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Room-temperature spin-layer locking of exciton–polariton nonlinearities in a WS2 microcavity

Abstract

Spintronics, whereby electron spin is harnessed for carrying and processing information, could play an important role in the future of information technology. However, despite ongoing research efforts, establishing a materials platform that suits spin-optronics, particularly one that operates effectively at ambient temperatures, continues to represent a challenge. Recent advancements in transition metal dichalcogenides are opening up new opportunities, with exciton-polaritons in these materials being promising for the development of spintronic customizable devices that function at ambient temperatures. Although transition metal dichalcogenide polaritons have shown promising potential, spin-anisotropic nonlinearities have been missing. Here we demonstrate the absence of spin-anisotropic interaction in a monolayer WS2 microcavity at room temperature and show how spin anisotropy can be recovered by engineering double WS2 layer structures with varied interlayer spacing. We attribute this phenomenon to a distinctive feature in exciton–polariton physics: layer-dependent polariton–phonon coupling. We use theoretical calculations of the phonon electrostatic potentials finding a drastically different coupling strength for single and double monolayer samples and discuss qualitatively how this explains the observed spin-anisotropic response. This is further consistent with experiments on multi-WS2 layer samples and the identification of a critical separation distance, above which an effective single monolayer spin-anisotropic response is recovered, both in experiment and theory. Our work lays the groundwork for the development of spin-optronic polaritonic devices at room temperature.

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Fig. 1: Optical characterization of TMD microcavities.
Fig. 2: Nonlinearities in ML TMD microcavity.
Fig. 3: The spin-dependent nonlinearities in double-layer WS2 microcavities.
Fig. 4: Circular/linear slope ratio and theoretical model.
Fig. 5: The spin-dependent nonlinearities in the multilayer WS2 sample.

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Data availability

All data needed to evaluate the conclusions in the paper are present in the paper and/or the Supplementary Materials. Data for Figs. 15 are available via figshare at https://figshare.com/s/8511d64f440908718652 (ref. 53). Additional data related to this paper may be requested from the authors.

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Acknowledgements

J.Z., A.F., K.D. and T.C.H.L. gratefully acknowledge funding support from the Singapore Ministry of Education (MOE) Academic Research Fund Tier 3 grant (MOE-MOET32023-0003) ‘Quantum Geometric Advantage’ and Tier 2 grant (MOE-T2EP50121-0020). Q.S., J.Z.-P., W.G. and T.C.H.L. gratefully acknowledge funding support from the National Research Foundation project N-GAP (NRF2023-ITC004-001). Q.X. gratefully acknowledges strong funding support from the National Key Research and Development Program of China (grant number 2022YFA1204700) and the National Natural Science Foundation of China (numbers 122507101126 and 12020101003), and support from the State Key Laboratory of Low-Dimensional Quantum Physics of Tsinghua University and the Tsinghua University Initiative Scientific Research Program. D.S., A.F. and V.A. gratefully acknowledge ‘Quantum Optical Networks based on Exciton-polaritons’ (Q-ONE, N. 101115575, HORIZON-EIC-2022-PATHFINDER CHALLENGES EU project), ‘National Quantum Science and Technology Institute’ (NQSTI, N. PE0000023, PNRR MUR project) and ‘Integrated Infrastructure Initiative in Photonic and Quantum Sciences’ (I-PHOQS, N. IR0000016, PNRR MUR project). W.G. gratefully acknowledges funding support from ASTAR (M24M8b0004), Singapore National Research Foundation (NRF-CRP22-2019-0004, NRF-CRP30-2023-0003, NRF-CRP31-0001, NRF2023-ITC004-001 and NRF-MSG-2023-0002) and Singapore Ministry of Education Tier 2 grant (MOE-T2EP50222-0018). R.S. gratefully acknowledges funding support from the Singapore Ministry of Education via the AcRF Tier 2 grant (MOE-T2EP50222-0008) and Nanyang Technological University via a Nanyang Assistant Professorship start-up grant. R.B. gratefully acknowledges the R&D project of Joint Funds of Liaoning Province (2023JH2/101800038). J.Z. gratefully acknowledges the Presidential Postdoctoral Fellowship support from the Nanyang Technological University.

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J.Z., A.F., D.S., Q.X. and T.C.H.L. conceived the ideas and designed the experiments. J.Z. prepared the multilayered microcavity samples. J.Z., A.F., Q.S., Y.L. and R.S. carried out the optical spectroscopy measurements. J.Z. and A.F. analysed the data. K.D., R.B., K.S., Y.Z. and T.C.H.L. performed the theoretical calculations. J.Z., A.F., K.D., J.Z.-P., W.G., V.A., D.S., Q.X. and T.C.H.L. wrote the paper with contributions from all authors. All authors discussed the results and commented on the paper.

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Correspondence to Antonio Fieramosca, Qihua Xiong or Timothy C. H. Liew.

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Zhao, J., Fieramosca, A., Dini, K. et al. Room-temperature spin-layer locking of exciton–polariton nonlinearities in a WS2 microcavity. Nat. Photon. 19, 1353–1360 (2025). https://doi.org/10.1038/s41566-025-01786-y

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