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Longitudinal spin relaxation in nitrogen-vacancy ensembles in diamond

MetadataDetails
Publication Date2015-10-29
JournalEPJ Quantum Technology
AuthorsMariusz MrĂłzek, Daniel Rudnicki, Pauli Kehayias, Andrey Jarmola, Dmitry Budker
InstitutionsJohannes Gutenberg University Mainz, Jagiellonian University
Citations84
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Technical Documentation & Analysis: Longitudinal Spin Relaxation in NV Ensembles

Section titled “Technical Documentation & Analysis: Longitudinal Spin Relaxation in NV Ensembles”

This document analyzes the research paper “Longitudinal spin relaxation in nitrogen-vacancy ensembles in diamond” (Mrózek et al., 2015) to highlight the critical material requirements and demonstrate how 6CCVD’s advanced MPCVD diamond solutions meet and exceed the needs for replicating and extending this quantum technology research.


This study provides crucial insights into the longitudinal spin relaxation ($T_1$) dynamics of Nitrogen-Vacancy (NV$^-$) ensembles, a cornerstone of diamond-based quantum sensing.

  • Core Finding: The longitudinal relaxation rate ($T_1^{-1}$) exhibits distinct resonant increases due to cross-relaxation between differently oriented NV$^-$ subensembles.
  • Mechanism: This cross-relaxation is driven by dipole-dipole interaction, enhanced when transition frequencies become degenerate.
  • Critical Conditions: Resonances were observed at zero magnetic field (zero-field relaxation resonance) and near 595 G, confirming the importance of precise magnetic field control.
  • Material Dependence: The amplitude of the zero-field relaxation resonance is strongly dependent on the NV$^-$ concentration, confirming that $T_1^{-1}$ measurements can serve as a practical diagnostic tool for estimating local NV$^-$ density.
  • Material Requirement: Replicating this work requires high-quality diamond substrates (CVD or HPHT) with precisely controlled initial nitrogen ([N]) and resulting NV$^-$ concentrations (ranging from 0.02 ppm to 40 ppm).
  • 6CCVD Value Proposition: 6CCVD specializes in MPCVD diamond with customizable purity and doping levels, enabling researchers to precisely engineer the NV$^-$ density required for advanced quantum sensing and spin probe applications.

The following hard data points were extracted from the research paper regarding material properties and experimental parameters:

ParameterValueUnitContext
Sample Dimensions2 x 2 x 0.5mm3Bulk diamond used in experiments
Synthesis MethodsHPHT, CVDN/AMaterial origin
Nitrogen Concentration [N]<1 to <200ppmRange across investigated samples
NV- Concentration [NV-]0.02 to 40ppmRange across investigated samples
Electron Beam Energy3, 14MeVUsed for vacancy creation
Radiation Dose Range1016 to 1018cm-2Used to control vacancy density
Annealing Temperature650 to 750°CPost-irradiation treatment
Measurement Temperature Range10 to 400KExperimental range
Magnetic Field Range (B)0 to 400GPrimary study range
Critical Resonance Field595GKnown cross-relaxation point
Maximum $T_1^{-1}$ Rate (77 K)Up to 104s-1Observed at zero-field resonance (Sample S5)

The experimental success relied on precise material preparation and advanced optical/microwave control:

  1. Substrate Selection: Bulk diamond samples (HPHT and CVD) were selected and cut along the (100) crystallographic surface.
  2. NV Center Creation: Vacancies were introduced via high-energy electron irradiation (3 MeV or 14 MeV).
  3. Thermal Annealing: Samples were annealed at 650 °C to 750 °C for two hours to mobilize vacancies, allowing them to bind with substitutional nitrogen (P1 centers) to form NV$^-$ centers.
  4. Concentration Diagnostics: NV$^-$ concentration was estimated using standard fluorescence and absorption techniques.
  5. Spin Polarization & Readout: A confocal microscopy setup was used, employing a 532 nm green laser for optical initialization and readout of the NV$^-$ ground state spin polarization.
  6. $T_1$ Measurement Sequence: Longitudinal relaxation time ($T_1$) was measured using a common-mode rejection pulse sequence: Optical polarization (1 ms) $\rightarrow$ Resonant MW $\pi$-pulse $\rightarrow$ Variable delay ($\tau$) $\rightarrow$ Optical readout.
  7. Field Control: Magnetic fields were precisely controlled (0 to 400 G) using Helmholtz coils or permanent magnets to study the dependence of $T_1^{-1}$ on both field strength and orientation relative to the diamond’s crystallographic axes ([111], [110], [100]).

The research demonstrates that the performance of NV$^-$ ensembles is fundamentally limited by material quality, specifically the ability to control nitrogen incorporation and subsequent NV$^-$ density. 6CCVD provides the necessary high-purity, customizable MPCVD diamond required to advance this research.

Research Requirement6CCVD Material SolutionTechnical Advantage
Controlled [N] and [NV-]Optical Grade SCD (Single Crystal Diamond)Ultra-low intrinsic nitrogen (< 1 ppb) allows for precise, intentional nitrogen doping during growth, enabling fine control over the resulting NV$^-$ concentration (0.02 ppm to 40 ppm range) post-irradiation.
High-Density NV EnsemblesHigh-Purity PCD (Polycrystalline Diamond)Available in large areas (up to 125mm wafers) and thicknesses up to 500 ”m, ideal for high-volume sensing applications where high NV density is required for signal strength.
Spin Probe ApplicationsBDD (Boron-Doped Diamond)While not the focus of this paper, BDD substrates are available for integrating NV centers with conductive layers, crucial for electrochemical or advanced magnetic sensing devices.

6CCVD’s in-house capabilities directly address the needs for advanced NV research and device integration:

  • Custom Dimensions and Thickness: The paper used 2 x 2 x 0.5 mm3 samples. 6CCVD offers custom laser cutting to produce plates and wafers in any required geometry. We supply SCD up to 500 ”m thick and PCD up to 500 ”m thick, with substrates available up to 10 mm.
  • Surface Quality: High-fidelity optical readout (as used in ODMR) requires exceptional surface quality. We provide SCD polishing to Ra < 1nm and inch-size PCD polishing to Ra < 5nm, minimizing scattering and maximizing signal-to-noise ratio.
  • Integrated Microwave Structures: The experiment utilized copper wires and striplines for MW delivery. 6CCVD offers custom metalization services (Au, Pt, Pd, Ti, W, Cu) directly onto the diamond surface, allowing researchers to integrate high-quality microwave transmission lines (e.g., coplanar waveguides) for enhanced spin manipulation fidelity.

6CCVD’s in-house PhD team possesses deep expertise in diamond growth kinetics and defect engineering. We can assist researchers in optimizing material selection and growth parameters to achieve the specific [N] and [NV$^-$] concentrations necessary to study cross-relaxation effects for NV-based quantum sensing projects.

For custom specifications or material consultation, visit 6ccvd.com or contact our engineering team directly.

View Original Abstract

We present an experimental study of the longitudinal electron-spin relaxation of ensembles of negatively charged nitrogen-vacancy (NV−) centers in diamond. The measurements were performed with samples having different NV− concentrations and at different temperatures and magnetic fields. We found that the relaxation rate $T_{1}^{-1}$ increases when transition frequencies in NV− centers with different orientations become degenerate and interpret this as cross-relaxation caused by dipole-dipole interaction.