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Identification and Control of Electron-Nuclear Spin Defects in Diamond

MetadataDetails
Publication Date2020-02-25
JournalPhysical Review Letters
AuthorsA. R. COOPER, Won Kyu Calvin Sun, Jean-Christophe Jaskula, Paola Cappellaro
InstitutionsCalifornia Institute of Technology, Massachusetts Institute of Technology
Citations26
AnalysisFull AI Review Included

This research demonstrates a systematic approach to scale quantum devices by identifying and controlling environmental spin defects (X spins) surrounding a Nitrogen-Vacancy (NV) center in isotopically-purified diamond.

  • Core Achievement: Successfully identified, located, and characterized two previously unknown electron-nuclear spin defects (X1 and X2) in the immediate environment of a single NV quantum probe.
  • Methodology: Employed rotational double electron-electron resonance spectroscopy (SEDOR) and Electron Spin Echo Envelope Modulation (ESEEM) to extract the full hyperfine and dipolar tensor parameters.
  • Defect Location: The defects were spatially located relative to the NV center: X1 at 9.23 nm and X2 at 6.58 nm.
  • Material Basis: Defects were created via 15N ion implantation (14 keV energy, 1013 cm-2 dose) into 99.999% 12C enriched CVD diamond.
  • Quantum Control: Demonstrated precise control over the three-spin system (NV, X1, X2) and successfully created quantum coherence among the three electron spins.
  • Future Impact: This approach provides a blueprint for assembling robust, multi-spin quantum registers necessary for scalable quantum information processing and quantum-enhanced sensing applications.
ParameterValueUnitContext
NV Zero-Field Splitting (Δ)2π · 2870MHzNV center electron spin ground state
Diamond Isotopic Purity99.999%12C enrichment level
Implantation Ion Species15NN/AUsed for creating NV centers and defects
Implantation Energy14keV15N ion implantation energy
Implantation Dose1013cm-215N ion implantation dose
Nano-aperture Diameter30nmUsed for confined ensemble implantation
Annealing Temperature800°CAnnealing time: 4 hours (to mobilize vacancies)
Mean Implantation Depth19.9nmSimulated depth of substitutional N defects
X1 Distance from NV (r1)9.23 ± 0.03nmEstimated spatial location
X2 Distance from NV (r2)6.58 ± 0.03nmEstimated spatial location
X1 Hyperfine A⊄17.2 ± 0.3MHzAxially symmetric tensor component
X1 Hyperfine A||29.4 ± 0.2MHzAxially symmetric tensor component
X2 Hyperfine A⊄1.6 ± 0.3MHzAxially symmetric tensor component
X2 Hyperfine A||11.2 ± 0.2MHzAxially symmetric tensor component
Dipolar Constant (dc)2π · 52.041kHzDipolar coupling for two electron spins at 1 nm distance
E-Beam Lithography Dose1400”C/cm2Used to pattern nano-apertures
SiO2 Layer Thickness10nmUsed to mitigate ion channeling
  1. Diamond Preparation: A single crystal CVD diamond substrate (100 ”m 12C layer on a 300 ”m electron grade substrate) was cleaned using boiling acid.
  2. Channeling Mitigation: A 10-nm SiO2 layer was deposited, followed by a 150 nm PMMA resist layer and thermally evaporated Au.
  3. Patterning: Electron-beam lithography (1400 ”C/cm2 dose) was used to pattern 30 nm diameter nano-aperture arrays in the resist stack.
  4. Ion Implantation: 15N ions were implanted through the apertures at 14 keV energy and a dose of 1013 cm-2 to create confined ensembles of defects.
  5. Defect Activation: The sample was annealed at 800 °C for 4 hours to promote vacancy mobility and form NV centers (low conversion efficiency).
  6. Surface Cleaning: Final cleaning involved a boiling mixture of concentrated acids (H2SO4:HNO3:HClO4 1:1:1) and routine piranha acid solution (H2O2:H2SO4 3:1).
  7. Magnetic Field Calibration: The static magnetic field strength (B0) and orientation (Ξ, φ) were precisely determined by measuring the NV electron spin resonance frequency (cw-ESR) and resolving spectral ambiguity using ESEEM spectroscopy of the host 15N nuclear spin.
  8. Defect Characterization and Location: Double electron-electron resonance (SEDOR) spectroscopy was performed across various magnetic field orientations. The resulting hyperfine and dipolar coupling strengths were fitted to parametric equations (tomographic reconstruction) to estimate tensor parameters and calculate the spatial coordinates (r, ζ, Ο) of X1 and X2.
  9. Quantum Control: The three-spin system was initialized using Hartmann-Hahn cross-polarization. CNOT gates were implemented using a recoupled spin-echo sequence to generate three-spin coherence, which was then detected via phase-modulated disentangling gates.
Industry/FieldApplicationRelevance to Paper
Quantum ComputingScalable Quantum RegistersThe ability to identify, locate, and control multiple environmental spins (X1, X2) allows for the assembly of larger, addressable quantum registers beyond the single NV center.
Quantum Sensing (Magnetometry)Enhanced Sensor SensitivityControlling environmental spins enables their use as auxiliary quantum resources, potentially leading to quantum-enhanced sensing protocols and improved sensitivity for detecting time-varying magnetic fields.
Solid-State Materials ScienceDefect Engineering & IdentificationProvides a systematic spectroscopic approach to characterize unknown electron-nuclear spin defects in solids, aiding in understanding defect formation mechanisms (e.g., nitrogen- or silicon-related centers from implantation).
Quantum CommunicationQuantum Repeater NodesThe controlled multi-spin system can serve as a quantum memory or repeater node, facilitating the transfer of quantum information between distant registers.
Surface ScienceMolecular Structure ProbingThe methodology is applicable to identifying complex spin systems, including unknown molecular structures or impurities placed near the diamond surface, relevant for nanoscale NMR.
View Original Abstract

We experimentally demonstrate an approach to scale up quantum devices by harnessing spin defects in the environment of a quantum probe. We follow this approach to identify, locate, and control two electron-nuclear spin defects in the environment of a single nitrogen-vacancy center in diamond. By performing spectroscopy at various orientations of the magnetic field, we extract the unknown parameters of the hyperfine and dipolar interaction tensors, which we use to locate the two spin defects and design control sequences to initialize, manipulate, and readout their quantum state. Finally, we create quantum coherence among the three electron spins, paving the way for the creation of genuine tripartite entanglement. This approach will be useful in assembling multispin quantum registers for applications in quantum sensing and quantum information processing.