Abstract Recently, there have been significant developments to detect nuclear spins with nitrogen vacancy (NV) centers in diamond. However, due to the nature of the short range dipole–dipole interaction, it takes a long time to detect distant nuclear spins with the NV centers. Here, we propose a rapid detection of nuclear spins with an entanglement between the NV centers. We show that the necessary time to detect the nuclear spins with the entanglement is several orders of magnitude shorter than that with separable NV centers. Our results pave the way for new applications in nanoscale nuclear magnetic resonance spectroscopy.
Abstract Recently, there have been significant developments to detect nuclear spins with nitrogen vacancy (NV) centers in diamond. However, due to the nature of the short range dipole–dipole interaction, it takes a long time to detect distant nuclear spins with the NV centers. Here, we propose a rapid detection of nuclear spins with an entanglement between the NV centers. We show that the necessary time to detect the nuclear spins with the entanglement is several orders of magnitude shorter than that with separable NV centers. Our results pave the way for new applications in nanoscale nuclear magnetic resonance spectroscopy.
Quantum sensing has witnessed rapid development and transition from laboratories to practical applications in the past decade. Applications of quantum sensors, ranging from nanotechnologies to biosensing, are expected to benefit from quantum sensors' unprecedented spatial resolution and sensitivity. Solid-state spin systems are particularly attractive platforms for quantum sensing technologies because room temperature operation is viable while reaching the quantum limits of sensitivity. Among various solid-state spin systems, nitrogen-vacancy (NV) centers in diamond demonstrated high-fidelity initialization, coherent control, and high contrast readout of the electron spin state. However, electron spin coherence due to noise from the surrounding spin bath and this environment effect limits the sensitivity of NV centers. Thus, a critical task in NV center-based quantum sensing is sensitivity enhancement through coherence protection. Several strategies, such as dynamical decoupling techniques, feedback control, and nuclear spin-assisted sensing protocols, have been developed and realized for this task. Among these strategies, nuclear spin-assisted protocols have demonstrated greater enhancement of electron spin coherence. In addition, the electron and nuclear spin pair of an NV center in diamond naturally allows the application of the nuclear spin-assisted sensitivity enhancement protocol. Owing to long nuclear coherence times, further enhancement of sensitivity can be achieved by exploiting active nuclear spins (e.g., 14N, 13C) in the proximity of an NV center as memory ancillas when coupled with the NV center. Here, we review the spin properties of NV centers, mechanisms of the nuclear spin-assisted protocol and its gate variation, and the status of quantum sensing applications in high-resolution nuclear spin spectroscopy, atomic imaging, and magnetic field sensing. We discuss the potential for commercialization, current challenges in sensitivity enhancement, and conclude with future research directions for promoting the development of nuclear spin-assisted protocol and its integration into industrial applications.
Nuclear magnetic resonance (NMR) spectroscopy is widely used in fields ranging from chemistry, materials science to neuroscience. Nanoscale NMR spectroscopy using Nitrogen-vacancy (NV) centers in diamond has emerged as a promising platform due to an unprecedented sensitivity down to the single spin level. At the nanoscale, high nuclear spin polarization through spin fluctuations (statistical polarization) far outweighs thermal polarization. However, until now efficient NMR detection using coherent averaging techniques could not be applied to the detection of statistical polarization, leading to long measurement times. Here we present two protocols to enable coherent averaging of statistically oscillating signals through rectification. We demonstrate these protocols on an artificial radiofrequency signal detected with a single NV center at 2.7 T. The signal-to-noise scaling with number of measurements 𝑁 increases from 𝑁0.5 to 𝑁1, improving the measurement time significantly. The relevance of rectification for the detection of statistically polarized nuclear spins using ensembles of NV centers is outlined, paving the way for efficient nanoscale NMR spectroscopy.
Two-dimensional Nuclear Magnetic Resonance (NMR) is essential in molecular structure determination. The Nitrogen-Vacancy (NV) center in diamond has been proposed and developed as an outstanding quantum sensor to realize NMR in nanoscale. In this work, we develop a scheme for two-dimensional nanoscale NMR spectroscopy based on quantum controls on an NV center. We carry out a proof of principle experiment on a target of two coupled 13C nuclear spins in diamond. A COSY-like sequences is used to acquire the data on time domain, which is then converted to frequency domain with the fast Fourier transform (FFT). With the two-dimensional NMR spectrum, the structure and location of the set of nuclear spin are resolved. This work marks a fundamental step towards resolving the structure of a single molecule.
Abstract 2D nuclear magnetic resonance (NMR) is essential in molecular structure determination. The nitrogen vacancy (NV) center in diamond is proposed and developed as an outstanding quantum sensor to realize NMR in nanoscale. In this work, a scheme for 2D nanoscale NMR spectroscopy is developed based on quantum controls on an NV center. A proof‐of‐principle experiment on a target of two coupled nuclear spins in diamond is carried out. A correlation spectroscopy (COSY) like sequence is used to acquire the data on time domain, which is then converted to frequency domain with the fast Fourier transform. With the 2D NMR spectrum, the structure and location of the set of nuclear spin are resolved. This work marks a fundamental step toward resolving the structure of a single molecule.
Defect centers in diamond are exceptional solid-state quantum systems that can have exceedingly long electron and nuclear spin coherence times. So far, single-qubit gates for the nitrogen nuclear spin, a two-qubit gate with a nitrogen-vacancy (NV) center electron spin, and entanglement between nearby nitrogen nuclear spins have been demonstrated. Here, we develop a scheme to implement a universal two-qubit gate between two distant nitrogen nuclear spins. Virtual excitation of an NV center that is embedded in an optical cavity can scatter a laser photon into the cavity mode; we show that this process depends on the nuclear spin state of the nitrogen atom. If two NV centers are simultaneously coupled to a common cavity mode and individually excited, virtual cavity photon exchange can mediate an effective interaction between the nuclear spin qubits, conditioned on the spin state of both nuclei, which implements a universal controlled-Z gate. We predict operation times below $10\phantom{\rule{0.16em}{0ex}}\ensuremath{\mu}\mathrm{s}$, which is four orders of magnitude faster than the decoherence time of nuclear spin qubits in diamond.
The recent decade has witnessed exciting developments in quantum science and technology. Quantum sensing is a rapidly growing branch, which exploits the fragility of quantum systems to detect small external signals. The extreme control at the single-atom level and the remarkably long coherence time of engineered quantum systems enable unprecedented sensitivity and precision, beating the performance of classical techniques. The nitrogen-vacancy (NV) center in diamond is one of the most promising quantum sensors. Its unique advantages have attracted considerable attention, including a long spin coherence time throughout a broad temperature range, nanoscale resolution limited by the sensor-sample distance, convenient optical control of its spin states and remarkably versatile sensing capabilities. Its properties are well studied under a bias magnetic field oriented along its quantization axis. However, its sensing capabilities in the presence of an off-axis magnetic field are much less explored. My research aims to unlock the full potential of NV quantum sensor by developing new sensing modalities under a magnetic field acting perpendicular to the NV axis, and furthermore, integrating them into a scanning probe microscope. In this dissertation, I will report our progress toward building a scanning NV multimodal quantum imaging platform, which will open up exciting opportunities in measuring nanoscale phenomena. The first chapter provides an introduction to the background of quantum sensing with NV centers, followed by a discussion on its basic properties and established sensing techniques. The second and third chapters are dedicated to two experiments performed under a perpendicular magnetic field where traditional NV magnetometry based on the Zeeman effect fails. In the second chapter, I will introduce a new sensing strategy that uses the entanglement between the electron and nuclear spins to restore the magnetic field sensitivity under this unfavored condition. This allows us to sense small changes in the magnetic field angle relative to the NV axis, and to detect anisotropic magnetic noise in the local environment. In the third chapter, I will present our latest development of scanning NV electrometry, where a single NV at the apex of a diamond scanning probe images external alternating (AC) and direct (DC) electric fields with sub-100 nm resolution. In the last chapter, I will discuss our efforts on four experiments that were left unfinished. I will present the results we have achieved, analyze the challenges that we faced and propose potential solutions to overcome them.