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Achieving 5% 13C nuclear spin hyperpolarization in high-purity diamond at room temperature and low magnetic field

MetadataDetails
Publication Date2025-03-29
JournalScientific Reports
AuthorsVladimir Vladimirovich Kavtanyuk, Changjae Lee, Keunhong Jeong, Jeong Hyun Shim
InstitutionsKorea University of Science and Technology, Korea Research Institute of Standards and Science
Citations1
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Technical Documentation & Analysis: High-Purity Diamond for Nuclear Spin Hyperpolarization

Section titled “Technical Documentation & Analysis: High-Purity Diamond for Nuclear Spin Hyperpolarization”

This research demonstrates a significant advancement in diamond-based quantum technology, achieving high levels of 13C nuclear spin hyperpolarization under practical conditions (Room Temperature and low magnetic field). The core value proposition relies entirely on the quality and purity of the Single Crystal Diamond (SCD) material.

  • Record Polarization: Achieved 5% 13C nuclear spin hyperpolarization, equivalent to an enhancement ratio exceeding 7 x 106 over thermal polarization.
  • Practical Conditions: Polarization achieved at Room Temperature (RT) and a low magnetic field of 9.4 mT, making the technique highly accessible for device integration.
  • Material Purity Criticality: The high polarization and exceptional storage time (Tdepol > 100 min) were enabled by using ultra-high purity CVD-grown SCD with initial Nitrogen (N) concentration below 1 ppm.
  • Orientation Optimization: Aligning the magnetic field along the [100] crystal orientation quadrupled the number of Nitrogen-Vacancy (NV) centers involved in the polarization transfer process.
  • Mechanism: The polarization transfer is predominantly attributed to the Integrated Solid Effect (ISE) followed by nuclear spin diffusion, highly efficient in low-N concentration diamonds.
  • Applications: This breakthrough is ideal for developing next-generation solid-state devices, including high-precision NMR gyroscopes, high-field magnetometers, and background-free MRI signal agents (RASER technology).

The following table summarizes the critical performance metrics and material parameters extracted from the research.

ParameterValueUnitContext
Maximum 13C Polarization5%Achieved at 9.4 mT
Polarization Enhancement Ratio> 7 x 106N/ARelative to thermal polarization
Optimal Low Magnetic Field (B)9.4mTUsed for hyperpolarization
NMR Readout Magnetic Field (B)6TUsed for signal quantification
Operating TemperatureRoom TemperatureN/AEnables practical device use
Initial N Concentration (Requirement)< 1ppmCritical for long Tdepol
Substitutional N (Ns) Concentration (Sample)≈ 0.2ppmEstimated concentration
NV Center Concentration (Sample)≈ 0.3ppmEstimated concentration
Polarization Build-up Time (Tpol)10.4minTime to reach saturation at 9.4 mT
Depolarization Storage Time (Tdepol)102minMeasured at 6 T (Laser off)
Diamond Crystal Orientation[100]N/AOptimized for NV alignment
Laser Wavelength532nmContinuous optical pumping
Optimal MW Sweep Width6MHzMinimal sweep width covering ODMR spectrum
Optimal MW Sweep Rate (Δ̇)1.5MHz/msAchieved maximum polarization

The high 13C polarization was achieved through systematic optimization of material selection and experimental parameters, focusing on the Integrated Solid Effect (ISE) mechanism.

  1. Material Selection: Utilized a CVD-grown Single Crystal Diamond (SCD) with ultra-low nitrogen concentration (N < 1 ppm) and a [100] surface orientation.
  2. Low-Field Polarization Setup: The diamond sample was placed in a low magnetic field regime (optimized to 9.4 mT).
  3. Optical Pumping: Continuous laser irradiation (532 nm) was applied to optically polarize the NV electron spins.
  4. Microwave (MW) Irradiation: A repetitive, frequency-swept MW chirp was applied (e.g., 2.740-2.746 GHz sweep width) to transfer polarization from NV centers to 13C nuclei.
  5. Parameter Optimization: A comprehensive search was performed to determine the optimal relationships between:
    • Magnetic Field (B) and MW Power (PMW).
    • MW Sweep Width (Δ) and Sweep Rate (Δ̇).
  6. Rapid Shuttling: A swift shuttling mechanism transferred the hyperpolarized diamond sample (< 1.5 s) from the low-field polarization region to a high-field (6 T) superconducting magnet.
  7. NMR Readout: The 13C NMR signal was recorded at 6 T to quantify the achieved polarization level, normalized against a thermal polarization reference.

6CCVD is uniquely positioned to supply the high-specification diamond materials required to replicate, scale, and advance this hyperpolarization research for commercial applications in quantum sensing and medical imaging.

Research Requirement6CCVD Solution & CapabilityTechnical Advantage & Sales Driver
Ultra-High Purity SCD (N < 1 ppm)Optical Grade Single Crystal Diamond (SCD): Our MPCVD process ensures extremely low substitutional nitrogen (Ns) concentration, critical for minimizing decoherence.Extended Tdepol and T2: Directly enables the long spin storage times (> 100 min) necessary for practical hyperpolarization storage and transfer, surpassing limitations of lower-grade materials.
Custom Crystal Orientation ([100])Precision Orientation Control: We offer SCD plates and wafers with custom crystallographic orientations, including [100], [110], and [111].Maximized NV Yield: Guarantees optimal alignment for the magnetic field, maximizing the number of NV centers contributing to the Integrated Solid Effect (ISE) polarization transfer.
Custom Dimensions & Mass (15 mg chip)Custom Dimensions & Dicing: We supply SCD wafers (0.1 ”m to 500 ”m thickness) and offer precision laser cutting for custom chips and plates.Experimental Flexibility: Provides researchers with samples perfectly tailored for specific MW cavities, NMR probes, or integration into microfluidic systems.
Integration for MW DeliveryIn-House Metalization Services: We offer deposition of Au, Pt, Pd, Ti, W, and Cu films.On-Chip Device Fabrication: Allows for the direct patterning of high-quality microwave transmission lines or antennas onto the diamond surface, enabling highly efficient PMW delivery and optimization of sweep parameters.
Scaling for RASER/GyroscopesLarge-Area PCD/SCD Substrates: We provide PCD wafers up to 125 mm diameter and thick SCD substrates (up to 10 mm).Commercial Viability: Supports the transition from small-scale lab experiments to scalable, high-volume manufacturing of diamond-based quantum sensors and NMR devices.

6CCVD’s in-house team of PhD material scientists and engineers provides expert consultation on material selection, defect engineering (e.g., controlled NV creation), and surface preparation (Ra < 1 nm polishing for SCD) for advanced hyperpolarization and quantum sensing projects.

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

View Original Abstract

Optically polarizable nitrogen-vacancy (NV) centers in diamond enable hyperpolarization of <sup>13</sup>C nuclear spins at a low magnetic field and room temperature. However, it remains a challenge to achieve a high level of polarization, comparable to that of conventional dynamic nuclear polarization. In this paper, we demonstrate that a <sup>13</sup>C polarization of 5%, equivalent to an enhancement ratio of over [Formula: see text], can be attained at less than 10 mT. We used a high-purity diamond with an initial nitrogen concentration below 1 ppm, which resulted in a storage time exceeding 100 min. Aligning the magnetic field along [100] increased the number of NV spins involved in polarization transfer by a factor of four. For this orientation, a comprehensive optimization of the magnetic field intensity and microwave (MW) sweep parameters has been performed. The optimum MW sweep width suggests that polarization transfer occurs primarily to the bulk <sup>13</sup>C spins through the integrated solid effect, followed by nuclear spin diffusion.

  1. 1970 - Spin Temperature and Nuclear Magnetic Resonance in Solids