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Spin-induced linear polarization of photoluminescence in antiferromagnetic van der Waals crystals

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Abstract

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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Fig. 1: Antiferromagnetic spin structure and sharp emission of NiPS3.
Fig. 2: Characterization of sharp peak X in NiPS3.
Fig. 3: Spin-induced linear polarization of PL and absorption anisotropy in NiPS3.
Fig. 4: Magnetic manipulation of PL polarization in the Voigt geometry.

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Source data are provided with this paper. All other data that support results in this article are available from the corresponding authors on reasonable request.

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Acknowledgements

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).

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Authors and Affiliations

  1. Department of Chemistry, Boston University, Boston, MA, USA

    Xingzhi Wang, Jun Cao, Hikari Kitadai, Qishuo Tan, Sahar Sharifzadeh & Xi Ling

  2. National High Magnetic Field Laboratory, Tallahassee, FL, USA

    Zhengguang Lu & Dmitry Smirnov

  3. Department of Physics, Florida State University, Tallahassee, FL, USA

    Zhengguang Lu

  4. Division of Materials Science and Engineering, Boston University, Boston, MA, USA

    Arielle Cohen, Tianshu Li, Sahar Sharifzadeh & Xi Ling

  5. Department of Physics and Astronomy, University of California, Riverside, CA, USA

    Matthew Wilson & Chun Hung Lui

  6. Department of Electrical and Computer Engineering, Boston University, Boston, MA, USA

    Sahar Sharifzadeh

  7. Department of Physics, Boston University, Boston, MA, USA

    Sahar Sharifzadeh

  8. The Photonics Center, Boston University, Boston, MA, USA

    Xi Ling

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  1. Xingzhi Wang
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Contributions

X.W. and X.L. conceived the experiment. X.W. carried out PL and absorption measurements. X.W., J.C. and Z.L. conducted the magneto-PL measurements with assistance from D.S. at the National High Magnetic Field Laboratory. J.C. and X.W. prepared samples. J.C., H.K., T.L. and Q.T. carried out the sample characterization. A.C. and S.S. performed theoretical calculations. M.W. performed the time-resolved PL measurement under the supervision of C.H.L.; X.W. and X.L. performed the analysis and interpretation of the data. All authors assisted in the interpretation of data and contributed to the writing of the manuscript.

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Correspondence to Xingzhi Wang or Xi Ling.

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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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