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All-optical nuclear quantum sensing using nitrogen-vacancy centers in diamond

MetadataDetails
Publication Date2023-06-10
Journalnpj Quantum Information
AuthorsBeat BĂŒrgler, Tobias F. Sjolander, Ovidiu Brinza, Alexandre Tallaire, Jocelyn Achard
InstitutionsCentre National de la Recherche Scientifique, Sorbonne Université
Citations22
AnalysisFull AI Review Included

This research introduces a novel, purely optical method for coherent quantum sensing using the 15N nuclear spin of the Nitrogen-Vacancy (NV) center in diamond, eliminating the need for traditional microwave (MW) or radio-frequency (RF) driving.

  • Core Innovation: Demonstration of all-optical Free Induction Decay (FID) measurements—the key protocol for low-frequency quantum sensing—on both single NV centers and NV ensembles.
  • Microwave-Free Operation: The scheme overcomes major limitations of conventional NV sensing (miniaturization, energy efficiency, and non-invasiveness) by relying solely on optical driving and static magnetic fields.
  • Coherent Initialization: Coherent superposition states of the 15N nuclear spin are prepared by optically pumping the NV center near the Excited State Level Anti-Crossing (ESLAC) in the presence of a small, static transverse magnetic field (Bperp).
  • Performance Metrics: Achieved nuclear spin coherence times (T2*) up to 508.5 ”s in NV ensembles, significantly longer than typical electron spin coherence times.
  • Optimal Conditions: Maximum FID contrast (Cmax ~4.2%) was observed at an optimal transverse magnetic field of approximately 8.6 G, corresponding to a tilt angle (Ίopt) of ~0.86°.
  • Projected Sensitivity: The all-optical protocol projects competitive shot-noise-limited sensitivities for ensemble magnetometry (1.22 nT Hz-1/2) and gyroscopy (135° hour-1/2).
  • Theoretical Framework: The dynamics are accurately modeled using an effective Hamiltonian derived via Van Vleck perturbation theory, confirming the role of the transverse field in tilting the nuclear quantization axis.
ParameterValueUnitContext
Sensing Resource15N Nuclear Spin (I=1/2)-Nitrogen-Vacancy (NV) Center
Electron SpinS=1-Quantized along NV axis
Electron Gyromagnetic Ratio (Îłs)2.8MHz G-1-
Nuclear Gyromagnetic Ratio (ÎłI)431.7Hz G-1-
Ground State ZFS (Dgs)2.87GHzZero-Field Splitting
Optimal Transverse Field (Bperp)~8.6GMaximizes FID contrast
Optimal Tilt Angle (Ίopt)~0.86°-
Max FID Contrast (Cmax)~4.2%Measured at Bext = 533 G
Single NV Coherence Time (T2*)248.1 ± 12.4”sAll-optical FID measurement
Ensemble NV Coherence Time (T2*)508.5 ± 17.4”sAll-optical FID measurement
Projected Ensemble Magnetometry Sensitivity1.22nT Hz-1/2Shot noise limited
Projected Ensemble Gyroscopy Sensitivity135° hour-1/2Shot noise limited
Excitation Wavelength515nmGreen laser (Cobolt 06-MLD)
Single NV Laser Power~50”WUsed for single nanopillar NV
Ensemble NV Laser Power2.2mWUsed for bulk unstructured diamond
Single NV Implantation Depth~9nmNominal depth (6 keV 15N ions)
Ensemble NV Density~300ppbEstimated 15NV density
  1. Sample Preparation (Single NV): Electronic grade diamond was implanted with singly charged 15N ions (6 keV, flux 1011 cm-2). Subsequent fabrication of parabolic diamond pillars enhanced photoluminescence (PL) collection efficiency.
  2. Sample Preparation (Ensemble NV): Unstructured diamond was grown via Chemical Vapor Deposition (CVD) along the (113) crystal orientation to promote preferential NV alignment. The growth used 12C and 15N enriched gas mixture, resulting in an estimated NV density of ~300 ppb.
  3. Optical Setup: Experiments were conducted using a home-built confocal microscope (NA = 0.8) employing a 515 nm green laser for excitation and collecting red PL for readout.
  4. Magnetic Field Control: A static magnetic field (Bext) was generated by a permanent neodymium disk magnet. This magnet was mounted on linear and goniometric stages for precise tuning of the field strength and tilt angle (Ί) near the NV Excited State Level Anti-Crossing (ESLAC).
  5. All-Optical FID Protocol: The measurement sequence consists of a green laser pulse separated by a variable free evolution delay (τ). The initial 350 ns of the pulse performs optical nuclear spin readout, while the remainder of the pulse (total duration 3 ”s) reinitializes the spin system.
  6. Theoretical Modeling: The system dynamics were simulated using a numerical model combining classical rate equations (for optical pumping) and master equations (for quantum evolution). An effective Hamiltonian for the 15N spin was derived using Van Vleck perturbation theory to predict precession frequency and quantization axis.

The development of all-optical, MW/RF-free coherent quantum sensing opens pathways for highly integrated and power-efficient devices in several key sectors:

  • Integrated Quantum Sensors: Enables the fabrication of highly compact, chip-scale quantum sensors by removing bulky and power-hungry MW/RF components.
  • Inertial Navigation and Gyroscopy: Provides a foundation for next-generation solid-state gyroscopes with competitive projected sensitivities (135° hour-1/2), suitable for autonomous systems and high-precision navigation.
  • Non-Invasive Magnetometry: Ideal for remote sensing applications (e.g., via optical fibers) or in environments where MW/RF fields must be avoided, such as sensitive biological or material science samples.
  • Medical and Biological Imaging: Potential for high-sensitivity magnetic detection of biological processes (e.g., single-neuron action potentials) without introducing RF heating or interference.
  • Fundamental Physics Research: Applicable to studying analogous dynamics in other novel solid-state color centers that exhibit suitable level anti-crossing behavior and coupling to nuclear spins.
View Original Abstract

Abstract Solid state spins have demonstrated significant potential in quantum sensing with applications including fundamental science, medical diagnostics and navigation. The quantum sensing schemes showing best performance under ambient conditions all utilize microwave or radio-frequency driving, which poses a significant limitation for miniaturization, energy efficiency, and non-invasiveness of quantum sensors. We overcome this limitation by demonstrating a purely optical approach to coherent quantum sensing. Our scheme involves the 15 N nuclear spin of the Nitrogen-Vacancy (NV) center in diamond as a sensing resource, and exploits NV spin dynamics in oblique magnetic fields near the NV’s excited state level anti-crossing to optically pump the nuclear spin into a quantum superposition state. We demonstrate all-optical free-induction decay measurements—the key protocol for low-frequency quantum sensing—both on single spins and spin ensembles. Our results pave the way for highly compact quantum sensors to be employed for magnetometry or gyroscopy applications in challenging environments.