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Nanoscale-NMR with Nitrogen Vacancy center spins in diamond

MetadataDetails
Publication Date2020-01-01
JournalJournal of the Korean Magnetic Resonance Society
AuthorsJung‐Hyun Lee
AnalysisFull AI Review Included

The research details the development and application of high-spectral-resolution nanoscale Nuclear Magnetic Resonance (NMR) using Nitrogen-Vacancy (NV) centers in diamond.

  • Problem Solved: Overcame the primary limitation of NV-NMR—poor spectral resolution—caused by the short NV sensor spin lifetime (T1 ~ 3ms), which is orders of magnitude shorter than typical nuclear spin coherence times.
  • Core Innovation (SR): The Synchronized Readout (SR) protocol was implemented. This technique actively detects the external AC signal, decoupling the NMR signal linewidth from the NV spin lifetime.
  • Resolution Achievement: SR-NMR demonstrated spectral linewidths approaching 1 Hz for real liquid samples (water spin echo FWHM: 2.8 ± 0.3 Hz), sufficient for resolving molecular signatures like J-couplings and chemical shifts.
  • SNR Maximization: Combining SR with Overhauser Dynamic Nuclear Polarization (DNP) resulted in a significant Signal-to-Noise Ratio (SNR) enhancement, achieving approximately x230 increase in signal magnitude.
  • Sensitivity and Scale: The ensemble NV sensor achieved a magnetic field sensitivity of 30 pT Hz-1/2, enabling femtomole sensitivity within a picoliter detection volume.
  • Versatility: The NV center system is a robust, solid-state spin sensor that operates under ambient conditions and is optically initialized (532 nm) and controlled via microwave signals.
ParameterValueUnitContext
NV Spin SystemSpin 1N/AElectronic ground state (3A2) and excited state (3E).
Optical Initialization Wavelength532nmGreen laser used for spin polarization.
Fluorescence Emission Band600 to 800nmReadout signal band.
NV Sensor Spin Lifetime (T1)~3msTraditional limit on interrogation duration.
Zero-Field Splitting (ZFS)~2.87GHzCenter frequency for Optically Detected Magnetic Resonance (ODMR).
Ensemble NV Concentration≈ 3x1017cm-3Concentration within the 13 ”m NV-doped layer.
Ensemble Magnetic Field Sensitivity30pT Hz-1/2Measured performance using a 20 ”m diameter optical beam.
Spectral Resolution (Artificial AC Field)0.4mHzAchieved using SR with T = 3000s averaging time.
Spectral Resolution (Water Spin Echo)2.8 ± 0.3HzAchieved using Coherently Averaged SR (CASR) on a real sample.
SNR Improvement (DNP)x230N/AIncrease achieved by combining DNP with CASR.
Maximum Coherent Averaging TimeUp to 103sDuration possible using the CASR protocol.

The high-resolution nanoscale NMR was achieved through a combination of advanced quantum control and signal processing techniques:

  1. Shallow NV Creation: NV sensor spins were created close to the diamond surface (few nm deep) using few keV nitrogen ion implantation energy to maximize the coupling to the external nuclear spin sample volume.
  2. AC Magnetometry Pulse Sequences: Conventional dynamical decoupling sequences, primarily CPMG (Carr-Purcell-Meiboom-Gill) or XY pulse sequences, were used to provide an AC signal filter, allowing the NV spin to accumulate phase only at the specific oscillating NMR signal frequency.
  3. Synchronized Readout (SR) Protocol: This technique involves periodic, synchronized readout of the NV sensor’s magnetometry response, mixing the external AC magnetic signal (Larmor oscillation) with the sensor’s spectral response.
    • The effective frequency measured is Δf = |fac - fo|, where fac is the NMR frequency and fo is the center frequency of the magnetometry response.
    • This active detection method ensures the NMR signal linewidth is independent of the short NV spin lifetime.
  4. Coherently Averaged Synchronized Readout (CASR): Used for real NMR samples where the initial phase of the oscillating field is locked to the SR sequence, allowing for coherent signal accumulation over extended periods (up to 1000s).
  5. Dynamic Nuclear Polarization (DNP): Overhauser DNP was employed to hyperpolarize the nuclear spins prior to CASR detection. This involved continuous pumping of polarization from the electronic spin to the nuclear spin (~300ms duration) to overcome the low SNR inherent to thermal polarization.

The demonstrated capabilities of high-resolution, high-sensitivity NV-NMR open doors for applications in fields requiring analysis of extremely small or dilute samples.

  • Pharmaceutical and Drug Discovery: High-resolution spectroscopy for identifying molecular NMR signatures (chemical shifts and J-couplings) in dilute solutions, enabling analysis with femtomole sensitivity.
  • Catalysis Research: Monitoring chemical reactions and structural changes in catalytic processes using picoliter detection volumes.
  • Single-Cell Biology: Performing NMR studies on single cells or small biological samples where volume constraints are critical.
  • Quantum Sensing and Metrology: Utilizing the NV center as a leading platform for highly sensitive, atomic-scale magnetic field sensing under ambient conditions.
  • Materials Science: Characterization of spin defects and nuclear environments in solid-state materials for quantum information science and device development.