We present an experimental and theoretical study of the optically detected magnetic resonance signals for ensembles of negatively charged nitrogen-vacancy (NV) centers in a C13 isotopically enriched single-crystal diamond. We observe four broad transition peaks with superimposed sharp features at zero magnetic field and study their dependence on an applied magnetic field. A theoretical model that reproduces all qualitative features of these spectra is developed. Understanding the magnetic-resonance spectra of NV centers in an isotopically enriched diamond is important for emerging applications in nuclear magnetic resonance.

Electron spin resonance (ESR) describes a suite of techniques for characterizing electronic systems with applications in physics, chemistry, and biology. However, the requirement for large electron spin ensembles in conventional ESR techniques limits their spatial resolution. Here we present a method for measuring ESR spectra of nanoscale electronic environments by measuring the longitudinal relaxation time of a single-spin probe as it is systematically tuned into resonance with the target electronic system. As a proof of concept, we extracted the spectral distribution for the P1 electronic spin bath in diamond by using an ensemble of nitrogen-vacancy centres, and demonstrated excellent agreement with theoretical expectations. As the response of each nitrogen-vacancy spin in this experiment is dominated by a single P1 spin at a mean distance of 2.7 nm, the application of this technique to the single nitrogen-vacancy case will enable nanoscale ESR spectroscopy of atomic and molecular spin systems.

The readout of negatively charged nitrogen-vacancy centre electron spins is essential for applications in quantum computation, metrology and sensing. Conventional readout protocols are based on the detection of photons emitted from nitrogen-vacancy centres, a process limited by the efficiency of photon collection. We report on an alternative principle for detecting the magnetic resonance of nitrogen-vacancy centres, allowing the direct photoelectric readout of nitrogen-vacancy centres spin state in an all-diamond device. The photocurrent detection of magnetic resonance scheme is based on the detection of charge carriers promoted to the conduction band of diamond by two-photon ionization of nitrogen-vacancy centres. The optical and photoelectric detection of magnetic resonance are compared, by performing both types of measurements simultaneously. The minima detected in the measured photocurrent at resonant microwave frequencies are attributed to the spin-dependent ionization dynamics of nitrogen-vacancy, originating from spin-selective non-radiative transitions to the metastable singlet state.

We present systematic measurements of longitudinal relaxation rates (1 / T 1) of spin polarization in the ground state of the nitrogen-vacancy (NV-) color center in synthetic diamond as a function of NV- concentration and magnetic field B. NV- centers were created by irradiating a Type 1b single-crystal diamond along the [100] axis with 200 keV electrons from a transmission electron microscope with varying doses to achieve spots of different NV- center concentrations. Values of (1 / T 1) were measured for each spot as a function of B.

Magnetic microscopy of malarial hemozoin nanocrystals is performed by optically detected magnetic resonance imaging of near-surface diamond nitrogen-vacancy centers. Hemozoin crystals are extracted from Plasmodium falciparum-infected human blood cells and studied alongside synthetic hemozoin crystals. The stray magnetic fields produced by individual crystals are imaged at room temperature as a function of the applied field up to 350 mT. More than 100 nanocrystals are analyzed, revealing the distribution of their magnetic properties. Most crystals (96%) exhibit a linear dependence of the stray-field magnitude on the applied field, confirming hemozoin's paramagnetic nature. A volume magnetic susceptibility of 3.4 × 10-4 is inferred with use of a magnetostatic model informed by correlated scanning-electron-microscopy measurements of crystal dimensions. A small fraction of nanoparticles (4/82 for Plasmodium falciparum-produced nanoparticles and 1/41 for synthetic nanoparticles) exhibit a saturation behavior consistent with superparamagnetism. Translation of this platform to the study of living Plasmodium-infected cells may shed new light on hemozoin formation dynamics and their interaction with antimalarial drugs.

We use magnetic-field-dependent features in the photoluminescence of negatively charged nitrogen-vacancy centers to measure magnetic fields without the use of microwaves. In particular, we present a magnetometer based on the level anti-crossing in the triplet ground state at 102.4 mT with a demonstrated noise floor of 6 nT/ Hz, limited by the intensity noise of the laser and the performance of the background-field power supply. The technique presented here can be useful in applications where the sensor is placed close to conductive materials, e.g., magnetic induction tomography or magnetic field mapping, and in remote-sensing applications since principally no electrical access is needed.

Characterizing the local internal environment surrounding solid-state spin defects is crucial to harnessing them as nanoscale sensors of external fields. This is especially germane to the case of defect ensembles which can exhibit a complex interplay between interactions, internal fields, and lattice strain. Working with the nitrogen-vacancy (NV) center in diamond, we demonstrate that local electric fields dominate the magnetic resonance behavior of NV ensembles at a low magnetic field. We introduce a simple microscopic model that quantitatively captures the observed spectra for samples with NV concentrations spanning more than two orders of magnitude. Motivated by this understanding, we propose and implement a novel method for the nanoscale localization of individual charges within the diamond lattice; our approach relies upon the fact that the charge induces a NV dark state which depends on the electric field orientation.

Sensors using nitrogen-vacancy centers in diamond are a promising tool for small-volume nuclear magnetic resonance (NMR) spectroscopy, but the limited sensitivity remains a challenge. Here we show nearly two orders of magnitude improvement in concentration sensitivity over previous nitrogen-vacancy and picoliter NMR studies. We demonstrate NMR spectroscopy of picoliter-volume solutions using a nanostructured diamond chip with dense, high-aspect-ratio nanogratings, enhancing the surface area by 15 times. The nanograting sidewalls are doped with nitrogen-vacancies located a few nanometers from the diamond surface to detect the NMR spectrum of roughly 1 pl of fluid lying within adjacent nanograting grooves. We perform ¹H and ¹⁹F nuclear magnetic resonance spectroscopy at room temperature in magnetic fields below 50 mT. Using a solution of CsF in glycerol, we determine that 4 ± 2 × 10^{12 19}F spins in a 1 pl volume can be detected with a signal-to-noise ratio of 3 in 1 s of integration.