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Varied Magnetic Phases in a van der Waals Easy-Plane Antiferromagnet Revealed by Nitrogen-Vacancy Center Microscopy

MetadataDetails
Publication Date2022-07-22
JournalACS Nano
AuthorsAlexander J. Healey, Sharidya Rahman, Sam C. Scholten, Islay O. Robertson, Gabriel Abrahams
InstitutionsCentre for Quantum Computation and Communication Technology, RMIT University
Citations13
AnalysisFull AI Review Included

Technical Documentation & Analysis: MPCVD Diamond for Cryogenic NV Magnetometry

Section titled “Technical Documentation & Analysis: MPCVD Diamond for Cryogenic NV Magnetometry”

This research successfully utilizes widefield Nitrogen-Vacancy (NV) center microscopy, enabled by a custom-engineered diamond substrate, to characterize the magnetic phases of few-layer van der Waals (vdW) antiferromagnet CuCrP2S6 (CCPS).

  • Core Achievement: Quantitative magnetic imaging of individual CCPS flakes down to the trilayer (3L) limit at cryogenic temperatures (5 K).
  • Magnetic Order Confirmation: Confirmed A-type antiferromagnetic order persists down to 3L, exhibiting robust, easily-switchable in-plane ferromagnetism in odd-layered stacks.
  • Key Finding: Observation of an anomalous, predominantly out-of-plane ferromagnetic phase in thicker flakes, attributed to surface anisotropies arising from sample preparation or ambient exposure.
  • Diamond Platform: The study relied on a custom type-Ib HPHT diamond substrate featuring a shallow, high-density NV sensing layer created via 100 keV $^{12}$C- ion implantation and high-temperature annealing (1100 °C).
  • Interface Engineering: The use of an Al/Al2O3 coating on the diamond surface was critical for flake adhesion, laser shielding, and minimizing thermal effects during the pulsed optically detected magnetic resonance (ODMR) protocol.
  • Implication for 6CCVD: The results underscore the necessity of ultra-high quality, precisely engineered diamond substrates for advanced cryogenic quantum sensing applications, particularly where surface effects dominate 2D material properties.

The following table summarizes the critical material and operational parameters extracted from the research paper, focusing on the NV diamond platform and experimental conditions.

ParameterValueUnitContext
Diamond Substrate TypeType-Ib HPHTN/A(100)-oriented, used for NV sensing
Native Nitrogen Density$\approx 100$ppmSubstrate characteristic
NV Layer Creation$^{12}$C- Ion ImplantationN/AFollowed by 1100 °C anneal
Implantation Energy100keVDefines NV depth profile
Implantation Fluence$10^{12}$ions/cm2High-density NV ensemble
NV Layer Thickness$\approx 100$nmEstimated thickness of sensing layer
NV Layer Standoff ($d_{so}$)250 - 300nmDistance from NV layer to CCPS flake
Minimum Spatial Resolution$\approx 500$nmLimited by optical diffraction and standoff
Metalization LayersAl (80 nm), Al2O3 (80 nm)nmLaser shield, adhesion, and grid for location
Base Measurement Temperature5KClosed-cycle cryostat operation
Applied Magnetic Field RangeUp to 1TSuperconducting vector magnet capability
CCPS Coercive Field ($H_c$)35 - 40mTTypical switching field for odd-layered flakes at 5 K
Interlayer Exchange Coupling ($J_{AFM}$)$(1.2 \pm 0.6) \times 10^{-4}$J/m2Fitted micromagnetic model parameter

The experiment employed a specialized fabrication and measurement sequence to achieve quantitative magnetic imaging of the vdW flakes:

  1. Diamond Substrate Engineering: (100)-oriented type-Ib HPHT diamond was selected. A dense, shallow NV sensing layer was created via 100 keV $^{12}$C- ion implantation ($10^{12}$ ions/cm2 fluence) followed by a high-temperature anneal (culminating at 1100 °C).
  2. Surface Functionalization: An 80 nm Al grid and an 80 nm Al2O3 layer were deposited onto the diamond surface using photolithography and Atomic Layer Deposition (ALD). The Al2O3 layer served as a protective coating and adhesion promoter, while the Al grid acted as a laser shield and location reference.
  3. 2D Material Exfoliation and Transfer: Bulk CCPS crystals were mechanically exfoliated. Thin flakes were identified and transferred onto the functionalized diamond substrate using a three-axis transfer stage, mildly heated (60-65 °C) to ensure ultraclean, contamination-free interfaces.
  4. Thickness and Quality Assessment: Flake thickness (down to monolayer) was verified using Atomic Force Microscopy (AFM) and Phase Shifting Interferometry (PSI). Raman spectroscopy confirmed crystal structure and phase transitions.
  5. Cryogenic Widefield NV Magnetometry: Measurements were performed in a closed-cycle cryostat (5 K base temperature) equipped with a superconducting vector magnet (up to 1 T).
  6. Pulsed ODMR Protocol: A pulsed optically detected magnetic resonance (ODMR) protocol was used, applying a 532 nm laser for NV initialization and readout, and microwave pulses to drive spin transitions. Magnetic images ($B_{NV}$) were obtained by fitting the resonance frequencies at each camera pixel.
  7. Vector Field Reconstruction: Fourier reconstruction techniques were applied to the measured $B_{NV}$ maps to differentiate between in-plane and out-of-plane magnetization components, crucial for identifying the anomalous ferromagnetic phase.

6CCVD is uniquely positioned to supply the advanced MPCVD diamond materials and customization services required to replicate and extend this critical research into vdW magnetism and quantum sensing.

The study highlights the need for high-quality, low-strain diamond substrates to minimize background noise and strain inhomogeneity (Fig. S7(d)).

Research Requirement6CCVD Recommended SolutionTechnical Advantage
High-Purity SubstrateOptical Grade SCD (Single Crystal Diamond)Superior crystal quality and lower intrinsic strain compared to HPHT type-Ib, optimizing NV coherence and sensitivity.
Large Area SensingOptical Grade PCD Wafers (up to 125mm)Enables high-throughput characterization of multiple vdW heterostructures on a single, large-format diamond platform.
NV Layer IntegrationCustom NV Layer FabricationPrecise control over NV density and depth (0.1 ”m to 500 ”m) via tailored ion implantation and annealing recipes, matching specific standoff requirements ($d_{so}$).

The success of the NV platform relies heavily on the integration of the NV layer with surface coatings and microwave components. 6CCVD offers comprehensive in-house services to meet these needs:

  • Precision Metalization: The paper used Al/Al2O3 coatings. 6CCVD offers Custom Metalization (Au, Pt, Pd, Ti, W, Cu) and dielectric deposition capabilities. We can engineer microwave structures (e.g., coplanar waveguides, MW loops) directly onto the diamond surface, ensuring optimal microwave delivery for ODMR protocols in cryogenic environments.
  • Surface Preparation: Achieving ultraclean, flat interfaces is crucial for vdW material transfer and minimizing surface anisotropy effects. 6CCVD guarantees Ultra-Low Roughness Polishing (Ra < 1 nm for SCD), providing the pristine surface quality necessary for robust magnetic coupling.
  • Custom Dimensions: 6CCVD supplies SCD plates and PCD wafers in Custom Dimensions (up to 125mm PCD, up to 10mm thick substrates), allowing researchers to design large-scale, integrated quantum sensing platforms.

The observed anomalous out-of-plane phase and variable coercivity highlight the sensitivity of vdW magnets to surface conditions and preparation.

6CCVD’s in-house PhD team provides expert engineering consultation to optimize diamond material selection and surface functionalization for Cryogenic Quantum Sensing and 2D Magnetism projects. We assist researchers in designing substrates that mitigate surface-induced effects, ensuring that measured magnetic properties accurately reflect the intrinsic bulk or few-layer behavior of the target material (e.g., CCPS).

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

View Original Abstract

Interest in van der Waals materials often stems from a desire to miniaturize existing technologies by exploiting their intrinsic layered structures to create near-atomically thin components that do not suffer from surface defects. One appealing property is an easily switchable yet robust magnetic order, which is only sparsely demonstrated in the case of in-plane anisotropy. In this work, we use widefield nitrogen-vacancy (NV) center magnetic imaging to measure the properties of individual flakes of CuCrP<sub>2</sub>S<sub>6</sub>, a multiferroic van der Waals magnet known to exhibit weak easy-plane anisotropy in the bulk. We chart the crossover between the in-plane ferromagnetism in thin flakes down to the trilayer and the bulk behavior dominated by a low-field spin-flop transition. Further, by exploiting the directional dependence of NV center magnetometry, we are able to observe an instance of a predominantly out-of-plane ferromagetic phase near zero field, in contrast with our expectation and previous experiments on the bulk material. We attribute this to the presence of surface anisotropies caused by the sample preparation process or exposure to the ambient environment, which is expected to have more general implications for a broader class of weakly anisotropic van der Waals magnets.