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Relaxometry and Dephasing Imaging of Superparamagnetic Magnetite Nanoparticles Using a Single Qubit

MetadataDetails
Publication Date2015-07-28
JournalNano Letters
AuthorsDominik Schmid-Lorch, Thomas HĂ€berle, Friedemann Reinhard, Andrea Zappe, Michael Slota
InstitutionsUniversity of Stuttgart, Max Planck Institute for Solid State Research
Citations61
AnalysisFull AI Review Included

6CCVD Technical Documentation: Nanoscale Magnetic Imaging via NV Center Relaxometry

Section titled “6CCVD Technical Documentation: Nanoscale Magnetic Imaging via NV Center Relaxometry”

This paper demonstrates a novel, ambient-condition nanoscale magnetometry technique using a shallow Nitrogen-Vacancy (NV) center in diamond to image the dynamic magnetic fluctuations of superparamagnetic magnetite nanoparticles. This research validates the utility of high-coherence MPCVD Single Crystal Diamond (SCD) in advancing quantum sensing for applications in materials science and nanomedicine.

  • Core Achievement: Successful application of T1 relaxometry and T2 dephasing imaging to characterize a single 10 nm magnetite nanoparticle, extracting key metrics (diameter, NV distance) at the nanoscale.
  • Material Requirement: The technique relied on high-quality bulk (100) SCD hosting shallow NV centers (approximately 5 nm below the surface) to ensure long intrinsic spin lifetimes.
  • Dynamic Range: Magnetic spin noise from the nanoparticle dramatically reduced the NV coherence times by factors up to 30 (T2) and two orders of magnitude (T1), confirming strong spin-noise coupling.
  • Frequency and Spatial Anisotropy: The combined T1 (sensitive to transverse magnetic noise, B⊥) and T2 (sensitive to longitudinal magnetic noise, B∥) measurements provided anisotropic information on magnetic fluctuations across different frequency ranges.
  • Ambient Conditions Advantage: Unlike cryogenic methods (SQUID), this NV-based approach operates under ambient conditions, making it an ideal, viable screening method for future biomedical agents (e.g., MRI contrast agents like ferritin).
  • 6CCVD Relevance: Replication and extension of this research necessitates high-purity, low-strain SCD substrates with precise crystallographic orientation, core capabilities of 6CCVD’s MPCVD manufacturing process.
ParameterValueUnitContext
NV Center Depth (Nominal)~5nmBelow diamond surface (100 orientation)
Applied DC Magnetic Field (B0)13mTAligned with the NV axis direction
Scan Area / Pixel Size500 x 500 / 10nm / nmSpatial imaging resolution
Intrinsic T1 Lifetime (Retracted)2713 ± 311”sSCD material limit (Intrinsic decoherence)
Intrinsic T2 Lifetime (Retracted)19 ± 1”sSCD material limit (Intrinsic decoherence)
Engaged T1 Lifetime (Minimum)31 ± 6”sMaximum T1 decoherence induced by particle
Engaged T2 Lifetime (Minimum)0.49 ± 0.05”sMaximum T2 decoherence induced by particle
Fitted Nanoparticle Diameter (r)7.06 ± 0.4nmDerived from Ornstein-Uhlenbeck fit
Fitted Vertical Distance (z)16.3 ± 4.7nmDistance between NV center and particle
Magnetite Anisotropy Constant (K)26kJ/m3Chosen for fit based on literature values
Max Second Moment (B⊥2)8.8mT2Transverse noise measured by T1
Max Second Moment (B∥2)1.8mT2Longitudinal noise measured by T2

The experiment successfully characterized the magnetic dynamics of superparamagnetic magnetite nanoparticles using pulsed optically detected magnetic resonance (ODMR) protocols on a single NV center.

  1. Substrate & Setup:

    • A commercial Atomic Force Microscope (AFM) was used, operating under ambient conditions (critical for bio-applications).
    • The base material was a bulk (100) Single Crystal Diamond plate containing shallow NV centers located approximately 5 nm from the surface.
    • A constant magnetic field of 13 mT was applied, aligned parallel to the NV center axis.
  2. Sample Preparation & Scanning:

    • Superparamagnetic magnetite nanoparticles (initial diameter 8 ± 3 nm) were diluted in sodium silicate.
    • This matrix served to firmly attach the particles to the AFM cantilever and act as a spacer.
    • The particle-loaded cantilever was scanned in contact mode over a fixed, individual NV center on the diamond surface.
  3. Spin Lifetime Measurement Protocols:

    • T1 Relaxometry (Longitudinal Relaxation):
      • The polarization is initialized and analyzed along the NV axis.
      • The T1 sequence is primarily sensitive to magnetic field fluctuations perpendicular (transverse) to the NV axis (B⊥).
      • It detects noise components at the NV center’s Larmor frequency (high frequency range).
    • T2 Dephasing (Transversal Relaxation via Spin Echo, SE):
      • The polarization is flipped into the transversal plane using a $\pi$/2 microwave pulse.
      • The SE method is mainly sensitive to low frequency magnetic field fluctuations along (longitudinal) the NV axis (B∥).
  4. Modeling and Data Extraction:

    • Magnetic field fluctuations were modeled using an Ornstein-Uhlenbeck process incorporating the NĂ©el relaxation time ($\tau$N) and anisotropy energy barrier (E = KV).
    • Decoherence rates ($\Gamma$tot) were calculated as the sum of intrinsic diamond lattice decoherence ($\Gamma$int, due to 13C) and external nanoparticle-induced decoherence ($\Gamma$ext).
    • Simulations were fitted to fluorescence contrast images (T1 and T2 maps) simultaneously to determine the particle radius (r) and the minimum vertical distance (z) to the NV center.

This quantum sensing research confirms the critical role of high-purity, highly coherent Single Crystal Diamond (SCD) as the fundamental platform. 6CCVD is an expert technical partner for synthesizing and preparing the custom SCD materials required to replicate or significantly enhance this work.

Material Requirement (Paper)6CCVD Material SolutionRelevance & Advantages
High Coherence / Low StrainOptical Grade SCD (High Purity)Guaranteed low concentrations of substitutional nitrogen (P1 centers) and other contaminants, maximizing intrinsic T1 (up to milliseconds) and T2 (up to tens of microseconds) lifetimes. Essential for high-sensitivity measurements.
Specific OrientationCustom Oriented SCD PlatesThe paper utilized (100) diamond. 6CCVD offers wafers with custom crystallographic orientation, including (111), which the paper notes would hypothetically yield better anisotropy control (Δ = 0.0).
Substrate Size & BulkSCD Substrates up to 500 ”m thickWe provide robust, large-area SCD substrates, ensuring stability and homogeneity for sophisticated scanning probe setups like the AFM used here.
Improved SNR (Future Work)SCD Templates for NanopillarsThe paper suggests improving signal-to-noise ratio (SNR) using nanopillars. 6CCVD supplies the high-purity SCD material necessary for subsequent high-resolution etching processes.

The ability to finely control material properties is paramount for replicating and advancing NV-center-based quantum sensing experiments.

  • Custom Dimensions: While this experiment used a small bulk sample, 6CCVD can supply SCD or PCD substrates in custom sizes and shapes, with polishing available up to inch-size PCD (Ra < 5 nm) and sub-nanometer roughness for SCD (Ra < 1 nm), crucial for high-precision AFM scanning.
  • Precision Thickness Control: We offer SCD material with thickness control ranging from 0.1 ”m films up to 500 ”m bulk plates, providing engineering flexibility for integrating diamond films into complex quantum devices.
  • Metalization Services: Although not explicitly used on the diamond in this paper, NV quantum sensing often requires precise microwave delivery or electrical contacts. 6CCVD provides in-house metalization (Au, Pt, Pd, Ti, W, Cu) for creating optimized microstrip lines or electrodes directly onto the SCD surface.

6CCVD’s in-house PhD team specializes in defect engineering and MPCVD growth parameters tailored for quantum applications. We can assist researchers in selecting materials specifically optimized for:

  • Shallow NV Optimization: Achieving the requisite ~5 nm depth for sensing external nanoparticles, a process highly dependent on the quality of the SCD starting material and subsequent implantation/annealing.
  • Biomedical Applications: Supporting material selection and design for novel MRI contrast agents or particle-aided tumor hyperthermia studies that require ambient-condition, nanoscale magnetic screening.
  • Relaxometry Refinement: Consulting on how different crystallographic orientations and intrinsic defect levels impact the anisotropy ($\varepsilon$) observed in T1 and T2 relaxometry images.

For custom specifications or material consultation, visit 6ccvd.com or contact our engineering team directly. We ship globally (DDU default, DDP available) to support your cutting-edge research.

View Original Abstract

To study the magnetic dynamics of superparamagnetic nanoparticles, we use scanning probe relaxometry and dephasing of the nitrogen vacancy (NV) center in diamond, characterizing the spin noise of a single 10 nm magnetite particle. Additionally, we show the anisotropy of the NV sensitivity’s dependence on the applied decoherence measurement method. By comparing the change in relaxation (T1) and dephasing (T2) time in the NV center when scanning a nanoparticle over it, we are able to extract the nanoparticle’s diameter and distance from the NV center using an Ornstein-Uhlenbeck model for the nanoparticle’s fluctuations. This scanning probe technique can be used in the future to characterize different spin label substitutes for both medical applications and basic magnetic nanoparticle behavior.