in excellent agreement with previous experimental results. The interplay between the Jahn–Teller effect and the hyperfine interaction in the P1 center plays a critical role in determining the bath dynamics and the resulting NV decoherence. Our results provide a theoretical upper bound for the NV-spin T2 over a wide range of P1 densities, serving as a key reference for materials optimization and spin bath characterization to develop highly coherent NV-based devices for quantum information technology.
We theoretically investigate spin decoherence of a single nitrogen-vacancy (NV) center in diamond. Using the spin coherent-state P-representation method, we simulate coherence evolution of the NV center coupled to surrounding nitrogen electron (N) spins. In the system, the strength of N-N coupling is the same order as that of NV-N coupling (the strong intrabath coupling regime). We find that spin decoherence time as well as free-induction decay of the NV center depend on the spatial configuration of N spins. Both the spin decoherence rate (1/T2) and dephasing rate (1/T2∗) of the NV center increase linearly with the concentration of the N spins. Using the P-representation method, we also demonstrate extracting the noise spectrum of the N spin bath. The capability to calculate the noise spectrum will provide promising pathways to suppress decoherence of spin systems in the strong intrabath coupling regime.
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.
Among the possible defects that can occur in diamonds, one that draws attention is the nitrogen-vacancy (NV) center.Studied since the early 90s, in recent years, they became one of the most promising platforms for field applications of quantum technology at room temperature, especially for quantum sensing.They are sensitive to electric and magnetic fields, temperature, and strain, making these nanosensors a versatile platform for many applications.The NV center's spin state is easy to read and manipulate by optical means, and, most interestingly, it works well at room temperature, which facilitates its use.The great challenge to implement quantum protocols and quantum algorithms is the coherence time of the quantum states.The NV center stands out for having relatively high coherence times at room temperature.This dissertation presents measurements to characterize the electron spin coherence of NV centers in an ultrapure sample of diamond designed for quantum sensing applications.These measurements combine optical e magnetic resonance techniques.For that, a method was implemented using a conventional CCD camera and a clever imaging protocol, making it possible to perform various pulsed microwave experiments on the electron spin, such as Rabi oscillations and Hahn spin-echo, which were used for determining the characteristic relaxation times (T 1 and T 2 ).Results show that this system provides at least two readily accessible qubits that can be used in quantum protocols even at room temperature.
Nitrogen-vacancy (NV) centers in diamond have emerged in the last decade as a prominent platform for quantum technologies. As for any qubit system, a good understanding of their local environment is crucial to build quantum devices protected from detrimental noise. Here, we describe in detail a method to spectroscopically characterize the spin bath around an NV center, even when the NV coherence time is short, and identify the coherent coupling with the nearest nuclear spins. In the regime of weak qubit-bath coupling, the acquired knowledge of the bath reliably predicts the qubit dynamics under different controls.
This thesis investigates the theoretical foundations, material properties, and experimental realization of quantum sensors based on the Nitrogen-Vacancy (NV) centers in diamond, a solid-state system that combines quantum coherence with room-temperature operability. The first chapter introduces the principles of quantum sensing, outlining the fundamental definitions, operating protocols, and physical processes underlying the quantum measurement paradigm. Emphasis is placed on the quantum sensing Hamiltonian and the distinction between various classes of quantum sensors. The second chapter focuses on diamond as a host material and on the NV center as a quantum defect. The electronic structure, optical transitions, and spin properties of the NV center are analyzed in detail. Several techniques of NV-based magnetometry are presented, including continuouswave and pulsed optically detected magnetic resonance (ODMR). The discussion also addresses coherence times (T1, T2, and T∗2 ) and methods of diamond synthesis together with NV-center generation through irradiation and annealing. Chapter three develops the physical theory describing the NV center. The Hamiltonian formalism includes spin-spin, hyperfine, and quadrupolar interactions, as well as couplings to external magnetic fields. The chapter further introduces the Bloch sphere representation, magnetic resonance phenomena, and models of lightmatter interaction, ranging from the semiclassical to the fully quantum Rabi framework. A seven-level rate-equation model is proposed to capture the spin dynamics and optical cycling processes of the NV center. The fourth chapter reports the experimental results. After describing materials and methods, several ODMR-based vector magnetometry experiments are presented, highlighting different spectral regimes and the dependence of resonance features on the external magnetic field geometry. Additional studies demonstrate temperature sensing and microwave-free magnetometry techniques for mapping magnetic field distributions. Sensitivity analysis and calibration procedures are also discussed.