Simulation of Indirect 13C–13C J-Coupling Tensors in Diamond Clusters Hosting the NV Center
At a Glance
Section titled “At a Glance”| Metadata | Details |
|---|---|
| Publication Date | 2022-04-22 |
| Authors | Alexander Nizovtsev, Aliaksandr Pushkarchuk, S. A. Kuten, Dominik L. Michels, Dmitry Lyakhov |
| Institutions | Institute of Physical and Organic Chemistry, National Research Nuclear University MEPhI |
| Citations | 1 |
| Analysis | Full AI Review Included |
Technical Documentation & Analysis: Indirect 13C-13C J-Coupling Tensors in NV-Hosting Diamond Clusters
Section titled “Technical Documentation & Analysis: Indirect 13C-13C J-Coupling Tensors in NV-Hosting Diamond Clusters”6CCVD specializes in providing high-pquality, custom-engineered MPCVD diamond materials essential for advanced quantum sensing and solid-state NMR research. This analysis connects the theoretical findings regarding nuclear spin interactions in NV-hosting diamond to specific material solutions available in our catalog.
Executive Summary
Section titled “Executive Summary”This research simulates the full 13C-13C J-coupling tensors in small H-terminated diamond clusters, focusing on the effect of the negatively charged Nitrogen-Vacancy (NV-) center. The findings are critical for advancing quantum memory and nanoscale sensing applications.
- Core Achievement: Successful simulation of the full JKL tensors for nearest-neighbor (N-N) 13C-13C pairs in diamond clusters, confirming the necessity of considering anisotropic contributions in solid-state NMR.
- NV Center Effect: The presence of the NV- center significantly perturbs the J-coupling characteristics, leading to an increase in the isotropic constant (Jiso) up to ~37.1 Hz for 13C pairs located near the vacancy.
- Material Implication: The observed ~9% increase in diagonal elements (JKK) near the NV vacancy highlights the sensitivity of nuclear spin dynamics to local electronic structure, demanding highly controlled, high-purity diamond hosts.
- Methodology: Density Functional Theory (DFT) calculations were performed using the ORCA 5.0.2 package (B3LYP/TZVPP level) on C10H16, C35H36, and C33[NV-]H36 clusters.
- Application Relevance: The data supports the development of long-lived quantum memory based on singlet-state 13C-13C dimers and the creation of nanoscale NV-based quantum sensors for chemical structure determination and biological imaging.
- 6CCVD Value Proposition: Experimental validation of these simulations requires high-quality Single Crystal Diamond (SCD) with precise isotopic control (13C enrichment/depletion) and ultra-low surface roughness (Ra < 1nm), all available through 6CCVD’s custom MPCVD capabilities.
Technical Specifications
Section titled “Technical Specifications”The following hard data points were extracted from the simulation results, focusing on the calculated J-coupling constants and structural parameters.
| Parameter | Value | Unit | Context |
|---|---|---|---|
| Experimental N-N 13C Jiso | 31.4 ± 0.5 | Hz | Reference value for nearest-neighbor 13C spins. |
| Calculated Jiso Range (C35H36) | 29.8 - 30.0 | Hz | Isotropic constant for N-N 13C pairs in the pure cluster. |
| Calculated Jiso (NV- Cluster, Max) | ~37.1 | Hz | Maximum Jiso observed for N-N 13C pairs nearest the NV vacancy. |
| JKK Diagonal Element Increase | ~9 | % | Increase in J-coupling matrix diagonal elements due to NV- presence. |
| Asymmetric Part (A1J) | -11.74 | Hz | Calculated for the C1-C2 pair in adamantane (transformed system). |
| C-C Bond Length (N-N) | ~1.54 | Å | Single bond separation in the diamond lattice model. |
| Cluster Size Modeled (NV Host) | C33[NV-]H36 | Atoms | H-terminated cluster hosting the negatively charged NV center. |
| Coordinate Angle (Tetrahedral) | 109.47 | ° | Angle between C-C bonds and the Z-axis for specific pairs. |
Key Methodologies
Section titled “Key Methodologies”The simulation relied on advanced quantum chemistry techniques to accurately model the spin interactions within the diamond lattice environment.
- Cluster Modeling: Diamond crystal structure was modeled using small H-terminated carbon clusters: C10H16 (adamantane), C35H36 (pure diamond model), and C33[NV-]H36 (NV center host).
- Software and Optimization: Geometry optimization was performed using the ORCA 5.0.2 software package.
- Optimization Level: B3LYP/def2/J/RIJCOSX level of theory was applied for geometry optimization.
- J-Coupling Simulation: The n-bond J-coupling tensors (JKL) were simulated using the B3LYP/TZVPP/AUTOAUX/decontract level of theory, recommended for high-resolution NMR calculations.
- Interaction Contributions: The calculation explicitly included all four primary contributions to the total JKL tensor:
- Diamagnetic contribution.
- Paramagnetic contribution.
- Fermi-Contact (FC) interaction (found to be the main contributor).
- Spin-Dipolar (SD) and SD/FC cross-term contributions.
- Focus: Analysis concentrated primarily on nearest-neighbor (N-N) 13C-13C pairs due to the rapid decrease in J-coupling magnitude with increasing bond order.
6CCVD Solutions & Capabilities
Section titled “6CCVD Solutions & Capabilities”The successful experimental realization and extension of this quantum simulation—particularly the creation of long-lived 13C quantum memory and high-sensitivity NV sensors—is fundamentally dependent on the quality and customization of the diamond substrate. 6CCVD provides the necessary materials and engineering support.
Applicable Materials
Section titled “Applicable Materials”To replicate or extend this research, researchers require diamond with precise control over purity and isotopic composition.
- Optical Grade SCD: Essential for maximizing the coherence time (T2) of the NV center, which is crucial for high-resolution NMR sensing. Our SCD material minimizes background defects that could interfere with the 13C spin bath.
- Custom Isotopic Diamond: Since the research focuses on 13C-13C interactions, control over the 13C concentration is paramount. 6CCVD offers:
- 12C Depleted SCD: To minimize the nuclear spin bath noise, allowing for clearer observation of specific 13C dimers.
- 13C Enriched SCD: To increase the density of the target 13C spins for enhanced signal or specific quantum memory designs.
- Substrate Thickness: We provide SCD plates ranging from 0.1µm to 500µm, and substrates up to 10mm thick, allowing flexibility for both thin-film device integration and bulk quantum experiments.
Customization Potential
Section titled “Customization Potential”6CCVD’s in-house capabilities directly address the stringent physical requirements of quantum device fabrication.
| Research Requirement | 6CCVD Customization Service | Specification Range |
|---|---|---|
| High-Resolution Sensing Surface | Precision Polishing | SCD: Ra < 1nm; PCD (Inch-size): Ra < 5nm. Essential for surface-based NV magnetometry. |
| Device Integration & Scaling | Custom Dimensions | Plates/wafers up to 125mm (PCD); custom laser cutting for specific chip geometries. |
| Electrical/Microwave Contact | In-House Metalization | Deposition of Au, Pt, Pd, Ti, W, and Cu for creating microwave striplines or electrical contacts necessary for NV manipulation. |
| NV Center Creation | Substrate Preparation | Providing ultra-low strain SCD substrates optimized for post-growth nitrogen implantation and annealing processes to achieve controlled NV- density. |
Engineering Support
Section titled “Engineering Support”6CCVD’s in-house PhD team specializes in the material science of diamond for quantum applications. We offer comprehensive support for projects involving:
- Material Selection: Assistance in choosing the optimal isotopic purity and crystal orientation for maximizing NV coherence (T2) and minimizing spectral diffusion.
- Surface Functionalization: Consultation on preparing diamond surfaces for detecting adsorbed molecules/radicals, a key application area identified in this paper.
- Custom Recipe Development: Collaboration on developing specific MPCVD growth recipes to meet unique thickness or doping requirements for similar solid-state NMR and quantum memory projects.
For custom specifications or material consultation, visit 6ccvd.com or contact our engineering team directly.
View Original Abstract
The full tensors nJKL (K,L = X,Y,Z), describing n-bond J-coupling of nuclear spins 13C in H-terminated diamond-like clusters C10H16 (adamantane) and C35H36, as well as in the cluster C33[NV&minus;]H36 hosting the negatively charged NV&minus;center, were simulated. We found that, in addition to the usually considered isotropic scalar nJ-coupling constant, the anisotropic contributions to the nJ-coupling tensor are essential. We also showed that the presence of the NV center affects the J-coupling characteristics, especially in the case of 13C&ndash;13C pairs located near the vacancy of the NV center.
Tech Support
Section titled “Tech Support”Original Source
Section titled “Original Source”References
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