Over the years, an enormous effort has been made to establish nitrogen vacancy (N-V) centers in diamond as easily accessible and precise magnetic field sensors. However, most of their sensing protocols rely on the application of bias magnetic fields, preventing their usage in zero- or low-field experiments. We overcome this limitation by exploiting the full spin S=1 nature of the N-V center, allowing us to detect nuclear spin signals at zero and low field with a linearly polarized microwave field. As conventional dynamical decoupling protocols fail in this regime, we develop robust pulse sequences and optimize pulse pairs, which allow us to sense temperature and weak ac magnetic fields and achieve an efficient decoupling from environmental noise. Our work allows for much broader and simpler applications of N-V centers as magnetic field sensors in the zero- and low-field regime and can be further extended to three-level systems in ions and atoms.

Nuclear spin hyperpolarization provides a promising route to overcome the challenges imposed by the limited sensitivity of nuclear magnetic resonance. Here we demonstrate that dissolution of spin-polarized pentacene-doped naphthalene crystals enables transfer of polarization to target molecules via intermolecular cross-relaxation at room temperature and moderate magnetic fields (1.45 T). This makes it possible to exploit the high spin polarization of optically polarized crystals, while mitigating the challenges of its transfer to external nuclei. With this method, we inject the highly polarized mixture into a benchtop NMR spectrometer and observe the polarization dynamics for target ¹H nuclei. Although the spectra are radiation damped due to the high naphthalene magnetization, we describe a procedure to process the data to obtain more conventional NMR spectra and extract the target nuclei polarization. With the entire process occurring on a time scale of 1 min, we observe NMR signals enhanced by factors between −200 and −1730 at 1.45 T for a range of small molecules.

We engineer an artificial optical clock transition in ⁴⁰Ca⁺ with a continuous dynamical decoupling scheme. It suppresses inhomogeneous tensor shifts as well as the linear Zeeman shift, making it suitable for multi-ion operation. Coherence times approaching the natural lifetime limit ensure low statistical uncertainties on the optical transition. We continuously apply the dressing fields, making the tailored transition robust against magnetic field fluctuations during the entire clock probe time.

Conventional control strategies for nitrogen-vacancy centers in quantum sensing are based on a two-level model of their triplet ground state. However, this approach fails in regimes of weak bias magnetic fields or strong microwave pulses, as we demonstrate. To overcome this limitation, we propose a novel control sequence that exploits all three levels by addressing a hidden Raman configuration with microwave pulses tuned to the zero-field transition. We report excellent performance in typical dynamical decoupling sequences, opening up the possibility for nano-NMR operation in low field environments.

Precise frequency measurements are important in applications ranging from navigation and imaging to computation and communication. Here we outline the optimal quantum strategies for frequency discrimination and estimation in the context of quantum spectroscopy, and we compare the effectiveness of different readout strategies. Using a single NV center in diamond, we implement the optimal frequency discrimination protocol to discriminate two frequencies separated by 2 kHz with a single 44 μs measurement, a factor of ten below the Fourier limit. For frequency estimation, we achieve a frequency sensitivity of 1.6 µHz/Hz² for a 1.7 µT amplitude signal, which is within a factor of 2 from the quantum limit. Our results are foundational for discrimination and estimation problems in nanoscale nuclear magnetic resonance spectroscopy.

Precise frequency measurements are important in applications ranging from navigation and imaging to computation and communication. Here we outline the optimal quantum strategies for frequency discrimination and estimation in the context of quantum spectroscopy, and we compare the effectiveness of different readout strategies. Using a single NV center in diamond, we implement the optimal frequency discrimination protocol to discriminate two frequencies separated by 2 kHz with a single 44 μs measurement, a factor of ten below the Fourier limit. For frequency estimation, we achieve a frequency sensitivity of 1.6 µHz/Hz² for a 1.7 µT amplitude signal, which is within a factor of 2 from the quantum limit. Our results are foundational for discrimination and estimation problems in nanoscale nuclear magnetic resonance spectroscopy.

Precise spectroscopy of oscillating fields plays a significant role in many fields. Here, we propose an experimentally feasible scheme to measure the frequency of a fast-oscillating field using a single-qubit sensor. By invoking a stable classical clock, the signal phase correlations between successive measurements enable us to extract the target frequency with extremely high precision. In addition, we integrate dynamical decoupling technique into the framework to suppress the influence of slow environmental noise. Our framework is feasible with a variety of atomic and single solid-state spin systems within the state-of-the-art experimental capabilities as a versatile tool for quantum spectroscopy.

Diffusion broadening of spectral lines is the main limitation to frequency resolution in non-polarized liquid state nano-NMR. This problem arises from the limited amount of information that can be extracted from the signal before losing coherence. For liquid state NMR as with most generic sensing experiments, the signal is thought to decay exponentially, severely limiting resolution. However, there is theoretical evidence that predicts a power law decay of the signal’s correlations due to diffusion noise in the non-polarized nano-NMR scenario. In this work we show that in the NV based nano-NMR setup such diffusion noise results in high spectral resolution.

The ultimate precision limit in estimating the Larmor frequency of N unentangled qubits is well established, and is highly important for magnetometers, gyroscopes, and other types of quantum sensors. However, this limit assumes perfect projective measurements of the quantum registers. This requirement is not practical in many physical systems, such as NMR spectroscopy, where a weakly interacting external probe is used as a measurement device. Here, we show that in the framework of quantum nano-NMR spectroscopy, in which these limitations are inherent, the ultimate precision limit is still achievable using control and a finely tuned measurement.

The NV-NMR spectrometer is a promising candidate for detection of NMR signals at the nanoscale. Field inhomogeneities, however, are a major source of noise that limits spectral resolution in state of the art NV-NMR experiments and constitutes a major bottleneck in the development of nanoscale NMR. Here we propose, a route in which this limitation could be circumvented in NV-NMR spectrometer experiments, by utilizing the nanometric scale and the quantumness of the detector.

We propose a scheme for sensing of an oscillating field in systems with large inhomogeneous broadening and driving field variation by applying sequences of phased, adiabatic, chirped pulses. These act as a double filter for dynamical decoupling, where the adiabatic changes of the mixing angle during the pulses rectify the signal and partially remove frequency noise. The sudden changes between the pulses act as instantaneous π pulses in the adiabatic basis for additional noise suppression. We also use the pulses' phases to correct for other errors, e.g., due to nonadiabatic couplings. Our technique improves significantly the coherence time in comparison to standard XY8 dynamical decoupling in realistic simulations in NV centers with large inhomogeneous broadening. Beyond the theoretical proposal, we also present proof-of-principle experimental results for quantum sensing of an oscillating field in NV centers in diamond, demonstrating superior performance compared to the standard technique.

Nano nuclear magnetic resonance (nano‐NMR) spectroscopy with nitrogen‐vacancy (NV) centers holds the potential to provide high‐resolution spectra of minute samples. This is likely to have important implications for chemistry, medicine, and pharmaceutical engineering. One of the main hurdles facing the technology is that diffusion of unpolarized liquid samples broadens the spectral lines thus limiting resolution. Experiments in the field are therefore impeded by the efforts involved in achieving high polarization of the sample which is a challenging endeavor. Here, a scenario where the liquid is confined to a small volume is examined. It is shown that the confinement “counteracts” the effect of diffusion, thus overcoming a major obstacle to the resolving abilities of the NV‐NMR spectrometer.

Because of its superior coherent and optical properties at room temperature, the nitrogen-vacancy (N-V) center in diamond has become a promising quantum probe for nanoscale quantum sensing. However, the application of N-V-containing nanodiamonds to quantum sensing suffers from their relatively short spin coherence times. Here we demonstrate energy-efficient protection of N-V spin coherence in nanodiamonds using concatenated continuous dynamical decoupling, which exhibits excellent performance with a less-stringent microwave-power requirement. When this is applied to nanodiamonds in living cells, we are able to extend the spin coherence time by an order of magnitude to the T1 limit of 30μs. Further analysis demonstrates concomitant improvements of sensing performance, which shows that our results provide an important step toward in vivo quantum sensing using N-V centers in nanodiamond.

Nitrogen-Vacancy (NV) centers in diamonds have been shown in recent years to be excellent magnetometers on the nanoscale. One of the recent applications of the quantum sensor is retrieving the Nuclear Magnetic Resonance (NMR) spectrum of a minute sample, whose net polarization is well below the Signal-to-Noise Ratio (SNR) of classic devices. The information in the magnetic noise of diffusing particles has also been shown in decoherence spectroscopy approaches to provide a method for measuring different physical parameters. Similar noise is induced on the NV center by a flowing liquid. However, when the noise created by diffusion effects is more dominant than the noise of the drift, it is unclear whether the velocity can be efficiently estimated. Here we propose a non-intrusive setup for measuring the drift velocity near the surface of a flow channel based on magnetic field quantum sensing using NV centers. We provide a detailed analysis of the sensitivity for different measurement protocols, and we show that our nanoscale velocimetry scheme outperforms current fluorescence based approaches even when diffusion noise is dominant. Our scheme can be applied for the investigation of microfluidic channels, where the drift velocity is usually low and the flow properties are currently unclear. A better understanding of these properties is essential for the future development of microfluidic and nanofluidic infrastructures.