Abstract
Fast thermal dephasing limits macroscopic quantum phenomena to cryogenic conditions1,2,3,4 and hinders their use at ambient temperatures5,6. For electronic excitations in condensed media, dephasing is mediated by thermal lattice motion1,7,8. Therefore, taming the lattice influence is essential for creating collective electronic quantum states at high temperatures. Although there are occasional reports of high-Tc quantum effects across different platforms, it is unclear which lattice characteristics and electron–lattice interactions lead to macroscopically coherent electronic states in solids9. Here we studied intensity fluctuations in the macroscopic polarization during the emergence of superfluorescence in a lead halide perovskite10 and showed that spontaneously synchronized polaronic lattice oscillations accompany collective electronic dipole emission. We further developed an effective field model and theoretically confirmed that exciton–lattice interactions lead to a new electronically and structurally entangled coherent extended solitonic state beyond a critical polaron density. The analysis shows a phase transition with two processes happening in tandem: incoherent disordered polaronic lattice deformations establish an order, while macroscopic quantum coherence among excitons simultaneously emerges. Recombination of excitons in this state culminates in superfluorescence at high temperatures. Our study establishes fundamental connections between the transient superfluorescence process observed after the impulsive excitation of perovskites and general equilibrium phase transitions achieved by thermal cooling. By identifying various electron–lattice interactions in the perovskite structure and their respective role in creating collectively coherent electronic effects in solids, our work provides unprecedented insight into the design and development of new materials that exhibit high-temperature macroscopic quantum phenomena.
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Data availability
All data in the main text are provided with this paper. All other data supporting the plots in this paper are available from the corresponding author upon request. Source data are provided with this paper.
Code availability
The FHI-aims code, which was used for DFT-based calculations in this work, is a community-developed electronic structure code that can be obtained from https://fhi-aims.org. The licensing organization, MS1P e.V., is a non-profit organization focused on advancing basic science, based in Berlin, Germany. At the time of writing, co-author V.B. was the vice chair of MS1P e.V. Academic licenses for the FHI-aims code can be obtained for a voluntary license fee (that is, free of charge if requested) by any academic group. The code is distributed with full access to its source code, including all development repositories. The ELSI infrastructure software, referenced in the paper, is an open-source library to which FHI-aims links. ELSI can be obtained freely under the BSD3 open-source license at https://gitlab.com/elsi_project/elsi_interface.
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Acknowledgements
K.G., M.B. and M.T. acknowledge funding support from the Department of Energy, Office of Science under award no. DE-SC0024396 (optical spectroscopy and analytical theory development). K.G. and M.T. acknowledge discussions with M. Unsal. K.G. and M.B. acknowledge the NCSU Imaging and Kinetic Spectroscopy facility. V.V.T. acknowledges support from the CNRS Tremplin, Toptica Photonics, the Physics Department of École Polytechnique and Institut Polytechnique de Paris within the framework of a Projet de Recherche en Laboratoire, and R. Pretorian and T. Mocioi from the École Polytechnique for help with C++ programming of time-dependent parameters for Monte Carlo simulations. V.B., X.Q. and U.H. acknowledge funding support from the NSF award no. DMR-2323803, NSF award no. DMR-1729297 and NSF award no OAC-1450280 (DFT calculations). DFT calculations were carried out on resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the US Department of Energy under contract no. DE-AC02-05CH11231 using NERSC award BES-ERCAP0024246.
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K.G. conceived the research problem and the proposed mechanism and supervised the studies. M.B. led the PL, TRPL and pump–probe characterization and analysis with the help of D.S., M.K. and M.A.; N.P. performed double-pulse TRPL experiments; M.T. developed the effective field theory. DFT simulations were performed by X.Q., and the Delta SCF method was implemented by U.H., both supervised by V.B. Monte Carlo simulations were performed by A.G. and V.V.T.; R.S., J.C. and F.S. provided the samples. K.G., M.B. and M.T. drafted the paper with the help of A.K.S., V.B. and V.V.T. All the authors edited the paper.
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Biliroglu, M., Türe, M., Ghita, A. et al. Unconventional solitonic high-temperature superfluorescence from perovskites. Nature 642, 71–77 (2025). https://doi.org/10.1038/s41586-025-09030-x
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DOI: https://doi.org/10.1038/s41586-025-09030-x
