Collective photon emission and ferroelectric exciton ordering near Mott insulating state in WSe<sub>2</sub>/WS<sub>2</sub> heterobilayers

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Nature Materials (2026)Cite this article Spontaneous symmetry breaking, driven by competing interactions and quantum fluctuations, is fundamental to understanding ordered electronic phases. Although electrically neutral, optical excitations like excitons can interact through their dipole moment, raising the possibility of optically active ordered phases. The effects of spontaneous ordering on optical properties remains underexplored. The excitonic Mott insulating state recently observed in semiconducting moiré crystals may help clarify this question. Here we present evidence for an in-plane ferroelectric phase of dipolar moiré excitons driven by strong exciton–exciton interactions. We reveal a speed-up of photon emission at late times and low densities in excitonic decay. This counterintuitive behaviour is attributed to collective radiance, linked to the transition between disordered and symmetry-broken ferroelectric phases of moiré excitons. Our findings provide evidence for strong dipolar intersite interactions in moiré lattices, demonstrate collective photon emission as a probe for moiré quantum materials and a path for exploring cooperative optical phenomena in strongly correlated systems.This is a preview of subscription content, access via your institution Access Nature and 54 other Nature Portfolio journals Get Nature+, our best-value online-access subscription $32.99 / 30 days cancel any timeSubscribe to this journal Receive 12 print issues and online access $259.00 per yearonly $21.58 per issueBuy this articleUSD 39.95Prices may be subject to local taxes which are calculated during checkoutAll the data that support the findings of this study are reported in the Article and its Supplementary Information. Source data are provided with this paper.Cai, J. et al. Signatures of fractional quantum anomalous Hall states in twisted MoTe2. Nature 622, 63–68 (2023).Article CAS PubMed Google Scholar Park, H. et al. Observation of fractionally quantized anomalous Hall effect. Nature 622, 74–79 (2023).Article CAS PubMed Google Scholar Zeng, Y. et al. Thermodynamic evidence of fractional Chern insulator in moiré MoTe2. Nature 622, 69–73 (2023).Article CAS PubMed Google Scholar Xu, Y. et al. Correlated insulating states at fractional fillings of moiré superlattices. Nature 587, 214–218 (2020).Article CAS PubMed Google Scholar Regan, E. C. et al. Mott and generalized Wigner crystal states in WSe2/WS2 moiré superlattices. Nature 579, 359–363 (2020).Article CAS PubMed Google Scholar Tang, Y. et al. Simulation of Hubbard model physics in WSe2/WS2 moiré superlattices. Nature 579, 353–358 (2020).Article CAS PubMed Google Scholar Shimazaki, Y. et al. Strongly correlated electrons and hybrid excitons in a moiré heterostructure. Nature 580, 472–477 (2020).Article CAS PubMed Google Scholar Smoleński, T. et al. Signatures of Wigner crystal of electrons in a monolayer semiconductor. Nature 595, 53–57 (2021).Article PubMed Google Scholar Zhou, Y. et al. Bilayer Wigner crystals in a transition metal dichalcogenide heterostructure. Nature 595, 48–52 (2021).Article CAS PubMed Google Scholar Jin, C. et al. Observation of moiré excitons in WSe2/WS2 heterostructure superlattices. Nature 567, 76–80 (2019).Article CAS PubMed Google Scholar Tran, K. et al. Evidence for moiré excitons in van der Waals heterostructures. Nature 567, 71–75 (2019).Article CAS PubMed PubMed Central Google Scholar Karni, O. et al. Structure of the moiré exciton captured by imaging its electron and hole. Nature 603, 247–252 (2022).Article CAS PubMed Google Scholar Lagoin, C., Suffit, S., Baldwin, K., Pfeiffer, L. & Dubin, F. Mott insulator of strongly interacting two-dimensional semiconductor excitons. Nat. Phys. 18, 149–153 (2022).Article CAS Google Scholar Xiong, R. et al. Correlated insulator of excitons in WSe2/WS2 moiré superlattices. Science 380, 860–864 (2023).Article CAS PubMed Google Scholar Park, H. et al. Dipole ladders with large Hubbard interaction in a moiré exciton lattice. Nat. Phys. 19, 1286–1292 (2023).Article CAS Google Scholar Wang, X. et al. Intercell moiré exciton complexes in electron lattices. Nat. Mater. 22, 599–604 (2023).Article CAS PubMed Google Scholar Gao, B. et al. Excitonic Mott insulator in a Bose-Fermi-Hubbard system of moiré WS2/WSe2 heterobilayer. Nat. Commun. 15, 2305 (2024).Article CAS PubMed PubMed Central Google Scholar Lian, Z. et al. Valley-polarized excitonic mott insulator in WS2/WSe2 moiré superlattice. Nat. Phys. 20, 34–39 (2024).Article CAS Google Scholar Rivera, P. et al. Valley-polarized exciton dynamics in a 2D semiconductor heterostructure. Science 351, 688–691 (2016).Article CAS PubMed Google Scholar Li, W., Lu, X., Dubey, S., Devenica, L. & Srivastava, A. Dipolar interactions between localized interlayer excitons in van der Waals heterostructures. Nat. Mater. 19, 624–629 (2020).Article CAS PubMed Google Scholar Kremser, M. et al. Discrete interactions between a few interlayer excitons trapped at a MoSe2-WSe2 heterointerface. npj 2DMater. Appl. 4, 39 (2020).
Google Scholar Lagoin, C. et al. Extended Bose–Hubbard model with dipolar excitons. Nature 609, 485–489 (2022).Article CAS PubMed Google Scholar Lagoin, C., Baldwin, K., Pfeiffer, L. & Dubin, F. Superlattice quantum solid of dipolar excitons. Phys. Rev. Lett. 132, 176001 (2024).Article CAS PubMed Google Scholar Kumlin, J., Srivastava, A. & Pohl, T. Superradiance of strongly interacting dipolar excitons in moiré quantum materials (2024). Phys. Rev. Lett. 134, 126901 (2025).Article CAS PubMed Google Scholar Huang, T.-S. et al. Collective optical properties of moiré‚ excitons. Phys. Rev. Lett. 134, 176901 (2025).Article CAS PubMed Google Scholar Lagoin, C., Morin, C., Baldwin, K., Pfeiffer, L. & Dubin, F. Evidence for a lattice supersolid of subradiant dipolar excitons. Preprint at http://arxiv.org/abs/2410.17162 (2024).Li, H. et al. Imaging two-dimensional generalized Wigner crystals. Nature 597, 650–654 (2021).Article CAS PubMed Google Scholar Montblanch, A. R.-P. et al. Confinement of long-lived interlayer excitons in WS2/WSe2 heterostructures. Commun. Phys. 4, 119 (2021).Article CAS Google Scholar Miller, B. et al. Long-lived direct and indirect interlayer excitons in van der Waals heterostructures. Nano Lett. 17, 5229–5237 (2017).Article CAS PubMed Google Scholar Jauregui, L. A. et al. Electrical control of interlayer exciton dynamics in atomically thin heterostructures. Science 366, 870–875 (2019).Article CAS PubMed Google Scholar Choi, J. et al. Twist angle-dependent interlayer exciton lifetimes in van der Waals heterostructures. Phys. Rev. Lett. 126, 047401 (2021).Article CAS PubMed Google Scholar Moody, G., Schaibley, J. & Xu, X. Exciton dynamics in monolayer transition metal dichalcogenides. J. Opt. Soc. Am. B 33, C39–C49 (2016).Article PubMed PubMed Central Google Scholar Zhang, X.-X., You, Y., Zhao, S. Y. F. & Heinz, T. F. Experimental evidence for dark excitons in monolayer WSe2. Phys. Rev. Lett. 115, 257403 (2015).Article PubMed Google Scholar Wu, F., Lovorn, T., Tutuc, E. & MacDonald, A. H. Hubbard model physics in transition metal dichalcogenide moiré bands. Phys. Rev. Lett. 121, 026402 (2018).Article CAS PubMed Google Scholar Shabani, S. et al. Deep moiré potentials in twisted transition metal dichalcogenide bilayers. Nat. Phys. 17, 720–725 (2021).Article CAS Google Scholar Wilson, N. R. et al. Determination of band offsets, hybridization, and exciton binding in 2D semiconductor heterostructures. Sci. Adv. 3, e1601832 (2017).Article PubMed PubMed Central Google Scholar Zhang, D., Schoenherr, P., Sharma, P. & Seidel, J. Ferroelectric order in van der Waals layered materials. Nat. Rev. Mater. 8, 25–40 (2023).Article Google Scholar de Paz, A. et al. Nonequilibrium quantum magnetism in a dipolar lattice gas. Phys. Rev. Lett. 111, 185305 (2013).Article PubMed Google Scholar Zhang, C., Safavi-Naini, A., Rey, A. M. & Capogrosso-Sansone, B. Equilibrium phases of tilted dipolar lattice bosons. New J. Phys. 17, 123014 (2015).Article Google Scholar Huber, J., Kirton, P. & Rabl, P. Nonequilibrium magnetic phases in spin lattices with gain and loss. Phys. Rev. A 102, 012219 (2020).Article CAS Google Scholar Su, L. et al. Dipolar quantum solids emerging in a Hubbard quantum simulator. Nature 622, 724–729 (2023).Article CAS PubMed Google Scholar Rui, J. et al. A subradiant optical mirror formed by a single structured atomic layer. Nature 583, 369–374 (2020).Article CAS PubMed Google Scholar Wu, F. Y. The Potts model. Rev. Mod. Phys. 54, 235–268 (1982).Article Google Scholar Park, H. Three-state Potts model on a triangular lattice. Phys. Rev. B 49, 12881–12887 (1994).Article CAS Google Scholar de Vega, I., Cirac, J. I. & Porras, D. Detection of spin correlations in optical lattices by light scattering. Phys. Rev. A 77, 051804 (2008).Article Google Scholar Pizzi, A., Gorlach, A., Rivera, N., Nunnenkamp, A. & Kaminer, I. Light emission from strongly driven many-body systems. Nat. Phys. 19, 551–561 (2023).Article CAS Google Scholar Zomer, P., Guimarães, M., Brant, J., Tombros, N. & Van Wees, B. Fast pick up technique for high quality heterostructures of bilayer graphene and hexagonal boron nitride. Appl. Phys. Lett. 105, 013101 (2014).Article Google Scholar Kim, K. et al. Van der Waals heterostructures with high accuracy rotational alignment. Nano Lett. 16, 1989–1995 (2016).Article CAS PubMed Google Scholar Download referencesWe thank L. Zhang, M. Hafezi, A. Imamoğlu, M. Claassen, T. Smoleński and M. Kroner for insightful discussions. A.S. acknowledges funding from the NSF Division of Materials Research (award number 1905809) and the State Secretariat for Education, Research and Innovation (SERI)-funded European Research Council Consolidator Grant TuneInt2Quantum (number 101043957). T.P. and J.K. acknowledge support from the European Union’s Horizon Europe research and innovation programme under the Marie Skłodowska-Curie grant agreement number 101106552 (QuLowD), from the Austrian Science Fund (grant number 10.55776/COE1) and the European Union (NextGenerationEU), and from the European Research Council through the ERC Synergy Grant SuperWave (grant number 101071882). Synthesis of WSe2 (S.L. and J.H.) was supported by the NSF MRSEC program through the Columbia University Center for Precision-Assembled Quantum Materials (DMR-2011738). K.W. and T.T. acknowledge support from the JSPS KAKENHI (grant numbers 21H05233 and 23H02052), the CREST (JPMJCR24A5), JST and World Premier International Research Center Initiative (WPI), MEXT, Japan.These authors contributed equally: Luka Matej Devenica, Zach Hadjri, Jan Kumlin.Department of Quantum Matter Physics, University of Geneva, Geneva, Geneva, SwitzerlandLuka Matej Devenica, Zach Hadjri, Runtong Li, Weijie Li & Ajit SrivastavaDepartment of Physics, Emory University, Atlanta, USALuka Matej Devenica, Daniel Suárez-Forero, Klevis Domi, Bosai Lyu, Ludivine Fausten, Valeria Vento, Nicolas Ubrig & Ajit SrivastavaInstitute for Theoretical Physics, TU Wien, Vienna, AustriaJan Kumlin & Thomas PohlDepartment of Mechanical Engineering, Columbia University, New York, NY, USASong Liu & James HoneInstitute of Microelectronics, Chinese Academy of Sciences, Beijing, ChinaSong LiuResearch Center for Electronic and Optical Materials, National Institute for Materials Science, Tsukuba, JapanKenji WatanabeInternational Center for Materials Nanoarchitectonics, National Institute for Materials Science, Tsukuba, JapanTakashi TaniguchiSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarA.S., T.P., L.M.D., Z.H. and D.S.-F. conceived the project. K.W. and T.T. provided the hBN crystals, and S.L. and J.H. provided the WSe2 crystals. L.M.D., B.L., W.L., Z.H. and L.F. prepared the samples. L.M.D., Z.H., R.L., D.S.-F., K.D., B.L., V.V., N.U. and L.F. carried out the measurements. J.K. and T.P. developed the theoretical model and conducted the Monte Carlo simulations. A.S. and T.P. supervised the project. All authors were involved in the analysis of the experimental data and contributed extensively.Correspondence to Daniel Suárez-Forero, Thomas Pohl or Ajit Srivastava.The authors declare no competing interests.Nature Materials thanks the anonymous reviewers for their contribution to the peer review of this work.Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.Supplementary Figs. 1–17 and Notes 1–5.Statistical source data.Statistical source data.Statistical source data.Statistical source data.Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.Reprints and permissionsDevenica, L.M., Hadjri, Z., Kumlin, J. et al. Collective photon emission and ferroelectric exciton ordering near Mott insulating state in WSe2/WS2 heterobilayers. Nat. Mater. (2026). https://doi.org/10.1038/s41563-025-02476-4Download citationReceived: 05 March 2025Accepted: 19 December 2025Published: 29 January 2026Version of record: 29 January 2026DOI: https://doi.org/10.1038/s41563-025-02476-4Anyone you share the following link with will be able to read this content:Sorry, a shareable link is not currently available for this article. Provided by the Springer Nature SharedIt content-sharing initiative
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