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Light-induced electronic polarization in antiferromagnetic Cr2O3

Nature Materials (2024)Cite this article

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Abstract

In a solid, the electronic subsystem can exhibit incipient order with lower point group symmetry than the crystal lattice. Ultrafast external fields that couple exclusively to electronic order parameters have rarely been investigated, however, despite their potential importance in inducing exotic effects. Here we show that when inversion symmetry is broken by the antiferromagnetic order in Cr2O3, transmitting a linearly polarized light pulse through the crystal gives rise to an in-plane rotational symmetry-breaking (from C3 to C1) via optical rectification. Using interferometric time-resolved second harmonic generation, we show that the ultrafast timescale of the symmetry reduction is indicative of a purely electronic response; the underlying spin and crystal structures remain unaffected. The symmetry-broken state exhibits a dipole moment, and its polar axis can be controlled with the incident light. Our results establish a coherent nonlinear optical protocol by which to break electronic symmetries and produce unconventional electronic effects in solids.

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Fig. 1: Equilibrium SHG of Cr2O3.
Fig. 2: Symmetry reduction in the two AFM domain states.
Fig. 3: Manipulation of light-induced electronic polarization.
Fig. 4: Floquet theory of the light-induced electronic polarization.

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Data availability

The data that support the findings of this study are present in the paper and/or in the Supplementary Information and are deposited in the Zenodo repository at https://doi.org/10.5281/zenodo.10674665 (ref. 41). Additional data related to the paper are available from the corresponding author upon request.

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Acknowledgements

We thank M. Ye, D. Kaplan, H. Ning, C. Belvin and W. Campbell for helpful conversations related to this work. Research at the University of California Los Angeles (UCLA) was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under award no. DE-SC0023017 (A.K.). The work at Rutgers was supported by the W. M. Keck Foundation (S.-W.C.). A.B.C. and R.R. acknowledge financial support from the University of California Laboratory Fees Research Program funded by the University of California Office of the President (grant number LFR-20-653926). A.B.C. acknowledges financial support from the Joseph P. Rudnick Prize Postdoctoral Fellowship (UCLA).

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Authors and Affiliations

  1. Department of Physics and Astronomy, University of California Los Angeles, Los Angeles, CA, USA

    Xinshu Zhang, Tyler Carbin, Adrian B. Culver, Rahul Roy & Anshul Kogar

  2. Mani L. Bhaumik Institute for Theoretical Physics, Department of Physics and Astronomy, University of California Los Angeles, Los Angeles, CA, USA

    Adrian B. Culver & Rahul Roy

  3. Rutgers Center for Emergent Materials, Rutgers University, Piscataway, NJ, USA

    Kai Du, Kefeng Wang & Sang-Wook Cheong

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Contributions

X.Z. and T.C. built the SHG set-up and performed the time-resolved SHG experiments under the supervision of A.K.; X.Z. analysed the data under the supervision of A.K.; K.D. and K.W. grew the single crystals under the supervision of S.-W.C. Theoretical calculations were carried out by A.B.C. with input from R.R., X.Z. and A.K. The paper was written by X.Z., A.B.C. and A.K. with input from all authors.

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Correspondence to Anshul Kogar.

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Nature Materials thanks Manfred Fiebig and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Figs. 1–7 and discussion.

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Zhang, X., Carbin, T., Culver, A.B. et al. Light-induced electronic polarization in antiferromagnetic Cr2O3. Nat. Mater. (2024). https://doi.org/10.1038/s41563-024-01852-w

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