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Subdiffraction optical manipulation of the charge state of nitrogen vacancy center in diamond

MetadataDetails
Publication Date2015-01-02
JournalLight Science & Applications
AuthorsXiang-Dong Chen, Chang‐Ling Zou, Zhao-Jun Gong, Chun‐Hua Dong, Guang‐Can Guo
InstitutionsUniversity of Science and Technology of China
Citations120
AnalysisFull AI Review Included

Technical Analysis: Subdiffraction Optical Manipulation of NV Charge State in Diamond

Section titled “Technical Analysis: Subdiffraction Optical Manipulation of NV Charge State in Diamond”

This analysis reviews a breakthrough in quantum sensing microscopy using NV centers in diamond, specifically focusing on the Charge-State Depletion (CSD) method to achieve nanometer-scale resolution (4.1 nm). 6CCVD offers the high-purity Single Crystal Diamond (SCD) materials and precision engineering required to replicate and advance this research in quantum computing and nanoscale metrology.


The following points summarize the core technical achievement and commercial value of the research utilizing diamond NV centers for super-resolution microscopy:

  • Subdiffraction Resolution: Demonstrated successful subdiffraction optical manipulation of Nitrogen Vacancy (NV) charge states, achieving a best-case spatial resolution of 4.1 nm via Ionization-Charge-State Depletion (iCSD) microscopy.
  • Methodology: Leveraged wavelength-specific laser sequences (637 nm, 532 nm) and doughnut-shaped beams to control the charge conversion between the NV⁻ and NV⁰ states through a two-photon ionization/recharging process.
  • Enhanced Functionality: The CSD technique allows for selective detection and measurement of electron spin-state dynamics (ODMR and Ramsey fringes) of adjacent NV centers with high spatial separation.
  • Critical Material Requirement: The experiment necessitated ultra-high purity diamond substrates, specifically <100> oriented SCD with nitrogen concentrations verified to be <5 ppb.
  • Application Focus: This CSD microscopy technique is critical for advancing high-fidelity quantum manipulation, nanoscale sensing of electromagnetic fields, and studying coupled spin systems in solid-state quantum platforms.
  • Scalability Potential: The resolution improvement is theoretically unlimited and primarily constrained by laser stability and piezo stage drift (<0.15 nm s-1).

The following hard data was extracted from the experimental results regarding NV center performance and CSD implementation parameters:

ParameterValueUnitContext
Best Spatial Resolution (FWHM)4.1nmAchieved using iCSD (532 nm Doughnut beam)
Alternate Resolution (FWHM)28.6nmAchieved using rCSD (637 nm Doughnut beam)
Substrate Orientation<100>N/ADiamond plate specification
Initial Nitrogen Concentration<5ppbRequired material purity for low NV density
Excited State Lifetimes (NV⁻/NV⁰)~13nsConversion time constant
Optimal NV⁻ Population (Steady State)~75%Achieved using 532 nm G laser for initialization
Ionization Laser (Doughnut)532nm48 mW power, 200 ”s duration (for 4.1 nm resolution)
Recharging Laser (Doughnut)637nm22 mW power, 160 ”s duration
Charge Conversion ProcessTwo-photonN/ANon-linear power dependence observed
Detection/Readout Laser589nm0.1 mW power, 5 ”s duration

The core of the subdiffraction measurement relies on sequential laser pulsing and beam shaping to spatially localize the NV charge state conversion:

  1. Material Sourcing and NV Creation: High-purity, low-nitrogen concentration (<5 ppb) <100> SCD diamond plates were acquired. NV centers were created via Nâș ion implantation followed by thermal annealing.
  2. Beam Shaping and Switching: Laser sources (532 nm, 637 nm, 589 nm) were rapidly switched using acoustic optical modulators (AOMs). Doughnut-shaped depletion beams were created using movable phase masks.
  3. iCSD (Ionization) Sequence:
    • Initialization (637 nm G-laser): Used to initialize the NV population primarily into the NV⁰ charge state (~95%).
    • Depletion (532 nm D-laser): The doughnut beam converts NV⁰ back to NV⁻ only outside the beam center (null spot).
    • Readout (589 nm laser): Fluorescence detected, showing dark spots where conversion occurred, resulting in 4.1 nm resolution.
  4. rCSD (Recharging) Sequence:
    • Initialization (532 nm G-laser): Used to initialize the NV population primarily into the desired NV⁻ charge state (~75%).
    • Depletion (637 nm D-laser): The doughnut beam converts NV⁻ back to NV⁰ only outside the null spot.
    • Readout (589 nm laser): Fluorescence detected, showing bright spots where NV⁻ state was maintained.
  5. Spin-State Detection (ODMR): Optically Detected Magnetic Resonance (ODMR) was performed using microwave pulses between the initialization and readout steps to measure the electron spin-state dynamics (Rabi oscillations, Ramsey fringes) with subdiffraction spatial filtering provided by the CSD sequence.

6CCVD is uniquely positioned to supply the advanced materials necessary to replicate and push the boundaries of subdiffraction quantum metrology based on NV center charge control.

The foundation of this 4.1 nm resolution lies in the purity and crystalline quality of the substrate. To replicate or extend this work, researchers require the highest quality MPCVD diamond:

  • Material Recommendation: Optical Grade Single Crystal Diamond (SCD).
    • Purity: Guaranteed nitrogen concentration <1 ppb (exceeding the <5 ppb minimum stated in the paper) to minimize spectral diffusion and increase T2 coherence times.
    • Orientation: Available in <100> orientation plates, optimized for predictable post-growth NV formation kinetics via implantation/annealing.
    • Substrate Quality: SCD wafers up to 12 mm x 12 mm, necessary for robust optical setups and large-area scanning.

The optimization of CSD relies on high-quality optics and stable mounting, demanding precise geometric tolerances for the diamond substrate.

Capability6CCVD OfferingRelevance to Research
DimensionsCustom SCD wafers available up to 125mm (PCD) and large square SCD plates.Enables large-area scanning and scalability for advanced microscopy setups.
Thickness ControlSCD thickness from 0.1 ”m up to 500 ”m, and substrates up to 10 mm.Crucial for adapting sample depth to different numerical aperture (NA) objectives (e.g., dry vs. oil immersion).
Surface FinishUltra-smooth polishing with Ra < 1 nm (SCD).Essential for minimizing optical scattering and maximizing photon collection efficiency necessary for super-resolution microscopy.
MetalizationIn-house deposition of custom metal electrodes (Au, Pt, Ti, W, Cu).Allows for integration of on-chip microwave antennas (e.g., Ti/Pt/Au contact pads) directly onto the diamond surface for high-frequency ODMR and Rabi control experiments.

Achieving nanoscale resolution (4.1 nm) depends heavily on the interface between material defects and complex optics.

6CCVD’s in-house PhD engineering team specializes in the controlled formation and characterization of NV centers. We can provide consultation and support in:

  • Material Selection: Guiding selection of diamond purity and isotopic composition (e.g., 12C-enriched) to maximize T2 coherence times, critical for high-fidelity quantum metrology projects.
  • Post-Growth Integration: Assisting clients who perform their own Nâș implantation and annealing to ensure the precursor SCD material meets the specific requirements for controlled NV yield and depth.
  • Microscopy Optimization: Advising on material preparation (polishing, cleaning) necessary to support high numerical aperture oil objectives, which the paper suggests for future resolution improvement.

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

View Original Abstract

As a potential candidate for quantum computation and metrology, the nitrogen vacancy (NV) center in diamond presents both challenges and opportunities resulting from charge-state conversion. By utilizing different lasers for the photon-induced charge-state conversion, we achieved subdiffraction charge-state manipulation. The charge-state depletion (CSD) microscopy resolution was improved to 4.1 nm by optimizing the laser pulse sequences. Subsequently, the electron spin-state dynamics of adjacent NV centers were selectively detected via the CSD. The experimental results demonstrated that the CSD can improve the spatial resolution of the measurement of NV centers for nanoscale sensing and quantum information. The nitrogen vacancy (NV) in diamond is useful for quantum optics and spintronics due to the long coherence time of its electron spin state. Scientists in China have now used the techniques of super-resolution microscopy to optically control the charge state of an NV defect with a subdiffraction spatial resolution of 4.1 nm. Xiangdong Chen and co-workers from the University of Science and Technology of China in Hefei used a green (532 nm) laser beam to switch the charge state of the defect between NV0 and NV-. They achieved this manipulation on a subdiffraction scale by using specially shaped doughnut laser beams, in common with the principles of super-resolution stimulated emission depletion microscopy. This achievement represents a significant step towards nanoscale sensing and quantum information processing.