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Strongly Interacting, Two-Dimensional, Dipolar Spin Ensembles in (111)-Oriented Diamond

MetadataDetails
Publication Date2025-04-30
JournalPhysical Review X
AuthorsLillian Hughes, Simon A. Meynell, Weijie Wu, Shreyas Parthasarathy, Lingjie Chen
InstitutionsUniversity of California, Santa Barbara, New York University
Citations2
AnalysisFull AI Review Included

Technical Documentation & Analysis: 2D Dipolar Spin Ensembles in (111) Diamond

Section titled “Technical Documentation & Analysis: 2D Dipolar Spin Ensembles in (111) Diamond”

This document analyzes the research paper “Strongly Interacting, Two-Dimensional, Dipolar Spin Ensembles in (111)-Oriented Diamond” to provide technical specifications and highlight how 6CCVD’s specialized MPCVD diamond materials and services can support and advance this critical quantum technology research.


The research successfully demonstrates the creation of highly dense, preferentially aligned, two-dimensional (2D) Nitrogen-Vacancy (NV) ensembles in (111)-oriented diamond, opening new avenues for entanglement-enhanced quantum sensing and simulation.

  • (111) Advantage: Diamond growth on the (111) plane yields significantly higher nitrogen incorporation (up to 60 times greater) compared to conventional (001) substrates.
  • 2D Confinement: Delta doping during PECVD growth successfully confines the NV centers to ultra-thin layers (FWHM 3.2 nm to 5.8 nm), establishing the necessary 2D dimensionality.
  • Maximized Dipolar Interactions: The (111) orientation affords uniformly positive dipolar interactions that do not average to zero, a crucial requirement for leveraging dipolar-driven entanglement schemes.
  • High Sensitivity: The resulting 2D NV ensembles achieve a high volume-normalized AC magnetic sensitivity of 810 pT ”m3/2 Hz-1/2, with projections for improvement down to 153 pT ”m3/2 Hz-1/2.
  • Material Control: Substrate miscut angle is identified as a key tuning knob for controlling the grown-in NV center density, demonstrating precise material engineering control.
  • Novel Characterization: A new XY8-ODMR protocol was developed to suppress disorder and directly characterize the asymmetric line shape indicative of strong, non-zero dipolar coupling.

ParameterValueUnitContext
Crystal Orientation(111)N/ARequired for preferential NV alignment and non-zero dipolar averaging
Nitrogen Incorporation Enhancement~60FactorRelative increase compared to (001) growth
Delta-Doped Layer Thickness (FWHM)3.2 - 5.8nmConfined 2D spin system (SIMS resolution limited)
Volume-Normalized AC Sensitivity (Achieved)810pT ”m3/2 Hz-1/2Measured on electron-irradiated Sample B
Volume-Normalized AC Sensitivity (Projected)153pT ”m3/2 Hz-1/2Projected with optimized photon collection efficiency
PECVD Power750WGentle growth condition
Growth Temperature~770°CMeasured by pyrometer
Growth Pressure25torrStandard PECVD condition
Methane Concentration0.05% - 0.1%12CH4Used in H2 plasma
Substrate Miscut Angle Range0.96 - 3.0°Used to tune grown-in NV density
Highest 2D Nitrogen Areal Density1.9 x 104ppm nmSample C (10 min doping time)
Post-Growth Electron Irradiation DoseUp to 6 x 1019e-/cm2Used to enhance NV concentration
Post-Growth Annealing Temperatures400 and 850°CUsed to promote vacancy diffusion and NV formation

The creation and characterization of the 2D NV ensembles relied on highly controlled MPCVD growth and advanced quantum measurement techniques:

  1. Substrate Selection and Preparation:
    • Electronic-grade CVD diamond substrates were sliced along the (111) plane.
    • Substrates were superpolished to achieve a surface roughness of Ra < 500 pm.
    • Miscut angle (0.96° to 3.0°) was precisely measured using X-ray diffractometry rocking curves.
  2. PECVD Epitaxial Growth:
    • Growth performed in a SEKI SDS6300 reactor under gentle conditions: 750 W plasma power, 25 torr pressure, and ~770 °C temperature.
    • Isotopically purified 99.998% 12C methane (0.05%-0.1% 12CH4) was used to minimize background spin noise.
  3. Delta Doping:
    • Thin nitrogen layers were introduced by interrupting growth and flowing 15N2 gas (1.25% of total gas content) for short, variable doping times (0.5 to 10 min).
  4. Post-Growth Processing:
    • NV creation was enhanced via focused electron irradiation (TEM) to generate vacancies.
    • Subsequent high-temperature annealing (400 °C and 850 °C) was performed in a vacuum furnace (4e-8 torr) to promote vacancy diffusion and NV formation.
  5. Characterization and Sensing:
    • Secondary Ion Mass Spectrometry (SIMS) was used for precise depth profiling and areal density quantification of 15N.
    • Optically Detected Magnetic Resonance (ODMR) and Rabi measurements confirmed preferential NV alignment and high contrast.
    • A novel XY8-ODMR protocol was employed to suppress lattice disorder and directly measure the dipolar-limited line shape, confirming the uniformly positive interactions unique to the (111) 2D system.

This research demonstrates the critical role of high-quality, crystallographically controlled diamond substrates and precise doping techniques. 6CCVD is uniquely positioned to supply the materials and engineering support necessary to replicate and scale this work for next-generation quantum devices.

Research Requirement6CCVD Solution & CapabilityTechnical Advantage for Quantum Research
(111) Substrate SupplyOptical Grade SCD (111) Wafers: We supply high-purity Single Crystal Diamond (SCD) substrates in the required (111) orientation.Guarantees the necessary preferential NV alignment and crystal structure required for non-zero dipolar coupling.
Custom Dimensions & MiscutCustom Dimensions up to 125mm: We offer SCD plates/wafers up to 125mm, including precise control over substrate miscut angle (e.g., 0.96° to 3.0°).Allows researchers to scale up experiments and use miscut angle as a reliable tuning knob for NV density, as demonstrated in the paper.
Ultra-Thin Layer ControlPrecision SCD Epitaxy (0.1 ”m - 500 ”m): Our MPCVD process ensures thickness control down to 0.1 ”m, enabling the fabrication of ultra-thin, nanometer-scale delta-doped layers.Critical for maintaining the 2D dimensionality of the spin ensemble, essential for enhanced spatial resolution and specific quantum simulation regimes.
Custom Doping ProfilesCustom Nitrogen Delta Doping: We implement precise doping recipes (N, B) to control the concentration and depth of the NV and P1 centers, optimizing the NV/P1 ratio for long coherence times (T2).Supports the creation of dipolar-limited ensembles necessary for entanglement-enhanced metrology protocols like DROID-60.
Surface QualityUltra-Low Roughness Polishing: SCD wafers are polished to Ra < 1 nm, ensuring atomically flat surfaces for high-quality epitaxy and minimizing inhomogeneous dopant aggregation.Essential for achieving the high-quality, low-defect epilayers required for stable, coherent shallow NV centers.
Integrated Device FabricationIn-House Metalization Services: We offer custom metalization (Au, Pt, Pd, Ti, W, Cu) for fabricating RF antennas, microwave waveguides, or contact pads directly onto the diamond surface.Streamlines the device fabrication workflow, supporting the implementation of complex ODMR and XY8-ODMR setups.

6CCVD’s in-house team of PhD material scientists and engineers specializes in optimizing MPCVD growth parameters for quantum applications. We can assist researchers in selecting the optimal (111) substrate specifications, designing custom delta-doping recipes, and advising on post-growth processing (e.g., irradiation and annealing) to maximize NV density and coherence for similar quantum sensing and simulation projects.

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

View Original Abstract

Systems of spins with strong dipolar interactions and controlled dimensionality enable new explorations in quantum sensing and simulation. In this work, we investigate the creation of strong dipolar interactions in a two-dimensional ensemble of nitrogen-vacancy (NV) centers generated via plasma-enhanced chemical vapor deposition on (111)-oriented diamond substrates. We find that diamond growth on the (111) plane yields high incorporation of spins, both nitrogen and NV centers, where the density of the latter is tunable via the miscut of the diamond substrate. Our process allows us to form dense, preferentially aligned, 2D NV ensembles with volume-normalized ac sensitivity down to <a:math xmlns:a=“http://www.w3.org/1998/Math/MathML” display=“inline”><a:mrow><a:msub><a:mrow><a:mi>η</a:mi></a:mrow><a:mrow><a:mi>ac</a:mi></a:mrow></a:msub><a:mo>=</a:mo><a:mn>810</a:mn><a:mtext> </a:mtext><a:mtext> </a:mtext><a:mi>pT</a:mi><a:mtext> </a:mtext><a:mi mathvariant=“normal”>ÎŒ</a:mi><a:msup><a:mrow><a:mi mathvariant=“normal”>m</a:mi></a:mrow><a:mrow><a:mn>3</a:mn><a:mo>/</a:mo><a:mn>2</a:mn></a:mrow></a:msup><a:mtext> </a:mtext><a:msup><a:mrow><a:mi>Hz</a:mi></a:mrow><a:mrow><a:mo>−</a:mo><a:mn>1</a:mn><a:mo>/</a:mo><a:mn>2</a:mn></a:mrow></a:msup></a:mrow></a:math>. Furthermore, we show that (111) affords maximally positive dipolar interactions among a 2D NV ensemble, which is crucial for leveraging dipolar-driven entanglement schemes and exploring new interacting spin physics.