Super-Resolution Diamond Magnetic Microscopy of Superparamagnetic Nanoparticles.

Scanning-probe and wide-field magnetic microscopes based on nitrogen-vacancy (NV) centers in diamond have enabled advances in the study of biology and materials, but each method has drawbacks. Here, we implement an alternative method for nanoscale magnetic microscopy based on optical control of the charge state of NV centers in a dense layer near the diamond surface. By combining a donut-beam super-resolution technique with optically detected magnetic resonance spectroscopy, we imaged the magnetic fields produced by single 30 nm iron-oxide nanoparticles. The magnetic microscope has a lateral spatial resolution of ∼100 nm, and it resolves the individual magnetic dipole features from clusters of nanoparticles with interparticle spacings down to ∼190 nm. The magnetic feature amplitudes are more than an order of magnitude larger than those obtained by confocal magnetic microscopy due to the narrower optical point-spread function and the shallow depth of NV centers. We analyze the magnetic nanoparticle images and sensitivity as a function of the microscope's spatial resolution and show that the signal-to-noise ratio for nanoparticle detection does not degrade as the spatial resolution improves. We identify sources of background fluorescence that limit the present performance, including diamond second-order Raman emission and imperfect NV charge state control. Our method, which uses <10 mW laser power and can be parallelized by patterned illumination, introduces a promising format for nanoscale magnetic imaging.

Super-resolution diamond magnetic microscopy of superparamagnetic nanoparticles.

Scanning-probe and wide-field magnetic microscopes based on Nitrogen-Vacancy (NV) centers in diamond have enabled remarkable advances in the study of biology and materials, but each method has drawbacks. Here, we implement an alternative method for nanoscale magnetic microscopy based on optical control of the charge state of NV centers in a dense layer near the diamond surface. By combining a donut-beam super-resolution technique with optically detected magnetic resonance spectroscopy, we imaged the magnetic fields produced by single 30-nm iron-oxide nanoparticles. The magnetic microscope has a lateral spatial resolution of ~100 nm, and it resolves the individual magnetic dipole features from clusters of nanoparticles with interparticle spacings down to ~190 nm. The magnetic feature amplitudes are more than an order of magnitude larger than those obtained by confocal magnetic microscopy due to the smaller characteristic NV-nanoparticle distance within nearby sensing voxels. We analyze the magnetic point-spread function and sensitivity as a function of the microscope's spatial resolution and identify sources of background fluorescence that limit the present performance, including diamond second-order Raman emission and imperfect NV charge-state control. Our method, which uses less than 10 mW laser power and can be parallelized by patterned illumination, introduces a new format for nanoscale magnetic imaging.

Nuclear quadrupole resonance spectroscopy with a femtotesla diamond magnetometer.

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 T2*=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.

Electric current paths in a Si:P delta-doped device imaged by nitrogen-vacancy diamond magnetic microscopy.

The recently-developed ability to control phosphorous-doping of silicon at an atomic level using scanning tunneling microscopy, a technique known as atomic precision advanced manufacturing (APAM), has allowed us to tailor electronic devices with atomic precision, and thus has emerged as a way to explore new possibilities in Si electronics. In these applications, critical questions include where current flow is actually occurring in or near APAM structures as well as whether leakage currents are present. In general, detection and mapping of current flow in APAM structures are valuable diagnostic tools to obtain reliable devices in digital-enhanced applications. In this paper, we used nitrogen-vacancy (NV) centers in diamond for wide-field magnetic imaging (with a few-mm field of view and micron-scale resolution) of magnetic fields from surface currents flowing in an APAM test device made of a P delta-doped layer on a Si substrate, a standard APAM witness material. We integrated a diamond having a surface NV ensemble with the device (patterned in two parallel mm-sized ribbons), then mapped the magnetic field from the DC current injected in the APAM device in a home-built NV wide-field microscope. The 2D magnetic field maps were used to reconstruct the surface current densities, allowing us to obtain information on current paths, device failures such as choke points where current flow is impeded, and current leakages outside the APAM-defined P-doped regions. Analysis on the current density reconstructed map showed a projected sensitivity of ∼0.03 A m-1, corresponding to a smallest-detectable current in the 200µm wide APAM ribbon of ∼6µA. These results demonstrate the failure analysis capability of NV wide-field magnetometry for APAM materials, opening the possibility to investigate other cutting-edge microelectronic devices.

Diamond magnetometer enhanced by ferrite flux concentrators.

Magnetometers based on nitrogen-vacancy (NV) centers in diamond are promising room-temperature, solid-state sensors. However, their reported sensitivity to magnetic fields at low frequencies (≾1 kHz) is presently ≿10 pT s1/2, 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 s1/2 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.

Two-dimensional nuclear magnetic resonance spectroscopy with a microfluidic diamond quantum sensor.

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.

Diamond Magnetic Microscopy of Malarial Hemozoin Nanocrystals.

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.