High spatial resolution quantum sensing of near-surface nitrogen vacancy (NV) centers in diamond has enabled detection of magnetic, electrical, and thermal signals at the nanoscale. At depths of just a few nanometers, NV centers serve as localized quantum probes for external spins or low-dimensional materials, but their proximity to the surface also enhances decoherence caused by fluctuating nuclear spins. While advances in surface engineering have stabilized the charge state of NV centers at depths of tens of nanometers, achieving both ultra-shallow implantation (0.5-2 nm) and long-term spin coherence remains a central challenge. In this work, we show using first-principles modeling that, by exploiting the interaction of surface-induced strain and weak dc magnetic fields, the spin coherence times of 1-nm-deep NV centers can be greatly improved near the spin-phonon-confined regime at room temperature in 12C-rich diamonds. We also demonstrate that this protocol benefits ~ 10-nm-deep NV centers in natural diamond, enabling vector magnetometry at the nanoscale. Shallow NV centers in diamond are advantageous for quantum sensing but suffer from surface magnetic noise. Using first-principles simulations supported by experiments, the authors show that a combination of small magnetic fields and surface strain can significantly enhance spin coherence of 1 nm-deep NV centers.
High spatial resolution quantum sensing of near-surface nitrogen vacancy (NV) centers in diamond has enabled detection of magnetic, electrical, and thermal signals at the nanoscale. At depths of just a few nanometers, NV centers serve as localized quantum probes for external spins or low-dimensional materials, but their proximity to the surface also enhances decoherence caused by fluctuating nuclear spins. While advances in surface engineering have stabilized the charge state of NV centers at depths of tens of nanometers, achieving both ultra-shallow implantation (0.5-2 nm) and long-term spin coherence remains a central challenge. In this work, we show using first-principles modeling that, by exploiting the interaction of surface-induced strain and weak dc magnetic fields, the spin coherence times of 1-nm-deep NV centers can be greatly improved near the spin-phonon-confined regime at room temperature in 12C-rich diamonds. We also demonstrate that this protocol benefits ~ 10-nm-deep NV centers in natural diamond, enabling vector magnetometry at the nanoscale. Shallow NV centers in diamond are advantageous for quantum sensing but suffer from surface magnetic noise. Using first-principles simulations supported by experiments, the authors show that a combination of small magnetic fields and surface strain can significantly enhance spin coherence of 1 nm-deep NV centers.
We demonstrate nanometer-precision depth control of nitrogen-vacancy (NV) center creation near the surface of synthetic diamond using an in situ nitrogen delta-doping technique during plasma-enhanced chemical vapor deposition. Despite their proximity to the surface, doped NV centers with depths (d) ranging from 5 to 100 nm display long spin coherence times, T2 > 100 μs at d = 5 nm and T2 > 600 μs at d ≥ 50 nm. The consistently long spin coherence observed in such shallow NV centers enables applications such as atomic-scale external spin sensing and hybrid quantum architectures.
Engineering shallow nitrogen-vacancy (NV) centers in diamond holds the key to unlocking new advances in nanoscale quantum sensing. We find that the creation of near-surface NVs through delta doping during diamond growth allows for tunable control over both NV depth confinement (with a twofold improvement relative to low-energy ion implantation) and NV density, ultimately resulting in highly-sensitive single defects and ensembles with coherence limited by NV-NV interactions. Additionally, we demonstrate the utility of our shallow delta-doped NVs by imaging magnetism in few-layer CrSBr, a two-dimensional magnet. We anticipate that the control afforded by near-surface delta doping will enable new developments in NV quantum sensing from nanoscale NMR to entanglement-enhanced metrology.
Deploying nitrogen vacancy (NV) centers in diamond as nanoscale quantum sensors for condensed matter and materials physics requires placing the NV centers close to the sensing target. One solution is to fabricate diamond nanostructures and integrate them with materials and devices. However, diamond etching and ion milling can introduce subsurface damage and surface defects that degrade the charge stability and spin coherence of NV centers near the surface. Here we report a procedure for fabricating low-damage nanostructured diamond membranes, and we show that this fabrication scheme preserves the optical and spin properties of state-of-the-art shallow NV center quantum sensors, within nanometers of the diamond surface, while providing significant photonic enhancement. Furthermore, we demonstrate a pick-and-place transfer method, which enables integration with diverse sensing targets.
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.
Nitrogen vacancy (NV) color centers in diamond have shown great potential for various applications in quantum technology due to their long coherence times, high sensitivity to magnetic fields and atomic scale resolution. However, one major challenge in utilizing near surface NV centers is the decoherence caused by spins and charges fluctuating on the surface, which affects the spin properties of the sensors. To reduce the induced noise, various oxygen surface treatments such as low power oxygen plasma treatment and annealing under oxygen atmosphere have been explored to terminate the diamond surface and reduce its impact on NV coherence. We showed that the NV center’s coherence time can be enhanced up to a factor of 3 over a large spectral range of noise. Double electron–electron resonance measurements revealed an extra source of decoherence, scaling similarly as the P1 spin bath. The improvement in coherence times is accompanied with an increase in measured ketone/ether content and reduction of sp2 signal in x-ray photoelectron spectroscopy measurements. Finally we compared the performance of different NV ensembles and surface treatments for sensing external proton spins. The oxygen annealing is an effective procedure of enhancing the spin coherence times and reducing broad band spin noise experienced by shallow implanted ensemble NV centers in diamond.
In modern-day quantum metrology, quantum sensors are widely employed to detect weak magnetic fields or nanoscale signals. Quantum devices, exploiting quantum coherence, are inevitably connected to physical constants and can achieve accuracy, repeatability, and precision approaching fundamental limits. As a result, these sensors have shown utility in a wide range of research domains spanning both science and technology. A rapidly emerging quantum sensing platform employs atomic-scale defects in crystals. In particular, magnetometry using nitrogen-vacancy (NV) color centers in diamond has garnered increasing interest. NV systems possess a combination of remarkable properties, optical addressability, long coherence times, and biocompatibility. Sensors based on NV centers excel in spatial resolution and magnetic sensitivity. These diamond-based sensors promise comparable combination of high spatial resolution and magnetic sensitivity without cryogenic operation. The above properties of NV magnetometers promise increasingly integrated quantum measurement technology, as a result, they have been extensively developed with various protocols and find use in numerous applications spanning materials characterization, nuclear magnetic resonance (NMR), condensed matter physics, paleomagnetism, neuroscience and living systems biology, and industrial vector magnetometry. In this chapter, NV centers are explored for magnetic sensing in a number of contexts. In general, we introduce novel regimes for magnetic-field probes with NV ensembles. Specifically, NV centers are developed for sensitive magnetometers for applications where microwaves (MWs) are prohibitively invasive and operations need to be carried out under zero ambient magnetic field. The primary goal of our discussion is to improve the utility of these NV center-based magnetometers.