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Enhancement of quantum coherence in solid-state qubits via interface engineering

MetadataDetails
Publication Date2025-07-01
JournalNature Communications
AuthorsWing Ki Lo, Yaowen Zhang, H. Chow, Jiahao Wu, Man Yin Leung
InstitutionsHong Kong University of Science and Technology, University of Hong Kong
AnalysisFull AI Review Included
  • Coherence Breakthrough: Quantum coherence time (T2) for shallow Nitrogen-Vacancy (NV) centers in diamond was extended to over 1 ms (1063.8 ”s max), approaching the theoretical T1 limit (1.6 ± 0.3 ms).
  • Interface Engineering: The enhancement is achieved via a Graphene/Oxygen-terminated (O-terminated) diamond heterojunction, which suppresses surface spin noise.
  • Mechanism Verified: Raman spectroscopy and Density Functional Theory (DFT) confirmed that the O-termination facilitates electron transfer from the gapless Graphene, resulting in hole doping (~1012 cm-2). These transferred electrons pair with unpaired surface electrons.
  • Spin Noise Reduction: Double Electron-Electron Resonance (DEER) spectroscopy confirmed an order of magnitude reduction in unpaired electron spin concentration (~0.72 × 1011 cm-2) after patching.
  • Sensitivity Improvement: AC magnetic field sensitivity was enhanced from 50 nT/Hz1/2 to 16 nT/Hz1/2 using the CPMG-64 sequence.
  • Nanoscale Sensing Demonstrated: The enhanced T2 enabled the detection of weakly coupled internal 13C nuclear spins and external 11B nuclear spins from a hexagonal boron nitride (h-BN) capping layer, achieving nanoscale NMR.
  • Robust Platform: A protective h-BN top layer stabilizes the platform, allowing the device to be repeatedly cleaned via acid boiling and reused without removing the coherence-enhancing Graphene patch.
ParameterValueUnitContext
Maximum Coherence Time (T2)1063.8 ± 71.2”sShallow NV center (NV 17) using CPMG-64 sequence.
T1 Limit of NV Centers1.6 ± 0.3msApproaching limit achieved by interface engineering.
Hahn-Echo T2 Improvement1.2 to 3.3foldEnhancement observed across 20 shallow NV centers.
Best AC Magnetic Field Sensitivity16nT/Hz1/2Achieved using CPMG-64 sequence.
Initial AC Magnetic Field Sensitivity50nT/Hz1/2Before interface engineering.
Unpaired Electron Spin Concentration~0.72 × 1011cm-2Measured via DEER after graphene patching.
Graphene Hole Doping Concentration~1012cm-2Estimated from Raman G band blue shift.
G Band Blue Shift (Graphene/O-term)~3.8cm-1Relative to Graphene/h-BN reference.
NV Center Depth~5 to 20nmDepth of implanted NV centers below diamond surface.
13C Hyperfine Coupling Strength (A⊄)28 and 17kHzWeakly coupled 13C nuclear spins detected.
Graphene Transfer Annealing Temp150°CAnnealing temperature for 1 h post-transfer.
Graphene Transfer Sacrificial Layer Removal50°CAcetone bath temperature for 1 h.
External Magnetic Field (B)286GStandard field used for T2 and DEER measurements.
  1. Diamond Surface Termination: The diamond sample was cleaned using triacid boiling (concentrated perchloric, nitric, and sulfuric acids) to achieve Oxygen-termination (O-terminated), which stabilizes the NV negative charge state.
  2. NV Center Implantation: NV centers were created by growing a 6 nm p+ boron layer, followed by 9.8 keV 15N ion implantation (~109 N/cm2 dose), and subsequent annealing at 950 °C for 2 h.
  3. Graphene Patching: Graphene was transferred onto the O-terminated diamond surface using a standard floating method, immediately following the triacid boiling.
  4. Post-Transfer Curing: The graphene/diamond assembly was air-dried (30 min), annealed at 150 °C (1 h), and stored under vacuum (> 24 h) to enhance adhesion.
  5. Sacrificial Layer Removal: The sacrificial layer was removed by immersion in 50 °C acetone (1 h), followed by isopropyl alcohol (1 h), and N2 gas drying.
  6. Protective Capping Layer: A few micrometers of h-BN were transferred on top of the graphene-patched diamond to create the robust h-BN/Graphene/Diamond hetero-structure for external sensing.
  7. Quantum Sensing Sequences: Coherence time was measured using Hahn-echo (T2) and extended using Carr-Purcell-Meiboom-Gill (CPMG) dynamical decoupling sequences (up to N=64).
  8. Charge Transfer Analysis: Raman spectroscopy (532 nm excitation, 500 ”W power) was used to measure G and 2D band shifts, indicating hole doping. DFT calculations modeled the band alignment and charge transfer mechanism for O-terminated versus OH-terminated surfaces.
  • Nanoscale NMR and Spectroscopy: High-resolution detection and characterization of molecular structures, proteins, and biological systems at the atomic scale, enabled by the extended T2 coherence.
  • Quantum Material Characterization: Sensing weak magnetic signals from exotic two-dimensional (2D) magnetic materials and studying their interactions at the atomic level.
  • Reporter Spin Networks: Utilizing the highly coherent shallow NV centers as robust, sensitive reporters for imaging individual proton spins on the diamond surface.
  • High-Sensitivity Magnetometry: Development of practical, high-sensitivity AC magnetic field sensors (16 nT/Hz1/2) for use in ambient conditions without requiring complex purification or cryogenic setups.
  • Reusable Quantum Devices: The h-BN/Graphene capping layer creates a chemically robust platform that can be repeatedly cleaned using harsh acids and reloaded with new target samples (e.g., bio-samples, high-pressure materials) for continuous use.
  • Interface Engineering for Qubits: The demonstrated charge transfer mechanism provides a generalizable strategy for mitigating surface noise in other shallow solid-state qubits (e.g., SiV, GeV centers).