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Minireview on Nuclear Spin Polarization in Optically-Pumped Diamond Nitrogen Vacancy Centers

MetadataDetails
Publication Date2016-12-20
JournalJournal of the Korean Magnetic Resonance Society
AuthorsKeunhong Jeong
Citations2
AnalysisFull AI Review Included

Advanced Technical Analysis: NV Center Spin Polarization in CVD Diamond

Section titled “Advanced Technical Analysis: NV Center Spin Polarization in CVD Diamond”

This minireview establishes the critical role of the Nitrogen Vacancy (NV) center in MPCVD diamond as an efficient platform for Dynamic Nuclear Polarization (DNP), enabling ultra-sensitive Nuclear Magnetic Resonance (NMR) and potential Magnetic Resonance Imaging (MRI) applications.

  • Core Achievement: Demonstrated efficient hyperpolarization of nuclear spins (primarily 13C, 14N, and 15N) utilizing the long electron spin coherence time (T1) of the NV center in diamond.
  • Performance Metrics: Achieved polarization levels approaching 100% for 13C and 15N nuclei in selected magnetic field regimes and cryogenic temperatures.
  • Key Methodology: Polarization is driven by continuous optical pumping (532 nm laser) coupled with precise Microwave (MW) and Radiofrequency (RF) irradiation, monitored via Optically Detected Magnetic Resonance (ODMR).
  • Critical Mechanisms: Polarization transfer utilizes internal quantum transitions, specifically through Level Anticrossing phenomena (Excited State, ESLAC, at ~500 G, and Ground State, GSLAC, at ~1000 G).
  • Material Requirements: Success hinges on using high-purity Single Crystal Diamond (SCD) with controlled defect concentrations (low P1 center concentration) and often requires isotopic enrichment (e.g., 1.1% or 100% 13C enrichment) to maximize target spin density.
  • Future Potential: The research paves the way for transferring diamond-polarized nuclear spins to external biological or inorganic materials, revolutionizing low-field NMR sensitivity.

The following parameters and performance metrics were extracted from the summarized research studies concerning NV center manipulation and polarization transfer.

ParameterValueUnitContext
NV Ground State ZFS (Dgs)2.87GHzZero Field Splitting, B ≈ 0 G
NV Excited State ZFS (Des)1.42GHzZero Field Splitting
ODMR Center Frequency2.87GHzUsed for reading electron spin state
Optical Pumping Wavelength532nmCommon green excitation source (2.32 eV)
Fluorescence Emission Wavelength637nmReadout signal
ESLAC Magnetic Field~500GExcited State Level Anticrossing
GSLAC Magnetic Field~1000GGround State Level Anticrossing
High Magnetic Field Experiment8.7TUsed for direct laser irradiation DNP
Maximum 15N Polarization98%Achieved in ESLAC, Low Temperature
Maximum 13C Polarization~100%Achieved in GSLAC, ODMR detection
Temperature Range5 to RT (Room)KExperiments performed across cryogenic and ambient conditions
Surface Transfer Distance Limit< 2nmRequired distance for effective hyperfine interaction transfer

The polarization transfer experiments rely on precise control over defect creation, external fields, and optical/microwave stimulation.

  1. Diamond Synthesis: Production of high-quality Single Crystal Diamond (SCD) either by High Pressure High Temperature (HPHT) or, preferably for purity and control, by Chemical Vapor Deposition (CVD).
  2. Defect Creation (NV Center): Introduction of Nitrogen atoms during CVD growth or post-growth implantation, followed by electron/neutron irradiation and subsequent high-temperature annealing (typically > 800 °C) to create stable NV centers (a substitutional nitrogen atom adjacent to a carbon vacancy).
  3. Isotopic Enrichment: Utilization of precursors enriched with 13C or 15N during CVD growth to enhance the density of target nuclear spins.
  4. Optical Polarization: Continuous Wave (CW) laser irradiation (532 nm) pumps the NV electron spin population into the Sz=0 ground state, creating electron spin polarization.
  5. Magnetic Field Alignment: Applying a specific external magnetic field (B) to induce Level Anticrossing (ESLAC at ~500 G or GSLAC at ~1000 G) conditions, where the electron spin state mixes with the nuclear spin state.
  6. MW/RF Stimulation: Microwave irradiation (around 2.87 GHz) is used to address specific electronic transitions (Sz=0 to Sz=±1), enabling electron spin state manipulation and polarization transfer into the adjacent nuclei via hyperfine interactions.
  7. Detection: Polarization state is measured using Optically Detected Magnetic Resonance (ODMR), observing changes in 637 nm fluorescence intensity relative to applied MW frequency.

6CCVD is uniquely positioned to supply the advanced diamond materials required to replicate and extend the state-of-the-art research reviewed in this paper, particularly in DNP and quantum sensing fields.

To replicate the high efficiency polarization results (up to 100% 13C polarization) and long coherence times (T1) necessary for DNP, researchers require ultra-pure, low-strain SCD with controlled defect engineering.

Material Requirement6CCVD Material SolutionContext & Advantage
High Purity SubstratesOptical Grade Single Crystal Diamond (SCD)Essential for minimizing detrimental P1 centers and achieving long T1 times necessary for efficient spin diffusion and polarization transfer. 6CCVD guarantees high structural quality.
Isotopic EnrichmentCustom 13C or 15N Doped SCDRequired for maximizing the density of polarized nuclei and studying specific nuclear species. 6CCVD offers custom CVD growth using enriched gas precursors (e.g., 13C or 15N).
Bulk DNP StudiesSCD Substrates up to 10 mm ThicknessIdeal for high magnetic field experiments (e.g., 8.7 T) and bulk diamond polarization studies cited in the research (Refs 21, 25, 29).
Surface Transfer/Nanodiamond PrecursorsThin Film SCD/PCD (0.1 ”m - 500 ”m)Thin films are crucial for subsequent processing into nanodiamonds or for investigating surface-enhanced polarization transfer to external materials.
External DNP IntegrationBoron-Doped Diamond (BDD)While not the primary focus, BDD films are available for integrated sensor environments requiring conductive diamond electrodes.

The precision required in NV research necessitates highly specific material preparation that 6CCVD can deliver directly.

  • Defect Engineering Control: 6CCVD’s MPCVD process allows for precise, controlled nitrogen doping during growth, optimizing NV center concentration ratios. This control is vital for balancing bulk polarization efficiency with spin diffusion length.
  • Custom Dimensions and Shaping: We provide custom plates and wafers up to 125 mm (PCD) and precise laser cutting and dicing services to match specific experimental geometries (e.g., creating samples optimized for shuttling systems).
  • Surface Preparation: Achieving high-fidelity ODMR and effective optical pumping requires pristine surfaces. 6CCVD offers Atomic Force Microscopy (AFM) polished SCD with surface roughness Ra < 1 nm, minimizing optical scattering losses and maximizing photon collection efficiency (637 nm).
  • Integrated Device Development: For microwave delivery and field control systems, 6CCVD offers custom metalization (Au, Pt, Pd, Ti, W, Cu) applied directly to the diamond surface for creating on-chip electrodes and antenna structures necessary for highly localized MW/RF addressing.

6CCVD’s commitment extends beyond material supply to comprehensive technical partnership.

  • Expert Consultation: 6CCVD’s in-house PhD engineering team possesses extensive expertise in solid-state defect physics and MPCVD growth. We can assist researchers in selecting the optimal diamond substrate specifications (e.g., doping levels, isotopic purity, thickness) for specific Dynamic Nuclear Polarization (DNP) and quantum magnetometry projects.
  • Global Logistics: We ensure reliable delivery of sensitive materials worldwide, with DDU (Delivered Duty Unpaid) default shipping, and DDP (Delivered Duty Paid) options available upon request.

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

View Original Abstract

Nitrogen vacancy-centered diamond has recently emerged as a promising material for various applications due to its special optical and magnetic properties. In particular, its applications as a fluorescent biomarker with small toxicity, magnetic field and electric field sensors have been a topic of great interest. Recent review (R. Schirhagl et al 2014) introduced those applications using single NV-center in nanodiamond. In this minireview, I introduce the rapidly emerging DNP (Dynamic Nuclear Polarization) field using optically-pumped NV center in diamonds. Additionally, the possibility of exploiting the optically-pumped NV center for polarization transfer source, which will produce a profound impact on room temperature DNP, will be discussed.