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Magnetometer with nitrogen-vacancy center in a bulk diamond for detecting magnetic nanoparticles in biomedical applications

MetadataDetails
Publication Date2020-02-12
JournalScientific Reports
AuthorsAkihiro Kuwahata, Takahiro Kitaizumi, Kota Saichi, Takumi Sato, Ryuji Igarashi
InstitutionsTokyo Institute of Technology, Center for Integrated Quantum Science and Technology
Citations132
AnalysisFull AI Review Included
  • Core Innovation: Development of a novel, compact, optical fiber-based magnetometer utilizing negatively charged nitrogen-vacancy (NV-) centers embedded in bulk diamond.
  • Application Focus: Highly sensitive detection of magnetic nanoparticles (MNPs) for biomedical applications, specifically targeting deep tissue sensing (e.g., sentinel lymph node biopsy).
  • Sensitivity Achievement: The system demonstrated a minimum detectable AC magnetic field sensitivity of 57.6 nT (at 1.025 kHz, with 1 second averaging time).
  • Magnetic Field Control: A specialized coil system was implemented, using an excitation coil to magnetize MNPs with an AC field, and a cancellation coil to suppress the residual excitation field at the NV- center location by approximately 99%.
  • Detection Range: Successfully detected micromolar concentrations of MNPs (ResovistÂź) at longitudinal distances up to 9 mm (for 40 ”L sample volume).
  • Operational Advantage: The NV- center sensor operates effectively at room temperature and ambient magnetic fields (geomagnetic field), offering a practical advantage over cryogenic SQUID or vacuum-dependent OPAM systems.
ParameterValueUnitContext
Diamond TypeBulk (100)N/AUsed for NV- center ensemble.
Diamond Dimensions2 x 2 x 0.5mm3Physical size of the bulk diamond.
NV Fabrication Dose1 x 1018cm-2High-energy electron beam irradiation (4.6 MeV).
NV Annealing Temperature800°CThermal annealing time: 1 hour.
Excitation Laser Wavelength532nmFrequency doubled YAG laser (Green).
Incident Laser Power~100mWApplied to the bulk diamond.
ODMR Center Frequency (f0)~2.87GHzWithout external magnetic field.
ODMR Dip HWHM (w)~4.3MHzHalf Width at Half Maximum.
AC Excitation Frequency1.025kHzFrequency used for MNP magnetization and lock-in detection.
Minimum Detectable AC Field (Experimental)57.6nTAt 1.025 kHz, 1 s averaging time (SNR ~1).
NV Center Sensitivity (Calculated)33.2nTBest sensitivity adjusted for NV- center angle.
Excitation Coil Field (at NV location)~2600”TField generated by excitation coil alone.
Residual Magnetic Field (at NV location)3.5”TAfter cancellation coil application (99% suppressed).
MNP Detectable Distance (40 ”L sample)9mmLongitudinal distance from probe head.
MNP Detectable Distance (5 ”L sample)5mmLongitudinal distance from probe head.
Probe Head Outer Diameter18mmPhysical dimension of the compact probe.

The magnetometer relies on Optically Detected Magnetic Resonance (ODMR) combined with lock-in detection and precise magnetic field control:

  1. NV- Center Fabrication:

    • Bulk (100) diamond was subjected to high-energy electron beam irradiation (4.6 MeV) at a dose of 1 x 1018 cm-2.
    • Subsequent thermal annealing was performed at 800 °C for 1 hour to mobilize vacancies and form the NV- centers.
  2. Optical Fiber System Integration:

    • A compact, bifurcated optical fiber bundle (2x1 coupler) was used for light management.
    • A 532 nm green laser (~100 mW) was delivered through the fiber to excite the NV- centers.
    • Red fluorescence (>600 nm) was collected through the same fiber port and filtered before detection by a photodiode (PD).
  3. Magnetic Resonance Control:

    • Microwave (MW) irradiation (~2.87 GHz) was applied via a thin copper film (0.04 mm thick) located beneath the diamond to drive the electron spin resonance (ESR).
    • A permanent magnet was positioned to apply a static magnetic field, splitting the four NV orientations into eight dips (Zeeman effect) and allowing selection of a single, highly sensitive NV axis for measurement.
  4. AC Field Generation and Cancellation:

    • An excitation coil generated a strong AC magnetic field (1.025 kHz) to actively magnetize the MNPs.
    • A concentric cancellation coil was used to nullify the excitation field at the precise location of the NV- center ensemble, reducing the background field from 2600 ”T down to 3.5 ”T.
  5. Signal Detection:

    • The system utilized lock-in detection (DC sensing principle) tuned to the AC excitation frequency (1.025 kHz).
    • The magnetic field generated by the magnetized MNPs caused fluctuations in the red fluorescence intensity, which were measured by the lock-in amplifier to extract the weak MNP signal.

This technology offers significant potential in fields requiring highly sensitive, non-cryogenic magnetic sensing:

  • Biomedical Diagnostics and Imaging:

    • Sentinel Lymph Node Biopsy (SLNB): Provides a non-radioactive, highly sensitive alternative to conventional gamma probes for detecting MNP tracers accumulating in lymph nodes.
    • Deep Tissue Sensing: Potential for detecting small amounts of MNPs (micromolar concentrations) at depths greater than 10 mm, crucial for non-invasive cancer diagnosis and tracking.
    • In Vivo MNP Tracking: Real-time monitoring and quantification of magnetic tracers used in drug delivery or hyperthermia treatments.
  • Quantum Sensing and Metrology:

    • Room-Temperature Magnetometry: Enables the deployment of highly sensitive magnetometers outside of laboratory environments, eliminating the need for liquid nitrogen or helium required by SQUID or OPAM systems.
    • Compact Sensor Development: The optical fiber-based design facilitates the creation of compact, handheld, or integrated magnetic probes for industrial or field applications.
  • Material Science and Research:

    • Nanoscale Magnetic Characterization: Used for magnetic field imaging and characterization of magnetic materials and phenomena at the millimeter scale and potentially smaller.