skip to main content


This content will become publicly available on July 1, 2024

Title: Optical and electronic spin properties of fluorescent micro- and nanodiamonds upon prolonged ultrahigh-temperature annealing
High-temperature annealing is a promising but still mainly unexplored method for enhancing spin properties of negatively charged nitrogen-vacancy (NV) centers in diamond particles. After high-energy irradiation, the formation of NV centers in diamond particles is typically accomplished via annealing at temperatures in the range of 800–900 °C for 1–2 h to promote vacancy diffusion. Here, we investigate the effects of conventional annealing (900 °C for 2 h) against annealing at a much higher temperature of 1600 °C for the same annealing duration for particles ranging in size from 100 nm to 15 μm using electron paramagnetic resonance and optical characterization. At this high temperature, the vacancy-assisted diffusion of nitrogen can occur. Previously, the annealing of diamond particles at this temperature was performed over short time scales because of concerns of particle graphitization. Our results demonstrate that particles that survive this prolonged 1600 °C annealing show increased NV T1 and T2 electron spin relaxation times in 1 and 15 μm particles, due to the removal of fast relaxing spins. Additionally, this high-temperature annealing also boosts magnetically induced fluorescence contrast of NV centers for particle sizes ranging from 100 nm to 15 μm. At the same time, the content of NV centers is decreased fewfold and reaches a level of <0.5 ppm. The results provide guidance for future studies and the optimization of high-temperature annealing of fluorescent diamond particles for applications relying on the spin properties of NV centers in the host crystals.  more » « less
Award ID(s):
2203904 1914945
NSF-PAR ID:
10428458
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ;
Date Published:
Journal Name:
Journal of Vacuum Science & Technology B
Volume:
41
Issue:
4
ISSN:
2166-2746
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. A broad effort is underway to improve the sensitivity of NMR through the use of dynamic nuclear polarization. Nitrogen vacancy (NV) centers in diamond offer an appealing platform because these paramagnetic defects can be optically polarized efficiently at room temperature. However, work thus far has been mainly limited to single crystals, because most polarization transfer protocols are sensitive to misalignment between the NV and magnetic field axes. Here we study the spin dynamics of NV−13C pairs in the simultaneous presence of optical excitation and microwave frequency sweeps at low magnetic fields. We show that a subtle interplay between illumination intensity, frequency sweep rate, and hyperfine coupling strength leads to efficient, sweep-direction-dependent13C spin polarization over a broad range of orientations of the magnetic field. In particular, our results strongly suggest that finely tuned, moderately coupled nuclear spins are key to the hyperpolarization process, which makes this mechanism distinct from other known dynamic polarization channels. These findings pave the route to applications where powders are intrinsically advantageous, including the hyperpolarization of target fluids in contact with the diamond surface or the use of hyperpolarized particles as contrast agents for in vivo imaging.

     
    more » « less
  2. The use of fluorescence microscopy to study fate and transport of nanoparticles in the environment can be limited by the presence of confounding background signals such as autofluorescence and scattered light. The unique spin-related luminescence properties of nitrogen vacancy (NV) centers in diamond nanoparticles (NVND) enable new types of imaging modalities such as selective imaging of nanoparticles in the presence of background fluorescence. These techniques make use of the fact that the spin properties, which affect the fluorescence of NV centers, can be modulated using applied magnetic or radio-frequency fields. This work presents the use magnetic fields to modulate the fluorescence of NVND for background-subtracted imaging of nanoparticles ingested by a model organism, C. elegans . With the addition of modest time-modulated magnetic fields from an inexpensive “hobby” electromagnet, the fluorescence of 40 nm NVND can be modulated by 10% in a widefield imaging configuration. Herein, differential magnetic imaging is used to image and to isolate the fluorescence arising from nanodiamond within the gut of the organism C. elegans . This method represents a promising approach to probing the uptake of nanoparticles by organisms and to assessing the movement and interactions of nanoparticles in biological systems. 
    more » « less
  3. Color-center–hosting semiconductors are emerging as promising source materials for low-field dynamic nuclear polarization (DNP) at or near room temperature, but hyperfine broadening, susceptibility to magnetic field heterogeneity, and nuclear spin relaxation induced by other paramagnetic defects set practical constraints difficult to circumvent. Here, we explore an alternate route to color-center–assisted DNP using nitrogen-vacancy (NV) centers in diamond coupled to substitutional nitrogen impurities, the so-called P1 centers. Working near the level anticrossing condition—where the P1 Zeeman splitting matches one of the NV spin transitions—we demonstrate efficient microwave-free 13 C DNP through the use of consecutive magnetic field sweeps and continuous optical excitation. The amplitude and sign of the polarization can be controlled by adjusting the low-to-high and high-to-low magnetic field sweep rates in each cycle so that one is much faster than the other. By comparing the 13 C DNP response for different crystal orientations, we show that the process is robust to magnetic field/NV misalignment, a feature that makes the present technique suitable to diamond powders and settings where the field is heterogeneous. Applications to shallow NVs could capitalize on the greater physical proximity between surface paramagnetic defects and outer nuclei to efficiently polarize target samples in contact with the diamond crystal. 
    more » « less
  4. Abstract

    Nitrogen vacancy (NV) centers, optically active atomic defects in diamond, have attracted tremendous interest for quantum sensing, network, and computing applications due to their excellent quantum coherence and remarkable versatility in a real, ambient environment. Taking advantage of these strengths, this paper reports on NV‐based local sensing of the electrically driven insulator‐to‐metal transition (IMT) in a proximal Mott insulator. The resistive switching properties of both pristine and ion‐irradiated VO2thin film devices are studied by performing optically detected NV electron spin resonance measurements. These measurements probe thelocaltemperature and magnetic field in electrically biased VO2devices, which are in agreement with theglobaltransport measurement results. In pristine devices, the electrically driven IMT proceeds through Joule heating up to the transition temperature while in ion‐irradiated devices, the transition occurs nonthermally, well below the transition temperature. The results provide direct evidence for nonthermal electrically induced IMT in a Mott insulator, highlighting the significant opportunities offered by NV quantum sensors in exploring nanoscale thermal and electrical behaviors in Mott materials.

     
    more » « less
  5. null (Ed.)
    Multimodal imaging—the ability to acquire images of an object through more than one imaging mode simultaneously—has opened additional perspectives in areas ranging from astronomy to medicine. In this paper, we report progress toward combining optical and magnetic resonance (MR) imaging in such a “dual” imaging mode. They are attractive in combination because they offer complementary advantages of resolution and speed, especially in the context of imaging in scattering environments. Our approach relies on a specific material platform, microdiamond particles hosting nitrogen vacancy (NV) defect centers that fluoresce brightly under optical excitation and simultaneously “hyperpolarize” lattice C 13 nuclei, making them bright under MR imaging. We highlight advantages of dual-mode optical and MR imaging in allowing background-free particle imaging and describe regimes in which either mode can enhance the other. Leveraging the fact that the two imaging modes proceed in Fourier-reciprocal domains (real and k-space), we propose a sampling protocol that accelerates image reconstruction in sparse-imaging scenarios. Our work suggests interesting possibilities for the simultaneous optical and low-field MR imaging of targeted diamond nanoparticles. 
    more » « less