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Probing the Evolution of the Electron Spin Wave Function of the Nitrogen-Vacancy Center in Diamond via Pressure Tuning

MetadataDetails
Publication Date2022-12-14
JournalPhysical Review Applied
AuthorsKin On Ho, Man Yin Leung, Prithvi Reddy, Jianyu Xie, King Cho Wong
InstitutionsUniversity of Hong Kong, Chinese University of Hong Kong, Shenzhen
Citations8
AnalysisFull AI Review Included

Technical Documentation: MPCVD Diamond for High-Pressure Quantum Sensing (NV Centers)

Section titled “Technical Documentation: MPCVD Diamond for High-Pressure Quantum Sensing (NV Centers)”

This document analyzes the research paper “Probing the Evolution of Electron Spin Wavefunction of NV Center in diamond via Pressure Tuning” and outlines how 6CCVD’s advanced MPCVD diamond materials and processing capabilities can support and extend this critical work in quantum metrology and defect physics.


The research successfully utilized hydrostatic pressure tuning combined with Optically Detected Magnetic Resonance (ODMR) to investigate the fundamental properties of the Nitrogen Vacancy (NV) center electron spin wavefunction in diamond.

  • Core Achievement: First demonstration of measuring stress-dependent hyperfine interaction in a point defect system, using the nearest-neighbor 13C nuclear spin as an atomic-scale probe.
  • Methodology: High-pressure ODMR spectroscopy was performed using a Diamond Anvil Cell (DAC) up to 104.5 kbar on 1-”m diamond particles.
  • Physical Insight: Applied pressure causes a prominent change in NV hyperfine parameters, resulting in an increase in the NV electron spin density ($\eta$) and a rehybridization of the defect orbitals from sp3 toward sp2 bonds.
  • Validation: Experimental results show excellent agreement with independent ab initio Density Functional Theory (DFT) calculations of strain dependence without introducing fitting parameters.
  • Technical Advantage: Pressure tuning provides a cleaner, stronger, and more systematic method for studying lattice changes and their effect on quantum defects compared to thermal methods.
  • 6CCVD Value Proposition: The paper explicitly notes that using 13C enriched samples would significantly enhance resolution and accuracy, a key customization capability offered by 6CCVD for SCD and PCD materials.

The following hard data points were extracted from the experimental and theoretical results presented in the paper, focusing on the NV center parameters under pressure tuning.

ParameterValueUnitContext
Maximum Hydrostatic Pressure Applied104.5kbarAchieved using 4:1 methanol:ethanol medium in DAC
NV Center Zero-Field Splitting (Ambient, D)~2870MHzStandard ODMR transition frequency
13C Hyperfine Splitting (Ambient, $\Delta$hf(0))127.604MHzTheoretical value (in agreement with experiment)
13C Hyperfine Center (Ambient, $\delta$hf(0))2876.86MHzTheoretical value (in agreement with experiment)
Pressure Dependence Slope ($\Delta$hf$/$dP) | 0.034 to 0.036 | MHz/kbar | Experimental range for 13C hyperfine splitting |
| Pressure Dependence Slope ($\delta$hf$/$dP) | 1.463 to 1.500 | MHz/kbar | Experimental range for 13C hyperfine center |
| Electron Spin Density Trend ($\eta$) | Increases | N/A | Under applied hydrostatic pressure |
| p-Orbital Hybridization Trend (|cp2)DecreasesN/A
Diamond Particle Size Used1”mCommercial Nanodiamonds (NDs)
MW Antenna Geometry150”m diameterOmega-shaped gold micro-structure fabricated on anvil

The experiment relied on precise material handling and advanced high-pressure ODMR techniques:

  1. Sample Preparation: Commercial 1-”m nanodiamond particles (NDs) were drop-casted onto the culet of one diamond anvil.
  2. High-Pressure Setup: A Diamond Anvil Cell (DAC) was employed, utilizing a metallic gasket with a 300 ”m central hole to confine the sample and the 4:1 methanol:ethanol pressure medium.
  3. MW Antenna Fabrication: A 150-”m diameter omega-shaped gold micro-structure was fabricated directly onto one anvil to serve as the microwave (MW) antenna, ensuring uniform and reliable MW transmission [50].
  4. Pressure Calibration: In situ pressure was calibrated by monitoring the center frequency (D) of the corresponding NV ODMR spectrum, using the known spin-stress interaction dD/dP = 1.49 MHz/kbar.
  5. ODMR Measurement: Non-uniform ODMR measurements were implemented, using smaller MW frequency steps in the hyperfine resonance regions to retain high spectral resolution while minimizing measurement time.
  6. Wavefunction Analysis: Measured hyperfine parameters ($\Delta$hf$/$P and $\delta$hf$/$P) were converted using established relations (Equations 4-7) to determine the pressure-dependent changes in the Fermi contact term ($f$), dipole term ($d$), electron spin density ($\eta$), and orbital hybridization (|cp|2).

This research highlights the critical need for high-quality, customized diamond materials to push the boundaries of quantum sensing under extreme conditions. 6CCVD is uniquely positioned to supply the necessary materials and processing services to replicate and extend this work, particularly addressing the sensitivity limitations noted in the paper.

The paper notes that the low natural abundance of 13C (1.1%) limits sensitivity and suggests using 13C enriched samples to reach higher accuracy.

Material Requirement6CCVD SolutionTechnical Advantage
High-Purity Host MaterialOptical Grade SCD (Single Crystal Diamond)SCD offers superior crystalline quality and minimal background defects, crucial for high-fidelity quantum measurements.
Enhanced Sensitivity/ResolutionCustom 13C Enriched SCD6CCVD offers CVD diamond grown with controlled 13C isotopic enrichment, directly addressing the paper’s limitation of low 13C concentration for improved ENDOR/NMR sensitivity.
High-Pressure SubstratesSCD Substrates (up to 10mm thickness)Providing robust, high-quality SCD material for use as DAC anvils or high-pressure windows, ensuring minimal background noise.
Nanodiamond ReplicationCustom PCD or SCD Micro-ParticlesWhile the paper used commercial NDs, 6CCVD can supply high-quality, size-controlled PCD or SCD micro-particles for drop-casting experiments, ensuring better material consistency.

The experimental setup required specialized micro-fabrication on the diamond anvils. 6CCVD offers comprehensive processing services to meet these precise engineering needs:

  • Custom Dimensions: 6CCVD can supply plates and wafers up to 125mm (PCD) or custom-cut SCD pieces, precisely sized for DAC components.
  • Precision Polishing: The SCD material can be polished to an ultra-low surface roughness (Ra < 1 nm), ensuring optimal optical access and minimal surface strain effects during ODMR measurements.
  • Advanced Metalization: The experiment required a 150 ”m omega-shaped gold micro-structure for the MW antenna. 6CCVD offers in-house metalization capabilities, including Au, Ti, Pt, Pd, W, and Cu, allowing researchers to integrate custom antenna geometries directly onto the diamond surface with high precision.
  • Laser Cutting and Shaping: We provide precise laser cutting services to shape diamond plates into specific geometries required for DAC components or custom MW transmission structures.

The analysis of NV center wavefunctions involves complex theoretical modeling (DFT, Hamiltonian solving) highly sensitive to material parameters (e.g., the $\delta$hf$/$dP slope).

6CCVD’s in-house PhD team specializes in the growth and characterization of quantum-grade diamond. We offer expert consultation to assist researchers in:

  1. Material Optimization: Selecting the optimal 13C enrichment level and nitrogen concentration for maximizing signal contrast and coherence time in similar high-pressure quantum sensing projects.
  2. Defect Engineering: Tailoring the CVD growth recipe to control the density and location of NV centers for specific experimental requirements (e.g., near-surface NV centers for enhanced sensing).
  3. Global Logistics: Ensuring reliable global shipping (DDU default, DDP available) for sensitive, high-value materials required for international research collaborations.

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

View Original Abstract

Understanding the profile of a qubit’s wave function is key to its quantum applications. Unlike conduct-ing systems, where a scanning tunneling microscope can be used to probe the electron distribution, there is no direct method for solid-state-defect-based qubits in wide-band-gap semiconductors. In this work, we use pressure as a tuning method and a nuclear spin as an atomic scale probe to monitor the hyperfine structure of negatively charged nitrogen-vacancy (N -V) centers in diamonds under pressure. We present a detailed study on the nearest-neighbor 13C hyperfine splitting in the optically detected magnetic reso-nance spectrum of N -V centers at different pressures. By examining the 13C hyperfine interaction upon pressurizing, we show that the N -V hyperfine parameters have prominent changes, resulting in an increase in the N -V electron spin density and rehybridization from sp3 to sp2 bonds. The ab initio calculations of strain dependence of the N -V center’s hyperfine levels are done independently. The theoretical results qualitatively agree well with experimental data without introducing any fitting parameters. Furthermore, this method can be adopted to probe the evolution of wave function in other defect systems. This potential capability could play a role in developing magnetometry and quantum information processing using the defect centers.