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Relaxation of a dense ensemble of spins in diamond under a continuous microwave driving field

MetadataDetails
Publication Date2021-08-11
JournalScientific Reports
AuthorsJeson Chen, Oliver Y. Chén, Huan‐Cheng Chang
InstitutionsInstitute of Atomic and Molecular Sciences, Academia Sinica, Feng Chia University
Citations5
AnalysisFull AI Review Included

This research investigates the fundamental spin relaxation dynamics, specifically the baseline decay (Tb), in dense ensembles of negatively charged nitrogen-vacancy (NV-) centers in diamond under continuous microwave (MW) driving.

  • Core Achievement: First in-depth experimental measurement and analysis of the simple exponential (baseline) decay component of damped Rabi oscillations (RO) in high-density NV- ensembles.
  • Power Dependence: The baseline decay time (Tb) decreases significantly (up to 50%) as the MW magnetic field strength (Rabi frequency, ΩR) increases, particularly above 1 MHz.
  • Frequency Dependence: The dependence of Tb on MW detuning (δ) exhibits a clear Lorentzian-like spectral profile, with the minimum Tb occurring at the ODMR resonance frequency.
  • Modeling Success: Excellent agreement between experimental Tb spectra and numerical simulations based on the Bloch formalism was achieved only after incorporating the effect of inhomogeneous broadening (modeled with a 7 MHz Lorentzian width).
  • Decoherence Insight: The study confirms that MW-driven spin relaxation in dense ensembles consists of two distinct components: a fast, microsecond-scale oscillatory decay (Tr) and a slower, millisecond-scale baseline decay (Tb).
  • Material Metrics: Measured intrinsic relaxation times were T1 = 1491 ± 257 µs and T2 = 1.70 ± 0.13 µs, highlighting the severe reduction in T2 coherence time typical of dense, Type-Ib diamond.
ParameterValueUnitContext
NV Center Density~10ppmConcentration in Type-Ib diamond microcrystal.
Substitutional N Density~150ppmConcentration of intrinsic defects in the host matrix.
Sample Size~100µmDiameter of the Fluorescent Microdiamond (FMD) crystal.
Laser Wavelength532nmContinuous-wave (CW) laser for optical pumping and probing.
Laser Power Density~1kW/cm2Used throughout the study to minimize charge recombination effects.
Static Magnetic Field (B||)~6.6mTApplied to lift the spin degeneracy (Zeeman splitting).
Zero Field Splitting (D)2.87GHzGround state transition frequency (
Spin-Lattice Relaxation (T1)1491 ± 257µsMeasured intrinsic longitudinal relaxation time.
Spin-Spin Relaxation (T2)1.70 ± 0.13µsMeasured bath-decoupled transverse coherence time (Hahn echo).
Initialization Pulse Duration300µsOptimized duration to reach saturation of spin polarization.
Readout Pulse Duration0.5µsMinimum duration used for optical detection.
Inhomogeneous Broadening (Δωfs/2π)~7MHzWidth required in simulation for accurate frequency dependence modeling.
Baseline Decay Time (Tb) ChangeUp to 50%Decrease observed when Rabi frequency (ΩR/2π) exceeds 1 MHz.

The experiment utilized a home-built wide-field fluorescence imaging setup combined with pulsed laser and MW control sequences to measure spin relaxation dynamics.

  1. Experimental Setup:

    • A 532 nm CW laser was used for optical pumping and probing, controlled by an acoustic optical modulator (AOM).
    • Fluorescence was collected via a 40x objective and detected by an Intensified Charge-Coupled Device (ICCD) camera.
    • MW fields were generated by a synthesizer and amplifier, fed through a gold wire placed approximately 5 µm from the FMD sample.
    • A static magnetic field (B|| ≈ 6.6 mT) was applied to lift the spin degeneracy.
  2. Pulse Sequence and Normalization:

    • The measurement sequence consisted of a laser initialization pulse (300 µs), followed by a variable delay time (t) where MW was applied (for driven relaxation) or absent (for MW-free depolarization), and concluded with an optical readout pulse (0.5 µs).
    • Signals were normalized by alternating between a signal frame (variable t) and a reference frame (fixed 2 µs delay) to correct for low-frequency noise and laser intensity drift.
  3. Relaxation Time Characterization:

    • MW-Free Depolarization: Measured using the sequence without MW driving; fitted with a stretched-exponential function (β ≈ 0.5) to determine the MW-off decay time (Toff).
    • Intrinsic Times: T1 was measured using MW π pulses and optical readout; T2 was measured using the Hahn echo sequence.
    • MW-Driven Baseline Decay (Tb): Measured by applying CW MW during the variable delay t; data fitted using a double-stretched exponential model (Eq. 3) to account for contributions from both MW-resonant and non-resonant NV- centers.
  4. Theoretical Modeling:

    • The spin dynamics of a single NV center were modeled using the Bloch equations (density matrix formalism).
    • The analytical solution for the baseline decay rate (1/Tb) was derived, showing dependence on Rabi frequency (ΩR), detuning (δ), T1, and T2.
    • To match the experimental results from the dense ensemble, the single-spin Tb solution was convoluted with a Lorentzian function representing the 7 MHz inhomogeneous broadening (Δωfs/2π).

The fundamental understanding of spin relaxation under continuous driving fields in dense NV ensembles is crucial for advancing solid-state quantum technologies, particularly those relying on high-density defect materials.

  • Quantum Metrology and Sensing:

    • High-Density Sensors: Enables better design and optimization of ensemble NV- sensors for large-scale sensing applications (e.g., magnetic field, temperature, strain) where high signal-to-noise ratio is critical.
    • Continuous Wave Sensing: Provides a framework for understanding and optimizing CW-ODMR protocols, which are often used for high-bandwidth or continuous monitoring.
  • Quantum Information Processing:

    • Ensemble Quantum Computing: Essential for developing schemes for ensemble quantum computation, where the short coherence time (T2) and complex relaxation dynamics must be managed.
    • Qubit Control Fidelity: The analysis of baseline decay (Tb) helps isolate and mitigate decoherence mechanisms that limit the fidelity of continuous quantum operations.
  • Solid-State Physics and Materials Science:

    • Defect Characterization: Provides a sensitive method to characterize the effects of spin baths and inhomogeneous broadening in high-defect-density solid-state materials beyond diamond.
    • Dressed State Physics: The observed discrepancies at high MW power suggest the need for models incorporating dressed spin states, paving the way for advanced control techniques like decoherence suppression.