Magnetometers based on nitrogen-vacancy (NV) centers in diamond are promising room-temperature, solidstate sensors. However, their reported sensitivity to magnetic fields at low frequencies (1 kHz) is presently 10 pT s 1/2 , precluding potential applications in medical imaging, geoscience, and navigation. Here we show that high-permeability magnetic flux concentrators, which collect magnetic flux from a larger area and concentrate it into the diamond sensor, can be used to improve the sensitivity of diamond magnetometers. By inserting an NV-doped diamond membrane between two ferrite cones in a bowtie configuration, we realize a ∼250-fold increase of the magnetic field amplitude within the diamond. We demonstrate a sensitivity of ∼0.9 pT s 1/2 to magnetic fields in the frequency range between 10 and 1000 Hz. This is accomplished using a dual-resonance modulation technique to suppress the effect of thermal shifts of the NV spin levels. The magnetometer uses 200 mW of laser power and 20 mW of microwave power. This work introduces a new degree of freedom for the design of diamond sensors by using structured magnetic materials to manipulate magnetic fields.

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 × 1012 19F spins in a 1 pl volume can be detected with a signal-to-noise ratio of 3 in 1 s of integration.

Quantum sensors based on nitrogen-vacancy centers in diamond have emerged as a promising detection modality for nuclear magnetic resonance (NMR) spectroscopy owing to their micrometer-scale detection volume and noninductive-based detection. A remaining challenge is to realize sufficiently high spectral resolution and concentration sensitivity for multidimensional NMR analysis of picoliter sample volumes. Here, we address this challenge by spatially separating the polarization and detection phases of the experiment in a microfluidic platform. We realize a spectral resolution of 0.65 ± 0.05 Hz, an order-of-magnitude improvement over previous diamond NMR studies. We use the platform to perform two-dimensional correlation spectroscopy of liquid analytes within an effective ∼40-picoliter detection volume. The use of diamond quantum sensors as in-line microfluidic NMR detectors is a major step toward applications in mass-limited chemical analysis and single-cell biology.

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.

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Microcavity surface plasmon resonance sensors (MSPRSs) develop out of the classic surface plasmon resonance technologies and aim at producing novel lab-on-a-chip devices. MSPRSs generate a series of spectral resonances sensitive to minute changes in the refractive index. Related sensitivity studies and biosensing applications are published elsewhere. The goal of this work is to test the hypothesis that MSPRS resonances are standing surface plasmon waves excited at the surface of the sensor that decay back into propagating photons. Their optical properties (mean wavelength, peak width, and peak intensity) appear highly dependent on the internal morphology of the sensor and the underlying subwavelength aperture architecture in particular. Numerous optical experiments were designed to investigate trends that confirm this hypothesis. An extensive study of prior works was supportive of our findings and interpretations. A complete understanding of those mechanisms and parameters driving the formations of the MSPRS resonances would allow further improvement in sensor sensitivity, reliability, and manufacturability.

Radio frequency (RF) magnetometers based on nitrogen vacancy centers in diamond are predicted to offer femtotesla sensitivity, but previous experiments were limited to the picotesla level. We demonstrate a femtotesla RF magnetometer using a diamond membrane inserted between ferrite flux concentrators. The device provides ~300-fold amplitude enhancement for RF magnetic fields from 70 kHz to 3.6 MHz, and the sensitivity reaches ~70 fT√s at 0.35 MHz. The sensor detected the 3.6-MHz nuclear quadrupole resonance (NQR) of room-temperature sodium nitrite powder. The sensor’s recovery time after an RF pulse is ~35 μs, limited by the excitation coil’s ring-down time. The sodium-nitrite NQR frequency shifts with temperature as −1.00±0.02 kHz/K, the magnetization dephasing time is T 2 *=887±51 μs, and multipulse sequences extend the signal lifetime to 332±23 ms, all consistent with coil-based studies. Our results expand the sensitivity frontier of diamond magnetometers to the femtotesla range, with potential applications in security, medical imaging, and materials science.

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