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Spin-correlated exciton–polaritons in a van der Waals magnet

Nature Nanotechnology volume 17, pages 1060–1064 (2022)Cite this article

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Abstract

Strong coupling between light and elementary excitations is emerging as a powerful tool to engineer the properties of solid-state systems. Spin-correlated excitations that couple strongly to optical cavities promise control over collective quantum phenomena such as magnetic phase transitions, but their suitable electronic resonances are yet to be found. Here, we report strong light–matter coupling in NiPS3, a van der Waals antiferromagnet with highly correlated electronic degrees of freedom. A previously unobserved class of polaritonic quasiparticles emerges from the strong coupling between its spin-correlated excitons and the photons inside a microcavity. Detailed spectroscopic analysis in conjunction with a microscopic theory provides unique insights into the origin and interactions of these exotic magnetically coupled excitations. Our work introduces van der Waals magnets to the field of strong light–matter physics and provides a path towards the design and control of correlated electron systems via cavity quantum electrodynamics.

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Fig. 1: Excitons in the vdW antiferromagnet NiPS3.
Fig. 2: Strong light–matter coupling in NiPS3 microcavities.
Fig. 3: Pronounced bottleneck of polariton relaxation.
Fig. 4: Polariton nonlinearities under increasing density.

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Data availability

The main data sets generated and/or analysed during the current study are available at . All supplementary data will be provided by the corresponding authors upon reasonable request.

Change history

  • 15 September 2022

    In the version of this article initially published, the email address for Florian Dirnberger was missing the first letter "f"; the email has been amended in the html and PDF versions of the article.

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Acknowledgements

We thank A. J. Millis, A. Punnoose, and X. Xu for useful discussions. Work at CUNY was supported through the NSF QII TAQS 1936276 (V.M.M., R.B.), the NSF CREST IDEALS center (V.M.M.), NSF DMR-2011738 (B.D.), and Army Research Office MURI grant W911NF-17-1-0312 (V.M.M. and A.H.M.). E.B. acknowledges support from the Robert A. Welch Foundation (grant F-2092-20220331). A.K. acknowledges support from a Graduate School Continuing Fellowship at the University of Texas at Austin. F.D. was funded by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) through Projektnummer 451072703.

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Author notes

  1. These authors contributed equally: Florian Dirnberger, Rezlind Bushati.

Authors and Affiliations

  1. Department of Physics, City College of New York, New York, NY, USA

    Florian Dirnberger, Rezlind Bushati, Biswajit Datta & Vinod M. Menon

  2. Department of Physics, The Graduate Center, City University of New York, New York, NY, USA

    Rezlind Bushati & Vinod M. Menon

  3. Department of Physics, University of Texas at Austin, Austin, TX, USA

    Ajesh Kumar, Allan H. MacDonald & Edoardo Baldini

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  1. Florian Dirnberger
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Contributions

V.M.M., E.B., F.D. and R.B. conceived the experimental idea and interpreted the results together with A.H.M. and A.K. F.D. and R.B. performed the experiments and conducted the data analysis with assistance from B.D. F.D. wrote the manuscript with input from all authors and V.M.M. supervised the project.

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Correspondence to Florian Dirnberger, Edoardo Baldini or Vinod M. Menon.

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Nature Nanotechnology thanks Alexey Kavokin and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Theoretical discussion and Supplementary Figs. 1–14.

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Dirnberger, F., Bushati, R., Datta, B. et al. Spin-correlated exciton–polaritons in a van der Waals magnet. Nat. Nanotechnol. 17, 1060–1064 (2022). https://doi.org/10.1038/s41565-022-01204-2

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