Abstract
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.
This is a preview of subscription content, access via your institution
Relevant articles
Open Access articles citing this article.
-
Computational spectropolarimetry with a tunable liquid crystal metasurface
eLight Open Access 04 November 2022
Access options
Access Nature and 54 other Nature Portfolio journals
Get Nature+, our best-value online-access subscription
$29.99 per month
cancel any time
Subscribe to this journal
Receive 12 print issues and online access
$209.00 per year
only $17.42 per issue
Rent or buy this article
Get just this article for as long as you need it
$39.95
Prices may be subject to local taxes which are calculated during checkout





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.
Code availability
The codes used in this study for plotting and modelling are available from the corresponding authors upon request.
References
Ermolaev, G. et al. Giant optical anisotropy in transition metal dichalcogenides for next-generation photonics. Nat. Commun. 12, 854 (2021).
Norden, B. Linear and circular dichroism of polymeric pseudoisocyanine. J. Phys. Chem. 81, 151–159 (1977).
Weber, M. F., Stover, C. A., Gilbert, L. R., Nevitt, T. J. & Ouderkirk, A. J. Giant birefringent optics in multilayer polymer mirrors. Science 287, 2451–2456 (2000).
Nicholls, L. H. et al. Ultrafast synthesis and switching of light polarization in nonlinear anisotropic metamaterials. Nat. Photon 11, 628–633 (2017).
Mao, N. et al. Optical anisotropy of black phosphorus in the visible regime. J. Am. Chem. Soc. 138, 300–305 (2016).
Wang, Y. Y. et al. In-plane optical anisotropy in ReS2 flakes determined by angle-resolved polarized optical contrast spectroscopy. Nanoscale 11, 20199–20205 (2019).
Kats, M. A. et al. Giant birefringence in optical antenna arrays with widely tailorable optical anisotropy. Proc. Natl Acad. Sci. USA 109, 12364–12368 (2012).
Huang, B. et al. Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit. Nature 546, 270–273 (2017).
Gong, C. et al. Discovery of intrinsic ferromagnetism in two-dimensional van der Waals crystals. Nature 546, 265–269 (2017).
Lançon, D. et al. Magnetic structure and magnon dynamics of the quasi-two-dimensional antiferromagnet FePS3. Phys. Rev. B 94, 214407 (2016).
Lançon, D., Ewings, R., Guidi, T., Formisano, F. & Wildes, A. R. Magnetic exchange parameters and anisotropy of the quasi-two-dimensional antiferromagnet NiPS3. Phys. Rev. B 98, 134414 (2018).
Lee, J.-U. et al. Ising-type magnetic ordering in atomically thin FePS3. Nano Lett. 16, 7433–7438 (2016).
Wang, X. et al. Raman spectroscopy of atomically thin two-dimensional magnetic iron phosphorus trisulfide (FePS3) crystals. 2D Mater. 3, 031009 (2016).
McCreary, A. et al. Quasi-two-dimensional magnon identification in antiferromagnetic FePS3 via magneto-Raman spectroscopy. Phys. Rev. B 101, 064416 (2020).
Kim, K. et al. Suppression of magnetic ordering in XXZ-type antiferromagnetic monolayer NiPS3. Nat. Commun. 10, 345 (2019).
Sun, Z. et al. Giant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI3. Nature 572, 497–501 (2019).
Chu, H. et al. Linear magnetoelectric phase in ultrathin MnPS3 probed by optical second harmonic generation. Phys. Rev. Lett. 124, 027601 (2020).
Ni, Z. et al. Imaging the Néel vector switching in the monolayer antiferromagnet MnPSe3 with strain-controlled Ising order. Nat. Nanotechnol. 16, 782–787 (2021).
Le Flem, G., Brec, R., Ouvard, G., Louisy, A. & Segransan, P. Magnetic interactions in the layer compounds MPX3 (M = Mn, Fe, Ni; X = S, Se). J. Phys. 43, 455–461 (1982).
Chittari, B. L. et al. Electronic and magnetic properties of single-layer MPX3 metal phosphorous trichalcogenides. Phys. Rev. B 94, 184428 (2016).
Wildes, A. R. et al. Magnetic structure of the quasi-two-dimensional antiferromagnet NiPS3. Phys. Rev. B 92, 224408 (2015).
Xie, Q.-Y. et al. Crystallographic and magnetic properties of van der Waals layered FePS3 crystal. Chin. Phys. B 28, 056102 (2019).
Joy, P. & Vasudevan, S. Magnetism in the layered transition-metal thiophosphates MPS3 (M = Mn, Fe, and Ni). Phys. Rev. B 46, 5425–5433 (1992).
Kim, S. Y. et al. Charge-spin correlation in van der Waals antiferromagnet NiPS3. Phys. Rev. Lett. 120, 136402 (2018).
Zhang, Q. et al. Observation of giant optical linear dichroism in a zigzag antiferromagnet FePS3. Nano Lett. 21, 6938–6945 (2021).
Hwangbo, K. et al. Highly anisotropic excitons and multiple phonon bound states in a van der Waals antiferromagnetic insulator. Nat. Nanotechnol. 16, 655–660 (2021).
Kats, M. A., Blanchard, R., Genevet, P., & Capasso, F. Nanometre optical coatings based on strong interference effects in highly absorbing media. Nat. Mater. 12, 20–24 (2013).
Jariwala, D., Davoyan, A. R., Tagliabue, G., Sherrott, M. C., Wong, J. & Atwater, H. A. Near-unity absorption in van der Waals semiconductors for ultrathin optoelectronics. Nano Lett. 16, 5482–5487 (2016).
Zhang, H. et al. Hybrid exciton-plasmon-polaritons in van der Waals semiconductor gratings. Nat. Commun. 11, 3552 (2020).
Zhang, X.-X. et al. Spin dynamics slowdown near the antiferromagnetic critical point in atomically thin FePS3. Nano Lett. 21, 5045–5052 (2021).
Wang, X. et al. Spin-induced linear polarization of photoluminescence in antiferromagnetic van der Waals crystals. Nat. Mater. 20, 964–970 (2021).
Little, A. et al. Three-state nematicity in the triangular lattice antiferromagnet Fe1/3NbS2. Nat. Mater. 19, 1062–1067 (2020).
Deng, Y. et al. Gate-tunable room-temperature ferromagnetism in two-dimensional Fe3GeTe2. Nature 563, 94–99 (2018).
Mandziak, A. et al. Tuning the Néel temperature in an antiferromagnet: the case of NixCo1−xO microstructures. Sci. Rep. 9, 13584 (2019).
Eid, K., Sheu, B., Maksimov, O., Stone, M., Schiffer, P. & Samarth, N. Nanoengineered Curie temperature in laterally patterned ferromagnetic semiconductor heterostructures. Appl. Phys. Lett. 86, 152505 (2005).
Li, Q. et al. Patterning-induced ferromagnetism of Fe3GeTe2 van der Waals materials beyond room temperature. Nano Lett. 18, 5974–5980 (2018).
Yang, Y. et al. In-plane optical anisotropy of low-symmetry 2D GeSe. Adv. Opt. Mater. 7, 1801311 (2019).
Zhong, M. et al. In-plane optical and electrical anisotropy of 2D black arsenic. ACS Nano 15, 1701–1709 (2021).
Acknowledgements
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.
Author information
Authors and Affiliations
Contributions
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.
Corresponding authors
Ethics declarations
Competing interests
The authors declare no competing interests.
Peer review
Peer review information
Nature Photonics thanks Han Wang, Yuanmu Yang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
Additional information
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary information
Supplementary Information
Supplementary Figs. 1–9.
Rights and permissions
About this article
Cite this article
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). https://doi.org/10.1038/s41566-022-00970-8
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1038/s41566-022-00970-8
This article is cited by
-
Computational spectropolarimetry with a tunable liquid crystal metasurface
eLight (2022)
-
Light control with atomically thin magnets
Nature Photonics (2022)