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Cavity-enhanced linear dichroism in a van der Waals antiferromagnet


Optical birefringence is a fundamental optical property of crystals widely used for filtering and beam splitting of photons. Birefringent crystals concurrently possess the property of linear dichroism (LD), which allows asymmetric propagation or attenuation of light with two different polarizations. This property of LD has been widely studied from small molecules to polymers and crystals but has rarely been engineered on demand. Here we use the newly discovered spin-charge coupling in the van der Waals antiferromagnetic insulator FePS3 to induce large in-plane optical anisotropy and consequently LD. We report that the LD in this antiferromagnetic insulator is tunable both spectrally and in terms of its magnitude as a function of the cavity coupling. We demonstrate near-unity LD in the visible–near-infrared range in cavity-coupled FePS3 crystals and derive its dispersion as a function of the cavity length and FePS3 thickness. Our results hold wide implications for the use of cavity-tuned LD as a diagnostic probe for strongly correlated quantum materials and offer new opportunities for miniaturized, on-chip beamsplitters and tunable filters.

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Fig. 1: Optical in-plane anisotropic behaviour in AFM van der Waals FePS3.
Fig. 2: LD spectrum of FePS3.
Fig. 3: Simulation model of cavity-enhanced multilayer FePS3.
Fig. 4: Spectral tuning of LD enhancement by tuning the cavity sizes.
Fig. 5: LD mapping and potential applications for birefringence tunability.

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Data availability

All data needed to evaluate the conclusions in the paper are present in the paper and the Supplementary Information. Additional data are available from the corresponding authors upon reasonable request.

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The codes used in this study for plotting and modelling are available from the corresponding authors upon request.


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D.J. acknowledges primary support for this work by the US Army Research Office under contract number W911NF-19-1-0109. H.Z. and Z.N. were supported by the Vagelos Institute of Energy Science and Technology graduate fellowship. L.W. acknowledges partial support from the ARO under the Grants W911NF1910342, W911NF2020166 and W911NF2110131, and the University Research Foundation for the development of scanning conformal microscopes. D.J. and Z.N. also acknowledge the support of a seed grant from the National Science Foundation (NSF) supported University of Pennsylvania Materials Research Science and Engineering Center (MRSEC) (DMR-1720530). F.P. acknowledges support from Kenyon College and NSF grant DMR-2004812. J.H. acknowledges support from the Air Force Office of Scientific Research (program manager G. Pomrenke) under award number FA9550-20RYCOR059. We acknowledge assistance from J. Lynch for the spectroscopic ellipsometry measurements.

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Authors and Affiliations



Z.N. discovered the large LD around 800 nm. D.J., H.Z. and Z.N. conceived the project. H.Z. and Z.N. made the samples, performed the linearly polarized reflectance measurements and atomic force microscopy characterization. H.Z. and Z.N. performed the calculation work. Under the supervision of L.W., Z.N. performed the LD imaging/spatial mapping. C.E.S. and J.R.H. performed the magnetic-field-tunable LD measurements. F.P. and A.B performed the ellipsometry measurements. With help from Z.N. and D.J., H.Z. analysed and interpreted the optical spectroscopy and simulation data. H.Z. and D.J. wrote the paper with input from all co-authors. D.J. supervised the entire study.

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Correspondence to Liang Wu or Deep Jariwala.

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Nature Photonics thanks Han Wang, Yuanmu Yang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Figs. 1–9.

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Zhang, H., Ni, Z., Stevens, C.E. et al. Cavity-enhanced linear dichroism in a van der Waals antiferromagnet. Nat. Photon. 16, 311–317 (2022).

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