Antiferromagnets are promising components for spintronics due to their terahertz resonance, multilevel states and absence of stray fields. However, the zero net magnetic moment of antiferromagnets makes the detection of the antiferromagnetic order and the investigation of fundamental spin properties notoriously difficult. Here, we report an optical detection of Néel vector orientation through an ultra-sharp photoluminescence in the van der Waals antiferromagnet NiPS3 from bulk to atomically thin flakes. The strong correlation between spin flipping and electric dipole oscillator results in a linear polarization of the sharp emission, which aligns perpendicular to the spin orientation in the crystal. By applying an in-plane magnetic field, we achieve manipulation of the photoluminescence polarization. This correlation between emitted photons and spins in layered magnets provides routes for investigating magneto-optics in two-dimensional materials, and hence opens a path for developing opto-spintronic devices and antiferromagnet-based quantum information technologies.
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This material is based upon work supported by the National Science Foundation under grant no. 1945364. X.W. and X.L. acknowledge the financial support from Boston University and the Photonics Center at Boston University. The transmission electron microscopy imaging was performed at the Center for Nanoscale Systems, a member of the National Nanotechnology Coordinated Infrastructure Network, which is supported by the National Science Foundation under award no. 1541959. The Center for Nanoscale Systems is part of Harvard University. A.C. and S.S. acknowledge financial support from the US Department of Energy, Office of Science, Basic Energy Sciences Early Career Program under award no. DE-SC0018080. We acknowledge the computational resources through the Extreme Science and Engineering Discovery Environment, which is supported by National Science Foundation grant no. ACI-1548562; and the National Energy Research Scientific Computing Center, a US Department of Energy Office of Science User Facility supported by the Office of Science of the US Department of Energy under contract no. DE-AC02-05CH11231. Z.L. and D.S. acknowledge support from the US Department of Energy (no. DE-FG02-07ER46451) for high-field magnetospectroscopy measurements performed at National High Magnetic Field Laboratory, which is supported by the National Science Foundation through NSF/DMR-1644779 and the state of Florida. C.H.L. acknowledges support from the American Chemical Society Petroleum Research Fund (ACS PRF No. 61640-ND6).
The authors declare no competing interests.
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Wang, X., Cao, J., Lu, Z. et al. Spin-induced linear polarization of photoluminescence in antiferromagnetic van der Waals crystals. Nat. Mater. 20, 964–970 (2021). https://doi.org/10.1038/s41563-021-00968-7
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