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Generation of Tin-Vacancy Centers in Diamond via Shallow Ion Implantation and Subsequent Diamond Overgrowth

MetadataDetails
Publication Date2020-02-07
JournalNano Letters
AuthorsAlison E. Rugar, Haiyu Lu, Constantin Dory, Shuo Sun, Patrick J. McQuade
InstitutionsSLAC National Accelerator Laboratory, Stanford University
Citations69
AnalysisFull AI Review Included

The research introduces the Shallow Ion Implantation and Growth (SIIG) method, a novel technique for generating high-quality, site-controlled Group-IV Tin-Vacancy (SnV-) centers in diamond.

  • Core Value Proposition: SIIG overcomes the critical trade-off between precise site control (achieved via implantation) and high emitter quality (typically achieved via synthesis/HPHT).
  • Methodology: Utilizes extremely low-energy (1 keV) Sn ion implantation through a thin PMMA mask, followed immediately by microwave-plasma Chemical Vapor Deposition (MPCVD) diamond overgrowth.
  • Quality Improvement: The subsequent CVD growth heals lattice damage and incorporates Sn atoms into the SnV- structure, resulting in clean bulk photoluminescence (PL) spectra free of extraneous defect peaks (631 nm and 647 nm).
  • Site Control: Demonstrated precise site-controlled generation with a 78% yield (at least one SnV- center per hole) in 30 nm patterned arrays.
  • Reduced Broadening: Optimized SIIG samples (Sample C) exhibit narrow inhomogeneous broadening (approximately 100 GHz), which is narrow enough for strain-tuning techniques required for quantum applications.
  • Compatibility: The method uses standard MPCVD growth conditions for pure diamond, making it highly compatible with existing diamond nanophotonic device fabrication techniques.
ParameterValueUnitContext
Implantation Energy (Shallow)1keVSIIG method (Sample B/C)
Implantation Energy (Baseline)370keVVacuum Anneal (Sample A)
Implantation Dose2 x 1013cm-2Used for all samples
Ion Localization Depth (SRIM)~2nmDepth of Sn ions after 1 keV implantation
Lateral/Longitudinal Straggle (SRIM)3AngstromCalculated straggle for 1 keV Sn+
PMMA Mask Thickness~50nmUsed to stop 1 keV ions
MPCVD Overgrowth Thickness90nmNominal thickness grown on Sample B
SnV- Zero-Phonon Line (ZPL)~620nmCharacteristic emission wavelength
Inhomogeneous Broadening (Sample A, C transition)263 ± 5GHzBaseline (Implanted/Vacuum Annealed)
Inhomogeneous Broadening (Sample C, C transition)101 ± 1GHzOptimized SIIG result
Site Control Yield78%Percentage of 30 nm holes yielding >= 1 SnV- center
Conversion Efficiency Estimate>1%Estimated for patterned array
Vacuum Anneal Temperature (Sample A)800 / 1100°CTwo stages, 30 minutes each
MPCVD Stage Temperature650°CDiamond overgrowth temperature
MPCVD Pressure23TorrDiamond overgrowth pressure

The SIIG method (Shallow Ion Implantation and Growth) applied to Sample B involved the following sequential steps:

  1. Initial Preparation:

    • Clean electronic grade diamond plate using a boiling tri-acid solution (1:1:1 sulfuric:nitric:perchloric acids).
    • Remove 500 nm of diamond via O2 plasma etch.
  2. Mask Fabrication:

    • Spin-coat a thin layer (~50 nm) of poly(methyl methacrylate) (PMMA, 950 PMMA A2).
    • Pattern arrays of square holes (20 nm to 150 nm side length) using electron-beam (e-beam) lithography.
    • Develop the PMMA mask in a 5°C 3:1 solution of isopropanol:water.
  3. Shallow Ion Implantation:

    • Implant 120Sn+ ions at a low energy of 1 keV.
    • Implantation dose was 2 x 1013 cm-2.
  4. Surface Preparation for Growth:

    • Remove the PMMA mask using Remover PG.
    • Clean the diamond surface using H2 plasma to remove unwanted sp2-bonded carbon resulting from implantation damage.
  5. Diamond Overgrowth (MPCVD):

    • Immediately grow a nominally 90-nm thick layer of diamond using Microwave-Plasma CVD (Seki Diamond Systems SDS 5010).
    • Gas Flows: H2 at 300 sccm; CH4 at 0.5 sccm.
    • Conditions: Stage temperature 650°C; Microwave power 1100 W; Pressure 23 Torr.
    • Mechanism: The growth process heals the damaged lattice and incorporates the shallowly implanted Sn atoms into the growing sp3 lattice to form SnV- centers.

The SIIG method provides a scalable, high-quality manufacturing route for quantum emitters, addressing key challenges in integrating solid-state spin qubits into functional devices.

  • Quantum Network Nodes: SnV- centers are highly promising solid-state spin qubits due to their long spin coherence times without requiring dilution refrigeration, making them ideal candidates for quantum memory and repeater nodes.
  • Integrated Nanophotonics: The high-precision, site-controlled placement of emitters is essential for coupling them efficiently to nanophotonic structures (e.g., diamond microdisks, photonic crystal cavities) for enhanced photon collection and quantum-optical interfaces.
  • Scalable Quantum Device Fabrication: SIIG is compatible with existing diamond fabrication techniques (etching, inverse design) and uses standard CVD growth parameters, enabling the mass production of quantum chips and arrays.
  • Quantum Sensing: High-quality, low-strain SnV- centers can be used as sensitive probes for electric and magnetic fields in diamond-based quantum sensors.
  • New Material Discovery: The versatility of SIIG—using low-damage implantation followed by growth—can be extended beyond diamond and SnV- to accelerate the discovery and optimization of new color centers in various host materials (e.g., Lead-related emitters).
View Original Abstract

Group IV color centers in diamond have garnered great interest for their potential as optically active solid-state spin qubits. The future utilization of such emitters requires the development of precise site-controlled emitter generation techniques that are compatible with high-quality nanophotonic devices. This task is more challenging for color centers with large group IV impurity atoms, which are otherwise promising because of their predicted long spin coherence times without a dilution refrigerator. For example, when applied to the negatively charged tin-vacancy (SnV<sup>-</sup>) center, conventional site-controlled color center generation methods either damage the diamond surface or yield bulk spectra with unexplained features. Here we demonstrate a novel method to generate site-controlled SnV<sup>-</sup> centers with clean bulk spectra. We shallowly implant Sn ions through a thin implantation mask and subsequently grow a layer of diamond via chemical vapor deposition. This method can be extended to other color centers and integrated with quantum nanophotonic device fabrication.