High contrast dual-mode optical and 13C magnetic resonance imaging in diamond particles
X. Lv, J. H. Walton, E. Druga, F. Wang, A. Aguilar, T. McKnelly, R. Nazaryan, F. L. Liu, L. Wu, O. Shenderova, D. B. Vigneron, C. A. Meriles, J. A. Reimer, A. Pines, A. Ajoy
Multichannel imaging -- the ability to acquire images of an object through more than one imaging mode simultaneously -- has opened interesting new perspectives in areas ranging from astronomy to medicine. Visible optics and magnetic resonance imaging (MRI) offer complementary advantages of resolution, speed and depth of penetration, and as such would be attractive in combination. In this paper, we take first steps towards marrying together optical and MR imaging in a class of biocompatible particulate materials constructed out of diamond. The particles are endowed with a high density of quantum defects (Nitrogen Vacancy centers) that under optical excitation fluoresce brightly in the visible, but also concurrently electron spin polarize. This allows the hyperpolarization of lattice 13C nuclei to make the particles over three-orders of magnitude brighter than in conventional MRI. Dual-mode optical and MR imaging permits immediate access to improvements in resolution and signal-to-noise especially in scattering environments. We highlight additional benefits in background-free imaging, demonstrating lock-in suppression by factors of 2 and 5 in optical and MR domains respectively. Ultimate limits could approach as much as two orders of magnitude in each domain. Finally, leveraging the ability of optical and MR imaging to simultaneously probe Fourier-reciprocal domains (real and k-space), we elucidate the ability to employ hybrid sub-sampling in both conjugate spaces to vastly accelerate dual-image acquisition, by as much as two orders of magnitude in practically relevant sparse-imaging scenarios. This is accompanied by a reduction in optical power by the same factor. Our work suggests interesting possibilities for the simultaneous optical and low-field MR imaging of targeted diamond nanoparticles.
A new pathway to nuclear magnetic resonance spectroscopy in high pressure diamond anvil cells is introduced, using inductively coupled broadband passive electro-magnetic lenses to locally amplify the magnetic flux at the isolated sample, leading to an increase in sensitivity. The lenses are adopted for the geometrical restrictions imposed by a toroidal diamond indenter cell, and yield high signal-to-noise ratios at pressures as high as 72 GPa, at initial sample volumes of only 230 pl. The corresponding levels of detection, LODt, are found to be up to four orders of magnitude lower compared to …
NV centers in diamond recommend themselves as good sensors of environmental fields as well as detectors of diamond impurities. In particular, C-centers, often also called ${{p}_{1}}$-centers, can be detected via double electron-electron resonance. This resonance can be used to measure the C-center concentration. Here, we measured the concentration of C-centers in several diamond plates and investigated the influence of the free precession time of the NV center on the observed contrast in the measured double electron-electron resonance spectrum. The dependence of the resonance amplitudes and wi…
Optically detected magnetic resonance of nitrogen vacancy centers in diamond offers novel routes to both DC and AC magnetometry in diamond anvil cells under high pressures ($>3$ GPa). However, a serious challenge to realizing experiments has been the insertion of microwave radiation in to the sample space without screening by the gasket material. We utilize designer anvils with lithographically-deposited metallic microchannels on the diamond culet as a microwave antenna. We detected the spin resonance of an ensemble of microdiamonds under pressure, and measure the pressure dependence of the ze…
A realization of the force-induced remnant magnetization spectroscopy (FIRMS) technique of specific biomolecular binding is presented where detection is accomplished with wide-field optical and diamond-based magnetometry using an ensemble of nitrogen-vacancy (NV) color centers. The technique may be adapted for massively parallel screening of arrays of nanoscale samples.
We present a novel technique based on an ensemble of Nitrogen-Vacancy (NV) centers in diamond to perform Magnetic Current Imaging (MCI) on an Integrated Circuit (IC). NV centers in diamond allow measuring the three components of the magnetic fields generated by a mA range current in an IC structure over a field of 50 x 200 μm^2 with sub-micron resolution. Vector measurements allow using a more robust algorithm than those used for MCI using Giant Magneto Resistance (GMR) or Superconducting Quantum Interference Device (SQUID) sensors and it is opening new current reconstruction prospects. Calcul…
We demonstrate a robust, scale-factor-free vector magnetometer, which uses a closed-loop frequency-locking scheme to simultaneously track Zeeman-split resonance pairs of nitrogen-vacancy (NV) centers in diamond. Compared with open-loop methodologies, this technique is robust against fluctuations in temperature, resonance linewidth, and contrast; offers a three-order-of-magnitude increase in dynamic range; and allows for simultaneous interrogation of multiple transition frequencies. By directly detecting the resonance frequencies of NV centers aligned along each of the diamond's four tetrahedra…
We demonstrate nuclear magnetic resonance (NMR) spectroscopy of picoliter-volume solutions with a nanostructured diamond chip. Using optical interferometric lithography, diamond surfaces were nanostructured with dense, high-aspect-ratio nanogratings, enhancing the surface area by more than a factor of 15 over mm^2 regions of the chip. The nanograting sidewalls were doped with nitrogen-vacancy (NV) centers so that more than 10 million NV centers in a (25 micrometer)^2 laser spot are located close enough to the diamond surface (5 nm) to detect the NMR spectrum of 1 pL of fluid lying within adjac…
We use electromagnetically-induced transparency (EIT) to probe the narrow electron-spin resonance of nitrogen-vacancy centers in diamond. Working with a multi-pass diamond chip at temperatures 6-30 K, the zero-phonon absorption line (637 nm) exhibits an optical depth of 6 and inhomogenous linewidth of ~30 GHz full-width-at-half-maximum (FWHM). Simultaneous optical excitation at two frequencies separated by the ground-state zero-field splitting (2.88 GHz), reveals EIT resonances with a contrast exceeding 6% and FWHM down to 0.4 MHz. The resonances provide an all-optical probe of external electr…
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 micron-scale detection volume and non-inductive 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, a…
The Zeeman splitting of a localized single spin can be used to construct a magnetometer allowing high precision measurements of magnetic fields with almost atomic spatial resolution. While sub-μT sensitivity can in principle be obtained using pulsed techniques and long measurement times, a fast and easy-to-use method without laborious data post-processing is desirable for a scanning-probe approach with high spatial resolution. In order to measure the resonance frequency in realtime, we applied a field-frequency lock to the continuous wave ODMR signal of a single electron spin in a nanodiamond.…
We provide an overview of the experimental techniques, measurement modalities, and diverse applications of the Quantum Diamond Microscope (QDM). The QDM employs a dense layer of fluorescent nitrogen-vacancy (NV) color centers near the surface of a transparent diamond chip on which a sample of interest is placed. NV electronic spins are coherently probed with microwaves and optically initialized and read out to provide spatially resolved maps of local magnetic fields. NV fluorescence is measured simultaneously across the diamond surface, resulting in a wide-field, two-dimensional magnetic field…
Magnetic imaging with ensembles of nitrogen-vacancy (NV) centres in diamond is a recently developed technique that allows for quantitative vector field mapping. Here we uncover a source of artefacts in the measured magnetic field in situations where the magnetic sample is placed in close proximity (a few tens of nm) to the NV sensing layer. Using magnetic nanoparticles as a test sample, we find that the measured field deviates significantly from the calculated field, in shape, amplitude and even in sign. By modelling the full measurement process, we show that these discrepancies are caused by …
