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Identification and Reversible Optical Switching of NV+ Centers in Diamond

MetadataDetails
Publication Date2025-03-30
JournalAdvanced Functional Materials
AuthorsMarcel Dickmann, Lucian Mathes, Ricardo Helm, Vassily Vadimovitch Burwitz, Werner Egger
InstitutionsTechnical University of Munich, Heinz Maier-Leibnitz Zentrum
Citations1
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Technical Analysis & Documentation: Reversible Optical Switching of NV+ Centers in Diamond

Section titled “Technical Analysis & Documentation: Reversible Optical Switching of NV+ Centers in Diamond”

This research successfully identifies and characterizes the positively charged Nitrogen-Vacancy (NV+) center in high-purity CVD diamond, a critical step for advanced quantum technologies.

  • NV+ Identification: Experimental confirmation of the elusive NV+ center, previously only inferred, using Positron Annihilation Lifetime Spectroscopy (PALS) combined with in situ light illumination.
  • Reversible Switching: Demonstration of reversible optical charge state switching from NV+ to the detectable neutral state (NV0).
  • Critical Energy Threshold: The charge transition (NV+ to NV0) requires a threshold photon energy of 1.234(8) eV, aligning with theoretical predictions.
  • Metastable State Lifetime: The resulting NV0 state is metastable in complete darkness, decaying back to NV+ with a characteristic lifetime of 1.73(22) hours.
  • Material Requirement: The study relies on ultra-low impurity, single crystal CVD diamond to ensure controlled defect creation via N+ implantation and subsequent high-temperature annealing (1200 °C).
  • Quantum Relevance: These findings are essential for developing long-lived quantum data storage and scalable quantum computer architectures utilizing the NV+ center’s unique spin properties.

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

ParameterValueUnitContext
Initial Nitrogen Purity< 5ppbSingle Crystal CVD Diamond (SCD)
Initial Boron Purity< 1ppbSingle Crystal CVD Diamond (SCD)
Crystal Orientation(100)N/ASubstrate used for implantation
N+ Implantation Energy0.5MeVUsed to create NV precursors
N+ Implantation Fluence1.0 · 1014cm-2Chosen for high NV concentration
Annealing Temperature1200°CUsed for NV center formation
Annealing Time2hUsed for NV center formation
NV+ to NV0 Transition Energy1.234(8)eVThreshold photon energy (Eph)
NV0 Decay Time (in darkness)1.73(22)hCharacteristic lifetime (t1/e)
Calculated Bulk Positron Lifetime103psPerfect diamond lattice
Measured NV Center Lifetime145(12)psAssociated with NV0 or NV- centers
Positron Implantation Depth (12 keV)596nmOverlaps well with N+ distribution

The experimental success hinges on precise material preparation and advanced spectroscopic techniques:

  1. High-Purity Substrate Preparation: Utilization of commercial single crystal CVD diamond with ultra-low native nitrogen (< 5 ppb) and boron (< 1 ppb) to ensure defect control.
  2. Controlled Defect Introduction: Implantation of 0.5 MeV N+ ions at a fluence of 1.0 · 1014 cm-2 to introduce nitrogen and vacancies without causing bulk amorphization.
  3. Thermal Activation: Subsequent high-temperature annealing at 1200 °C for 2 hours to mobilize vacancies, allowing them to bind with substitutional nitrogen to form NV centers.
  4. Depth-Resolved Positron Spectroscopy: Application of Mono-energetic Positron Spectroscopy (MePS) at variable energies (4 keV and 12 keV) to probe defect structures at specific depths (82 nm and 596 nm).
  5. In Situ Charge Manipulation: Combination of Doppler-Broadening Spectroscopy (DBS) and PALS with monochromatic light illumination (1.1 - 1.4 eV range) to induce and monitor the NV+ to NV0 charge transition.
  6. DFT Verification: Density Functional Theory (DFT) calculations were used to predict positron lifetimes for various defects (NV0, NV-, V1, Vn clusters) to verify experimental PALS results.

6CCVD is uniquely positioned to supply the foundational materials and customization services required to replicate, extend, and scale this critical quantum research.

To achieve the controlled NV center formation and high-fidelity measurements demonstrated in this paper, researchers require the highest quality starting material:

  • Optical Grade Single Crystal Diamond (SCD): The core material used in this study. 6CCVD supplies ultra-high purity SCD with native nitrogen levels typically < 1 ppb. This low background impurity is essential for controlling the Fermi level and ensuring that implanted nitrogen dominates the NV center population.
  • Boron-Doped Diamond (BDD): The paper notes that NV+ formation requires a Fermi level close to the valence band, often achieved by acceptor doping (e.g., boron). 6CCVD offers custom BDD materials, allowing precise control over boron concentration to tune the Fermi level and optimize the initial NV+ population for quantum device integration.

6CCVD’s advanced MPCVD and post-processing capabilities directly address the needs of quantum material engineering:

Research Requirement6CCVD CapabilityTechnical Specification
Substrate DimensionsCustom Plates and WafersSCD up to 500 ”m thick; PCD up to 125mm diameter
Surface QualityUltra-Precision PolishingSCD: Ra < 1 nm; Inch-size PCD: Ra < 5 nm
OrientationSpecific Crystal CutsAvailable (100) orientation, matching the study’s requirements
Post-ProcessingMetalization ServicesIn-house deposition of Au, Pt, Pd, Ti, W, Cu for electrical contacts (critical for bias-voltage switching applications)
Thickness ControlSCD Layer GrowthSCD layers available from 0.1 ”m up to 500 ”m, allowing precise control over the active quantum layer depth

The successful manipulation of NV charge states requires deep expertise in defect engineering and material science.

  • Defect Engineering Consultation: 6CCVD’s in-house PhD team can assist researchers in optimizing material selection and specifications for similar NV Center Quantum Technology projects, including advising on optimal starting purity, target implantation fluence, and post-growth annealing protocols (like the 1200 °C anneal used here).
  • Global Logistics: We ensure reliable, secure global shipping (DDU default, DDP available) of sensitive, high-value diamond substrates directly to research facilities worldwide.

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

View Original Abstract

Abstract Positive nitrogen‐vacancy centers (NV + ) in diamond are predicted to exist in conjunction with neutral (NV 0 ) and negative (NV − ) centers. However, the existence of NV + has only been indirectly inferred through a shift of the Fermi level. Evidence of NV + coexisting with NV 0 and NV - in diamond has not yet been observed. In this paper, positron annihilation spectroscopy in combination with in situ light illumination is applied, in order to investigate the presence of NV + centers in nitrogen implanted and subsequently annealed diamond. Switching of NV + to NV 0 centers is observed with a threshold photon energy of 1.234(8) eV. In complete darkness, a decay of NV 0 centers with a decay time of 1.73(22) h can be detected. In conclusion, previously converted NV 0 centers are metastable and partially decay in darkness, leading to the reformation of NV + centers.