Skip to content

Resonance-inclined optical nuclear spin polarization of liquids in diamond structures

MetadataDetails
Publication Date2016-02-24
JournalPhysical review. B./Physical review. B
AuthorsQ. Chen, Ilai Schwarz, Fedor Jelezko, Alex Retzker, Martin B. Plenio
InstitutionsUniversitÀt Ulm, Hebrew University of Jerusalem
Citations22
AnalysisFull AI Review Included

Technical Analysis and Documentation: Resonance-Inclined Optical Nuclear Spin Polarization in Diamond

Section titled “Technical Analysis and Documentation: Resonance-Inclined Optical Nuclear Spin Polarization in Diamond”

This document analyzes the research paper detailing the SPRINT (Spin polarisation via resonance-inclined transfer) mechanism for achieving high dynamic nuclear polarization (DNP) in liquids using optically polarized Nitrogen-Vacancy (NV) centers embedded in nanodiamonds. This technology significantly boosts NMR/MRI sensitivity.

  • Core Achievement: Demonstrated 4700-fold nuclear spin polarization enhancement of flowing water molecules compared to thermal equilibrium.
  • Novel Mechanism: SPRINT is introduced, allowing efficient resonance-based DNP even in liquid solutions characterized by large interaction correlation times (τc ≈ 100 ns).
  • Material Platform: NV centers in nanodiamonds (NDs) were immobilized in a hydrogel flow cell, providing the necessary high electron spin polarization via 532 nm optical pumping.
  • Scalable Output: Achieved 0.6% polarization in 1 ”l liquid volumes within 1 second, a signal amplitude detectable by commercial NMR scanners.
  • Tolerance and Robustness: The mechanism proves robust, maintaining high polarization over a wide range of detuning from the resonance frequency, a critical advantage over conventional solid-state DNP methods.
  • Future Applications: The methodology is transferable to biomedically relevant molecules like 13C pyruvic acid or 13C glucose, dramatically enhancing metabolic MR imaging capabilities.

The following hard data points were extracted from the theoretical model and projected experimental parameters:

ParameterValueUnitContext
Polarization Enhancement Factor4700foldRelative to thermal polarization at 0.35 T
Steady-State Nuclear Polarization (Plim)0.6%Achieved in flowing solvent (water)
Applied DC Magnetic Field (B)0.35TUniform field defining the z-axis
Optimized Polarized Volume1”lAchieved polarization in 1 second
Nanodiamond Radius (b)5nmAssumed radius for maximal efficiency
Hydrogel Diffusion Decrease Ratio (k)100unitlessDW/DT, critical for achieving high τc
Interaction Correlation Time (τc)100nsAchieved by hydrogel immobilization (k=100)
Average Polarization Rate (Weff)1.4ms-1Rate calculated for b=5 nm, k=100
Optical Pumping Wavelength532nmGreen laser illumination source
Target H-H Resonance Frequency ($\omega_{E}$)(2π)16MHzMatching condition $\omega_{E} = \omega_{S}$

The theoretical framework proposes a robust system utilizing high-quality diamond material engineering and specialized quantum spin control.

  1. Material Selection & Immobilization: Nitrogen-Vacancy (NV) centers embedded in nanodiamonds (b=5 nm) are utilized as hyperpolarization agents. These NDs are immobilized within a specialized hydrogel flow cell to control molecular kinetics.
  2. Diffusion Rate Control: The hydrogel layer is engineered to reduce the translational diffusion coefficient (DT) of the solvent molecules by a factor of k=100 (relative to free water, DW), achieving the necessary large interaction correlation time ($\tau_{c} = b^{2} / D_{T} \approx 100$ ns).
  3. Optical Pumping: Continuous-wave (CW) 532 nm green laser illumination is applied to the setup. The unique optical properties of the NV centers allow for rapid, high-purity electron spin polarization (PC ≈ 0.25).
  4. Microwave (MW) Control: Continuous MW radiation is applied, tuned to match the Hartmann-Hahn (H-H) resonant condition ($\omega_{E} = \omega_{S}$). This drives the electron spin to approach resonance with the nuclear spins of the flowing liquid.
  5. Resonance-Inclined Transfer (SPRINT): The combination of large correlation time and H-H resonance enables net polarization transfer from the electron spins to the solvent nuclear spins (protons). The key novelty is the robustness to large detuning ($\Delta^{\prime} \sim (2\pi)10$ MHz).
  6. Continuous Flow Detection: The hyperpolarized liquid (Plim ≈ 0.6%) flows downstream through the cell (v = 10-3 m/s, Tp ≈ 1s) for detection by commercial NMR systems.

This research highlights the indispensable role of high-purity, engineered diamond materials for realizing scalable quantum sensing and hyperpolarization technologies. 6CCVD stands ready as the expert partner to transition these laboratory achievements into robust, mass-producible devices.

The foundation of high-performance NV center systems relies on ultra-pure, low-strain, and precisely manufactured diamond substrates.

  • Optical Grade Single Crystal Diamond (SCD): This research depends on the efficiency of 532 nm optical pumping. 6CCVD offers optical grade SCD, ideal for applications requiring superior transparency and extremely low strain, ensuring maximum optical penetration depth and efficient NV center formation/control.
    • Relevance: While the paper uses nanodiamonds, high-quality SCD is the foundation for creating large quantities of uniform, high-density NV nanodiamonds or for use in bulk diamond devices (e.g., integrated microfluidic channels or waveguides) necessary for commercial scaling.
  • Polycrystalline Diamond (PCD): For flow cells, microfluidic chips, or platforms requiring large-area coverage up to 125 mm, our PCD substrates offer high thermal management and structural integrity necessary for handling continuous optical (532 nm) and microwave excitation.
  • Boron-Doped Diamond (BDD): The paper stresses the importance of polarizing 13C molecules (e.g., pyruvate). 6CCVD can supply specialized BDD films that are crucial for electrochemical systems often used to enhance the lifetime or transfer efficiency of hyperpolarized agents post-DNP.

To optimize the $\tau_{c}$ and the $\text{N}{e}/\text{N}{p}$ ratio crucial for DNP efficiency, precise control over geometry and integration is required. 6CCVD specializes in providing materials engineered to demanding specifications:

Requirement in Paper6CCVD CapabilityBenefits for DNP/NMR
Microfluidic IntegrationPlates/wafers up to 125 mmEnables large-scale device fabrication and high throughput flow cells.
Precise Layer ThicknessSCD films from 0.1 ”m up to 500 ”mTailored diamond thickness for optimized microwave coupling and minimal optical absorption/scattering.
Low Surface RoughnessPolishing Ra < 1 nm (SCD)Essential for minimizing surface defects, which can affect NV stability and reduce proton relaxation time (T1).
Custom InterfacesMetalization (Au, Pt, Pd, Ti, W, Cu)Enables integration of high-frequency microwave transmission lines (CPW structures) directly onto the diamond substrate surface for highly localized MW delivery.
Structural ComplexityLaser cutting and micromachiningAllows for custom geometries, apertures, or complex channel definition required for flow cells and hydrogel immobilization platforms.

The realization of robust SPRINT-based DNP systems requires bridging material science (diamond quality, NV creation) and quantum physics (spin control, resonance tuning).

6CCVD’s in-house PhD team provides specialized material consultation to assist researchers and engineers in selecting or designing the optimal diamond platform for similar hyperpolarization, quantum sensing, or metabolic MR imaging projects. We ensure that substrate properties—such as lattice purity, nitrogen content (for NV concentration control), and surface termination—are precisely matched to the specific demands of your experiment.

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

View Original Abstract

Dynamic nuclear polarization (DNP) of molecules in a solution at room\ntemperature has potential to revolutionize nuclear magnetic resonance\nspectroscopy and imaging. The prevalent methods for achieving DNP in solutions\nare typically most effective in the regime of small interaction correlation\ntimes between the electron and nuclear spins, limiting the size of accessible\nmolecules. To solve this limitation, we design a mechanism for DNP in the\nliquid phase that is applicable for large interaction correlation times.\nImportantly, while this mechanism makes use of a resonance condition similar to\nsolid-state DNP, the polarization transfer is robust to a relatively large\ndetuning from the resonance due to molecular motion. We combine this scheme\nwith optically polarized nitrogen vacancy (NV) center spins in nanodiamonds to\ndesign a setup that employs optical pumping and is therefore not limited by\nroom temperature electron thermal polarisation. We illustrate numerically the\neffectiveness of the model in a flow cell containing nanodiamonds immobilized\nin a hydrogel, polarising flowing water molecules 4700-fold above thermal\npolarisation in a magnetic field of 0.35 T, in volumes detectable by current\nNMR scanners.\n

  1. 1961 - The Principles of Nuclear Magnetism