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An ultrafast diamond nonlinear photonic sensor

MetadataDetails
Publication Date2025-09-25
JournalNature Communications
AuthorsDaisuke Sato, Junjie Guo, Takuto Ichikawa, Dwi Prananto, Toshu An
InstitutionsKeio University, Japan Advanced Institute of Science and Technology
AnalysisFull AI Review Included

This research introduces an ultrafast diamond nonlinear photonic sensor, leveraging Nitrogen-Vacancy (NV) centers to achieve unprecedented spatio-temporal resolution for electric field sensing.

  • Core Achievement: Developed a nanoscopic electro-optic (EO) sampling technique that breaks the diffraction limit of light and the nanosecond time resolution limit of conventional NV sensing (ODMR).
  • Resolution Metrics: Achieved spatial resolution potentially ≀ 500 nm and temporal resolution ≀ 100 fs.
  • Sensing Mechanism: Utilizes the Pockels EO effect in a diamond nanotip. NV defects locally break the crystal’s spatial inversion symmetry, resulting in a non-zero second-order nonlinear susceptibility (χ(2) ≠ 0).
  • Demonstration: Successfully measured the dynamics of the surface electric field (carrier screening and relaxation) on a prototypical semiconductor (n-GaAs) and a two-dimensional material (WSe2 monolayer and bulk).
  • Key Finding in WSe2: Observed distinct double exponential relaxation dynamics in bulk WSe2 (t1 ≈ 0.3 ps, t2 ≈ 2.2 ps), attributed to intervalley scattering followed by trapping by surface defect states.
  • Value Proposition: Provides a critical tool for developing next-generation nanometer-scale quantum devices by enabling high-resolution sensing of electric, magnetic, and thermal fields.
ParameterValueUnitContext
Spatial Resolution (Potential)≀ 500nmLimited by NV tip apex size and EO enhancement
Temporal Resolution (Achieved)≀ 100fsFWHM of shortest EO response
Pump Laser Pulse Length≀ 10fsTi: sapphire oscillator
Pump Laser Wavelength795nmCenter wavelength (1.56 eV)
Pump Fluence (WSe2)215”J cm-2Generates carrier density ~1.35 x 1013 cm-2
NV Implantation Energy30keV14N+ ions
NV Implantation Depth~40nmDeduced from SRIM simulation
NV Annealing Temperature900°C1 hour in Ar atmosphere
GaAs Relaxation Time (Macroscopic)~1.1psCarrier relaxation/diffusion
GaAs Relaxation Time (Local, NV Tip)~0.5psFaster due to surface effects
WSe2 Bulk Relaxation Time (t2)2.2 ± 0.1psAttributed to trapping by surface defect states
WSe2 1ML Relaxation Time0.2 ± 0.1psStrong coupling to SiO2 substrate
Estimated Electric Field Sensitivity~100V cm-1 Hz-1/2Based on n-GaAs EO signal and noise level
GaAs Macroscopic ΔE~-3.1 x 106V m-1Maximum experimental EO response
  1. Diamond NV Probe Fabrication:

    • Material: (100)-oriented CVD-grown electronic-grade bulk diamond (< 5 ppb initial N impurities).
    • NV Creation: 14N+ ion implantation at 30 keV, followed by annealing at 900 °C for 1 hour in an Argon (Ar) atmosphere.
    • Tip Shaping: Laser cutting and Gallium ion (Ga+) Focused Ion Beam (FIB) milling used to define the nanotip geometry.
    • Integration: Probe attached to a self-sensing cantilever for Atomic Force Microscopy (AFM) force detection.
  2. WSe2 Sample Preparation:

    • Monolayer (1ML) and bulk WSe2 prepared from a single crystal.
    • Substrate was Si covered with a 100-nm SiO2 layer.
    • Au-assisted transfer method used to place WSe2 onto the substrate.
  3. Ultrafast Electro-Optic (EO) Sampling Setup:

    • Technique: Reflective pump-probe scheme combined with AFM (Scanning Probe Microscopy).
    • Light Source: Ti: sapphire femtosecond oscillator (≀ 10 fs pulse length, 795 nm center wavelength, 75 MHz repetition rate).
    • Optics: Reflective (Schwarzschild) objective lens used to inject the probe beam from the back side of the tip to minimize dispersion.
    • Time Delay: Modulated by an oscillating retroreflector (shaker) in the pump path at 10 Hz.
  4. Sensing Mode (Pin-Point AFM):

    • The AFM system operated in “pin-point mode,” vertically approaching and retracting the diamond NV probe at designated points.
    • This ensures the diamond probe maintains a quasi-zero distance (typically 0.1-0.3 nm) from the sample surface during measurement.
    • The EO signal (anisotropic reflectivity change) was detected by a 1 GHz high-speed Si-PIN photodetector, with noise reduction achieved via signal integration (5000 accumulations).
Industry/FieldApplication AreaRelevance to Technology
Quantum Sensing & MetrologyNext-generation quantum sensors and electrometers.Provides the necessary spatio-temporal resolution (nm/fs) to characterize localized electric fields in single-spin systems and quantum devices, surpassing ODMR limits.
2D Materials ResearchCharacterization of Transition Metal Dichalcogenides (TMDCs) and topological insulators.Enables direct, nanoscopic measurement of ultrafast carrier dynamics (Mott transition, scattering, defect trapping) crucial for optimizing 2D material performance.
High-Speed PhotonicsOptical switches, modulators, and integrated circuits.The EO effect is fundamental to these devices. The technique allows for high time-resolution testing of components operating in the sub-picosecond regime.
Semiconductor Device EngineeringPower device materials (e.g., SiC) and compound semiconductors (GaAs).Allows for the measurement of electric field distribution and carrier transport dynamics near surfaces and interfaces, critical for device reliability and performance.
Nanoscopy Tool DevelopmentAdvanced Scanning Probe Microscopy (SPM) systems.The diamond NV probe concept can be integrated into commercial SPM platforms (e.g., QZabre, Qnami) to create hybrid tools offering combined AFM, ultrafast spectroscopy, and quantum sensing capabilities.