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High-resolution nanoscale NMR for arbitrary magnetic fields

MetadataDetails
Publication Date2023-10-17
JournalCommunications Physics
AuthorsJonas Meinel, Minsik Kwon, R. Maier, Durga Bhaktavatsala Rao Dasari, Hitoshi Sumiya
InstitutionsUniversity of Stuttgart, Sumitomo Electric Industries (Japan)
Citations9
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Technical Documentation & Analysis: High-Resolution Nanoscale NMR using NV Centers

Section titled “Technical Documentation & Analysis: High-Resolution Nanoscale NMR using NV Centers”

This document analyzes the requirements and findings of the research paper “High-resolution nanoscale NMR for arbitrary magnetic fields” and aligns them with the advanced capabilities of 6CCVD’s MPCVD diamond products, specifically targeting engineers and scientists working in quantum sensing and high-resolution spectroscopy.


The research introduces a novel Electron-Nuclear Double Resonance (ENDOR) quantum heterodyne (qdyne) protocol, significantly advancing nanoscale Nuclear Magnetic Resonance (NMR) spectroscopy using Nitrogen Vacancy (NV) centers in diamond.

  • High-Field Applicability: The new ENDOR qdyne method eliminates the need for pulse-intensive dynamical decoupling (DD) sequences, enabling high-resolution NMR sensing at high magnetic fields where chemical shift resolution is maximized.
  • Material Requirement: Success hinges on ultra-high purity, isotopically enriched Single Crystal Diamond (SCD) (99.995% $^{12}$C) to ensure long NV electron spin coherence times ($T_2 \approx 300 \text{ ”s}$).
  • Spectral Resolution Improvement: The protocol demonstrated a decay rate ($\Gamma$) of $0.6 \pm 0.1 \text{ kHz}$ on a weakly coupled $^{13}\text{C}$ spin, significantly better than the conventional qdyne baseline ($1.4 \pm 0.3 \text{ kHz}$).
  • Decoherence Mechanism Identified: The primary linewidth-limiting factor was identified as NV-spin-initialization infidelity combined with strong sensor-target coupling, guiding future material and protocol optimization.
  • Methodology: The technique uses phase-coherent Radio Frequency (RF) pulses to map transverse nuclear spin polarization ($I_x, I_y$) to longitudinal polarization ($I_z$), which is then sensed via a Ramsey sequence on the NV electron spin.
  • 6CCVD Value Proposition: 6CCVD specializes in providing the necessary quantum-grade, isotopically enriched SCD wafers, custom dimensions, and integrated metalization services (e.g., for Coplanar Waveguides) required to replicate and scale this high-field quantum sensing platform.

The following hard data points were extracted from the experimental results and material requirements:

ParameterValueUnitContext
Diamond Material TypeSCD (HPHT Grown)N/ASingle Crystal Diamond used as sensor platform.
Isotopic Purity99.995% $^{12}$C EnrichmentMinimum purity required to achieve long $T_2$ times.
Crystal Orientation(111)N/APolished slice orientation.
Sample Dimensions$2 \times 2 \times 0.08$mmSCD slice size (80 ”m thickness).
Magnetic Field ($B_0$)0.25TModerate field demonstration.
Target Spin$^{13}\text{C}$N/AWeakly coupled nuclear spin.
Hyperfine Coupling ($A_{zz}$)6kHzCoupling strength of the target $^{13}\text{C}$ spin.
ENDOR Qdyne Decay Rate ($\Gamma$)$0.6 \pm 0.1$kHzAchieved spectral resolution limit.
Conventional Qdyne Decay Rate ($\Gamma$)$1.4 \pm 0.3$kHzDecay rate using DD-based protocol.
Electron $T_2$ (Typical)$\approx 300$”sNV center coherence time.
Electron $T_2^*$ (Typical)50”sNV center dephasing time.
Electron Irradiation Energy2MeVUsed for NV creation.
Annealing Temperature1000°CPost-irradiation processing temperature.

The experiment combined advanced material engineering with complex quantum control sequences to achieve high-resolution NMR sensing.

  1. Material Synthesis and Preparation:
    • The diamond was grown via the High-Pressure High-Temperature (HPHT) method, ensuring ultra-high purity and 99.995% $^{12}\text{C}$ isotopic enrichment.
    • The crystal was processed into a polished (111)-oriented slice with a thickness of $80 \text{ ”m}$.
  2. NV Center Creation:
    • Intrinsic nitrogen was used as the source.
    • NV centers were created by irradiation with 2 MeV electrons at a fluence of $1.3 \times 10^{11} \text{ cm}^{-2}$.
    • Subsequent annealing was performed at $1000^\circ \text{C}$ for 2 hours in vacuum to mobilize vacancies and form NV centers.
  3. Quantum Control and Sensing (ENDOR Qdyne Protocol):
    • The setup utilized a confocal microscope for optical initialization (520 nm laser) and readout (red fluorescence detection).
    • Microwave (MW) and Radio Frequency (RF) pulses were delivered via a coplanar waveguide (CPW) glued to the diamond, driven by an Arbitrary Waveform Generator (AWG).
    • The protocol employed sequential measurements, where the nuclear spin precession was sampled phase-coherently over multiple cycles, persisting longer than the NV electron $T_1$.
    • A critical step involved using a $3\pi/2$ RF pulse to convert the fast-oscillating transverse nuclear polarization ($I_x, I_y$) into the static longitudinal component ($I_z$), which is then sensed via a Ramsey sequence on the NV electron spin.

6CCVD is uniquely positioned to supply the quantum-grade diamond materials and fabrication services required to replicate and advance this high-resolution nanoscale NMR research, particularly for scaling the protocol to high magnetic fields.

To achieve the long coherence times and high spectral resolution demonstrated, researchers require diamond with exceptional isotopic purity and precise thickness control.

  • Quantum Grade Single Crystal Diamond (SCD):
    • Requirement Match: The paper used 99.995% $^{12}\text{C}$ enriched diamond. 6CCVD offers Isotopically Pure SCD with enrichment levels exceeding 99.999%, providing the lowest possible concentration of lattice defects and maximizing the NV center $T_2$ coherence time, which is critical for achieving sub-kHz spectral resolution.
  • Custom SCD Thickness and Dimensions:
    • Requirement Match: The experiment used an $80 \text{ ”m}$ thick slice. 6CCVD provides Custom Dimensions for SCD wafers ranging from $0.1 \text{ ”m}$ up to $500 \text{ ”m}$ thickness, and plates up to $125 \text{ mm}$ (PCD equivalent). This allows optimization of the NV layer depth ($d_{NV}$) to balance linewidth ($\Gamma$) and signal sensitivity, as discussed in Fig. 5 of the paper.
  • Polishing and Orientation:
    • We supply (111)-oriented SCD wafers with Ultra-Low Roughness Polishing (Ra < $1 \text{ nm}$), ensuring high-fidelity optical access and optimal surface quality for subsequent device fabrication.

The integration of the diamond sensor with the microwave delivery system (CPW) is a key technical challenge. 6CCVD offers integrated solutions to simplify device fabrication.

  • Integrated Metalization Services:
    • The CPW requires precise metal layers. 6CCVD offers Internal Metalization Capability including Au, Pt, Pd, Ti, W, and Cu. We can deposit multi-layer stacks directly onto the polished SCD surface, ensuring robust electrical contact and optimal RF/MW transmission efficiency for the quantum control pulses.
  • Precision Shaping and Cutting:
    • We offer Laser Cutting and Shaping services to produce custom geometries required for mounting the diamond sensor onto specialized stages (e.g., 3-axis piezo-positioners) or integrating into high-field magnet systems.
  • Expert Consultation: 6CCVD’s in-house PhD team specializes in quantum sensing materials and can assist researchers in optimizing material selection (e.g., choosing between SCD and PCD for ensemble sensing), determining optimal nitrogen doping strategies (intrinsic vs. implanted), and advising on post-processing parameters (irradiation fluence and annealing) for similar Nanoscale NMR and Quantum Sensing projects.
  • Global Logistics: We ensure reliable Global Shipping (DDU default, DDP available) of sensitive, high-value quantum-grade diamond materials, supporting international collaboration and research timelines.

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

View Original Abstract

Abstract Nitrogen vacancy (NV) centers are a major platform for the detection of nuclear magnetic resonance (NMR) signals at the nanoscale. To overcome the intrinsic electron spin lifetime limit in spectral resolution, a heterodyne detection approach is widely used. However, application of this technique at high magnetic fields is yet an unsolved problem. Here, we introduce a heterodyne detection method utilizing a series of phase coherent electron nuclear double resonance sensing blocks, thus eliminating the numerous Rabi microwave pulses required in the detection. Our detection protocol can be extended to high magnetic fields, allowing chemical shift resolution in NMR experiments. We demonstrate this principle on a weakly coupled 13 C nuclear spin in the bath surrounding single NV centers, and compare the results to existing heterodyne protocols. Additionally, we identify the combination of NV-spin-initialization infidelity and strong sensor-target-coupling as linewidth-limiting decoherence source, paving the way towards high-field heterodyne NMR protocols with chemical resolution.