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Microscopic Study of Optically Stable Coherent Color Centers in Diamond Generated by High-Temperature Annealing

MetadataDetails
Publication Date2022-08-16
JournalPhysical Review Applied
AuthorsKing Cho Wong, San Lam Ng, Kin On Ho, Yang Shen, Jiahao Wu
InstitutionsCenter for Integrated Quantum Science and Technology, University of Hong Kong
Citations12
AnalysisFull AI Review Included

Technical Documentation & Analysis: High-Temperature Annealing (HTA) for Coherent NV Centers

Section titled “Technical Documentation & Analysis: High-Temperature Annealing (HTA) for Coherent NV Centers”

This research demonstrates a novel, implantation-free High-Temperature Annealing (HTA) method for creating high-quality Nitrogen Vacancy (NV) centers in diamond, addressing critical challenges in solid-state quantum technology.

  • Implantation-Free Qubit Creation: HTA at 1700 °C utilizes thermal-induced vacancy activation and defect reformation, eliminating the lattice damage and noise sources inherent in traditional ion implantation methods.
  • Enhanced Coherence Time: The technique achieved a 3.3-fold improvement in the spin coherence time (T2) for high-nitrogen concentration samples (HPHT100), significantly reducing paramagnetic P1 noise centers.
  • High Yield in Ultra-Pure Diamond: For ultra-low nitrogen concentration SCD (< 3 ppb), the NV center yield was over 17%, resulting in an ideal concentration (> 1 center per 5 ”m3) for quantum computing and communication.
  • Spectrally Stable Qubits: Created NV centers exhibit exceptional optical stability, achieving a Fourier transform-limited linewidth of 24 MHz at 7 K, crucial for spin-photon entanglement.
  • Mechanism for Noise Reduction: HTA drives the conversion of noisy P1 centers into spinless defects (like H3) or NV centers, fundamentally reconfiguring the spin bath environment.
  • Industrial Applicability: This robust, scalable method is ideal for mass production of high-performance optical cavity and nanophotonics devices based on vacancy-based solid-state qubits.

The following hard data points summarize the key experimental parameters and performance metrics achieved using the HTA method:

ParameterValueUnitContext
HTA Peak Temperature1700°CHeld constant for 30 minutes
HTA Ramp-Up Rate45°C/minHeating from Room Temperature (RT)
HTA Cool-Down Rate-30°C/minCooling back to RT
Annealing Environment~1mbarVacuum purged with Argon (Ar)
NV Center Linewidth24MHzFourier transform-limited, measured at 7 K (Sample PPB-M)
NV Center Yield (Low [N])> 17%For samples with [N] < 3 ppb (PPB-B/M)
NV Concentration (Target)> 1 per 5 ”m3N/AEquivalent to 0.5 ppb [NV], ideal for quantum applications
T2 Coherence Time Improvement3.3FactorObserved in P1-dominated sample (HPHT100)
P1 Concentration Reduction (HPHT100)~17%Average reduction of original [P1] value after HTA
Ensemble Sensor Sensitivity Improvement3.6TimesOver naturally grown samples (Sample HPHT100)
Excitation Wavelength (PL)520nmUsed for normalized optical spectra
Excitation Wavelength (H3 PL)405nmUsed to confirm H3 defect increase

The experiment successfully created high-quality NV centers using a precise, thermal-activation-based protocol:

  1. Sample Selection: Four categories of diamond were used, ranging from ultra-low nitrogen SCD membranes (PPB-M, 20 ”m thick, [N] < 3 ppb) to high-concentration HPHT bulk diamond (HPHT100, [N] = 100 ppm).
  2. High-Temperature Annealing (HTA): Samples were placed in double graphite crucibles within a high-temperature furnace under a vacuum (~1 mbar Ar).
  3. Thermal Cycle: The temperature was ramped up at 45 °C/min to the peak of 1700 °C, held constant for 30 minutes, and then rapidly cooled down at -30 °C/min.
  4. Surface Cleaning: Post-annealing, samples underwent a boiling acid treatment (perchloric acid : nitric acid : sulfuric acid = 1:1:1) to remove graphitized surface layers.
  5. Characterization: Optical and spin properties were measured using:
    • Confocal microscopy (to confirm uniform NV creation in the bulk).
    • Photoluminescence Excitation (PLE) spectroscopy (to confirm Fourier transform-limited linewidth and spectral stability).
    • Free Induction Decay (FID) and Hahn Echo sequences (to measure T1 and T2 coherence times).
    • Double Electron-Electron Resonance (DEER) spectroscopy (to microscopically quantify P1 paramagnetic defect concentration).

The success of the HTA method hinges on the quality and purity of the starting diamond material, particularly the ultra-low nitrogen SCD and custom-dimension membranes. 6CCVD is uniquely positioned to supply the necessary materials and customization services required to replicate and advance this research.

To replicate the high-coherence results demonstrated in this paper, researchers require high-purity, low-strain diamond.

  • Optical Grade Single Crystal Diamond (SCD):
    • Requirement Match: The paper utilized ultra-low nitrogen concentration SCD (PPB-B/M, [N] < 3 ppb) to achieve high NV yield and spectral stability.
    • 6CCVD Offering: We provide Optical Grade SCD (Type IIa) with extremely low intrinsic nitrogen content, serving as the ideal host material for creating spectrally narrow, coherent NV centers via HTA.
  • Controlled-Doped SCD/PCD:
    • Requirement Match: The paper studied ensemble effects in CVD1 (1 ppm N) and HPHT100 (100 ppm N).
    • 6CCVD Offering: We offer Controlled Nitrogen-Doped SCD (Type Ib) or Polycrystalline Diamond (PCD) wafers, allowing precise control over the initial P1 center concentration for optimizing HTA parameters and maximizing ensemble sensor sensitivity.

The HTA method is cited as ideal for building high-performance optical cavity and nanophotonics devices, which require precise geometry and integration.

Research Requirement6CCVD Customization CapabilityValue Proposition
Diamond Membranes (e.g., 20 ”m thick)Custom Thickness SCD: We supply SCD wafers from 0.1 ”m up to 500 ”m thick, perfectly suited for membrane fabrication and subsequent HTA processing.Enables the creation of thin, high-quality quantum devices (e.g., solid immersion lenses, photonic structures) with optimal NV depth control.
High-Quality Surface FinishUltra-Low Roughness Polishing: SCD polished to Ra < 1 nm; Inch-size PCD polished to Ra < 5 nm.Minimizes surface defects and strain, ensuring the intrinsic spectral stability and low noise environment required for Fourier transform-limited linewidths.
Integrated Photonic StructuresCustom Metalization Services: We offer in-house deposition of Au, Pt, Pd, Ti, W, and Cu.Allows researchers to integrate NV centers with on-chip microwave antennas or optical components immediately following HTA processing.
Large-Scale ProductionLarge Format Wafers: PCD plates/wafers available up to 125 mm diameter.Supports industrial applications and mass production of quantum systems, leveraging the scalability of the HTA technique.

6CCVD’s in-house PhD team specializes in MPCVD growth and post-processing optimization. We can assist researchers in selecting the optimal starting material purity and crystal orientation to maximize NV center yield and coherence time for similar vacancy-based quantum technology projects.

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

View Original Abstract

Single color centers in solid have emerged as promising physical platforms for quantum information science. Creating these centers with excellent quantum properties is a key foundation for further technological developments. In particular, the microscopic understanding of the spin-bath environments is the key to engineer color centers for quantum control. In this work, we propose and demonstrate a distinct high-temperature annealing (HTA) approach for creating high-quality nitrogen vacancy (N-V) centers in implantation-free diamonds. Simultaneously using the created N-V centers as probes for their local environment we verify that no damage is microscopically induced by the HTA. Nearly all single N-V centers created in ultralow-nitrogen-concentration membranes possess stable and Fourier-transform-limited optical spectra. Furthermore, HTA strongly reduces noise sources naturally grown in ensemble samples, and leads to more than threefold improvements of decoherence time and sensitivity. We also verify that the vacancy activation and defect reformation, especially H3 and P1 centers, can explain the reconfiguration between spin baths and color centers. This distinct approach will become a powerful tool in vacancy-based quantum technology. © 2022 American Physical Society.