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Wide-Field Dynamic Magnetic Microscopy Using Double-Double Quantum Driving of a Diamond Defect Ensemble

MetadataDetails
Publication Date2021-05-14
JournalPhysical Review Applied
AuthorsZeeshawn Kazi, Isaac M. Shelby, Hideyuki Watanabe, Kohei M. Itoh, V. Shutthanandan
InstitutionsEnvironmental Molecular Sciences Laboratory, National Institute of Advanced Industrial Science and Technology
Citations25
AnalysisFull AI Review Included

Technical Documentation & Analysis: Wide-Field Dynamic Magnetic Microscopy

Section titled “Technical Documentation & Analysis: Wide-Field Dynamic Magnetic Microscopy”

6CCVD Reference Document: DDQ-MAG-2021-01 Source Paper: Kazi et al., “Wide-field dynamic magnetic microscopy using double-double quantum driving of a diamond defect ensemble” (arXiv:2002.06237v3)


This research demonstrates a significant advancement in wide-field Nitrogen Vacancy (NV) ensemble magnetometry by introducing the Double-Double Quantum (DDQ) driving technique. This method directly addresses the primary limitation of large-area NV sensors: spatial inhomogeneities.

  • Core Innovation: DDQ driving utilizes four-tone radio frequency (RF) pulses to suppress variations in the NV resonance curve shape (contrast $C$ and linewidth $\delta\nu$) across the imaging field of view.
  • Inhomogeneity Mitigation: The technique eliminates non-magnetic perturbations (strain, temperature, electric field) and curve-shape variations, enabling robust, absolute magnetic field projection mapping without prior per-pixel calibration.
  • High-Speed Dynamic Imaging: DDQ facilitates high-frame-rate magnetic microscopy, achieving 15.6 Hz (64 ms exposure time) imaging of dynamic fields, suitable for single-molecule biophysics applications.
  • Performance Gain: The DDQ modality provides similar magnetic sensitivity to traditional static frequency scanning methods but achieves a greater than four-fold reduction in acquisition time.
  • Material Requirements: Success relies critically on a high-quality, near-surface 15N-doped NV ensemble layer (150 nm thick) grown on an ultra-pure, electronic-grade 12C diamond substrate (99.999% purity) to maximize spin coherence time (T2 = 2.5 ”s).

The following hard data points were extracted from the experimental methods and results sections, highlighting the material and performance metrics achieved.

ParameterValueUnitContext
Diamond Layer Thickness150nm15N doped, 12C purified layer
12C Isotope Purity99.999%Required for long T2 coherence time
NV Ensemble Density1.7 x 1016cm-3High density required for ensemble sensing
Ensemble Spin Coherence Time (T2)2.5”sAchieved T2 time
He+ Implantation Energy25keVUsed for vacancy creation
He+ Implantation Dose5 x 1011ions/cm2Used for vacancy creation
NV Formation Anneal Temperature900°CVacuum anneal duration: 2 h
Charge State Stabilization Temp425°CO2 anneal duration: 2 h
External Static Magnetic Field (Bext)1mTApplied along the <111> NV orientation
Average Volume Normalized Sensitivity31nT Hz-1/2 ”m3/2Achieved sensitivity in the magPI platform
Dynamic Imaging Frame Rate15.6HzCorresponds to 64 ms exposure time per frame
RF Tone Separation (Hyperfine)3.05MHzUsed for simultaneous driving of 15N-NV transitions

The experiment relied on precise material engineering and advanced quantum control sequences to achieve high-fidelity wide-field imaging.

  1. Material Growth: A 150 nm thick layer of 15N doped, isotope-purified (99.999% 12C) diamond was grown via Chemical Vapor Deposition (CVD) on an electronic-grade diamond substrate.
  2. Vacancy Creation: The sample was implanted with 25 keV He+ ions at a dose of 5 x 1011 ions/cm2 to introduce vacancies near the surface.
  3. Annealing Protocol: Sequential annealing was performed: 900 °C in vacuum (2 h) for NV formation, followed by 425 °C in O2 (2 h) for charge state stabilization.
  4. Optical Pumping: A 532 nm laser pulse was used to initialize the NV ensemble into the |ms = 0> ground state.
  5. RF Excitation (DDQ): Four-tone RF π-pulses were applied simultaneously via a broadband microwave antenna. The tones were positioned at the outer (f1, f4) and inner (f2, f3) inflection points of the two Zeeman-split resonance curves.
  6. Readout: The photoluminescence (PL) intensity reduction was monitored using a sCMOS camera during pulsed excitation sequences (4 ms total duration).
  7. Data Processing: The DDQ difference image (DDQ DI) was constructed using only two images, $I_{on}(f_{1}, f_{4})$ and $I_{on}(f_{2}, f_{3})$, enabling high-frame-rate mapping of the magnetic field projection $\mathbf{B} - \langle\mathbf{B}\rangle$.

The successful implementation of DDQ dynamic magnetometry requires diamond substrates with exceptional purity, precise doping profiles, and high surface quality—all core competencies of 6CCVD’s MPCVD manufacturing.

To replicate or extend this research, 6CCVD recommends the following materials:

Application Requirement6CCVD Material RecommendationTechnical Rationale
High Coherence Time (T2)Isotopically Pure Single Crystal Diamond (SCD)Guaranteed 12C purity (>99.999%) minimizes spin bath noise, essential for achieving the T2 = 2.5 ”s required for high-fidelity quantum control sequences like DDQ.
Near-Surface High-Density NV LayerCustom 15N Doped SCDWe offer precise control over nitrogen doping during CVD growth, allowing for the creation of high-density 15N ensembles (1.7 x 1016 cm-3) necessary for ensemble sensing sensitivity.
Wide-Field Imaging PlatformLarge Format Polycrystalline Diamond (PCD)For scaling the wide-field platform beyond typical SCD sizes, 6CCVD offers PCD plates up to 125 mm diameter, suitable for large-area sensor integration.

6CCVD’s in-house engineering capabilities directly address the specific fabrication and integration challenges presented in this work:

  • Custom Dimensions and Thickness: The paper utilized a 150 nm sensing layer. 6CCVD provides custom SCD thicknesses from 0.1 ”m up to 500 ”m, allowing researchers to optimize the NV depth for specific magnetic field gradients (e.g., nanoscale vs. bulk fields). We also supply substrates up to 10 mm thick.
  • Precision Polishing: Achieving reliable bio-integration (DNA tethering) and minimizing optical scattering requires an ultra-smooth surface. 6CCVD guarantees Ra < 1 nm polishing for SCD, ensuring optimal surface quality for sensitive microscopy.
  • RF Integration and Metalization: The DDQ technique relies on efficient delivery of four-tone RF pulses via a microwave antenna. 6CCVD offers internal metalization services (Au, Pt, Pd, Ti, W, Cu) to fabricate custom antenna structures directly onto the diamond surface, facilitating robust quantum control.
  • Post-Processing Advisement: While the paper used He+ implantation, 6CCVD’s PhD team can advise on optimizing CVD growth parameters or post-processing recipes (implantation dose and annealing protocols) to achieve the target NV density and charge state stability (900 °C and 425 °C anneals).

6CCVD’s in-house PhD team specializes in defect engineering and material optimization for quantum sensing. We can assist with material selection for similar dynamic magnetic microscopy projects, ensuring the substrate properties (purity, strain, doping) are perfectly matched to the demanding requirements of high-speed, inhomogeneity-mitigated quantum control sequences like DDQ.

For custom specifications or material consultation, visit 6ccvd.com or contact our engineering team directly.

View Original Abstract

Wide-field magnetometry can be realized by imaging the optically-detected magnetic resonance of diamond nitrogen vacancy (NV) center ensembles. However, NV ensemble inhomogeneities significantly limit the magnetic-field sensitivity of these measurements. We demonstrate a double-double quantum (DDQ) driving technique to facilitate wide-field magnetic imaging of dynamic magnetic fields at a micron scale. DDQ imaging employs four-tone radio frequency pulses to suppress inhomogeneity-induced variations of the NV resonant response. As a proof-of-principle, we use the DDQ technique to image the dc magnetic field produced by individual magnetic-nanoparticles tethered by single DNA molecules to a diamond sensor surface. This demonstrates the efficacy of the diamond NV ensemble system in high-frame-rate magnetic microscopy, as well as single-molecule biophysics applications.