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Imaging the Néel Vector in Few-Layer CrPS4 with Second-Harmonic Generation.

Yi Wei Ho1,2, Mingjun Chen3, Cheng Quan Wong1

  • 1Department of Physics, National University of Singapore, 2 Science Drive 3, 117551, Singapore.

Nano Letters
|March 26, 2025
PubMed
Summary
This summary is machine-generated.

Second-harmonic generation (SHG) reveals magnetic order in chromium thiophosphate (CrPS4) by probing both crystallographic and time-reversal symmetry breaking. SHG microscopy shows AFM order is influenced by neighboring ferromagnetic layers.

Keywords:
Néel vectorantiferromagnetchromium thiophosphatesecond-harmonic generation

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Area of Science:

  • Condensed Matter Physics
  • Materials Science
  • Magnetism

Background:

  • Second-harmonic generation (SHG) is a nonlinear optical technique sensitive to crystal symmetry.
  • SHG can probe time-reversal symmetry, enabling studies of magnetic order in materials.
  • Layered antiferromagnetic (AFM) materials are of interest for spintronic applications.

Purpose of the Study:

  • To investigate the magnetic properties of chromium thiophosphate (CrPS4) using SHG.
  • To understand the interplay between crystallographic and magnetic symmetry breaking in CrPS4.
  • To explore the potential of SHG for probing AFM order and Néel vector direction.

Main Methods:

  • Second-harmonic generation (SHG) spectroscopy on bulk CrPS4.
  • Polarization-dependent SHG measurements.
  • Polarized SHG microscopy on terraced CrPS4 crystals.

Main Results:

  • SHG intensity in CrPS4 breaks both crystallographic and magnetic symmetry below the Néel temperature.
  • A specific SHG tensor element was identified, correlating with magnetic order.
  • SHG polarization response in even-layer crystals showed history dependence, indicating sensitivity to Néel vector direction.
  • AFM order in even-layer regions was found to be dictated by the ferromagnetic order of adjacent odd-layer regions.

Conclusions:

  • SHG is a powerful tool for investigating complex magnetic orders in layered AFM materials like CrPS4.
  • The study elucidates the relationship between structural and magnetic symmetries and their manifestation in nonlinear optical signals.
  • CrPS4 exhibits unique layer-dependent magnetic ordering, influenced by ferromagnetic interactions.