Multimode phonon-polaritons in lead-halide perovskites in the ultrastrong coupling regime

Dasom Kim, Jin Hou, Geon Lee, Ayush Agrawal, Sunghwan Kim, Hao Zhang, Di Bao, Andrey Baydin, Wenjing Wu, Fuyang Tay, Shengxi Huang, Elbert E. M. Chia, Dai-Sik Kim, Minah Seo, Aditya D. Mohite, David Hagenmüller and Junichiro Kono ()
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Dasom Kim: Rice University
Jin Hou: Rice University
Geon Lee: Korea Institute of Science and Technology
Ayush Agrawal: Rice University
Sunghwan Kim: Ulsan National Institute of Science and Technology (UNIST)
Hao Zhang: Rice University
Di Bao: Nanyang Technological University
Andrey Baydin: Rice University
Wenjing Wu: Rice University
Fuyang Tay: Rice University
Shengxi Huang: Rice University
Elbert E. M. Chia: Nanyang Technological University
Dai-Sik Kim: Seoul National University
Minah Seo: Korea Institute of Science and Technology
Aditya D. Mohite: Rice University
David Hagenmüller: Université de Strasbourg and CNRS
Junichiro Kono: Rice University

Nature Communications, 2025, vol. 16, issue 1, 1-9

Abstract: Abstract Phonons play a central role in fundamental solid-state phenomena, including superconductivity, Raman scattering, and symmetry-breaking phases. Harnessing phonons to control these effects and enable quantum technologies is therefore of great interest. However, most existing phonon control strategies rely on external driving fields or anharmonic interactions, limiting their applicability. Here, we realize multimode ultrastrong light–matter coupling and theoretically show the modulation of phonon emission. This regime is realized by coupling two optical phonon modes in lead halide perovskites to a nanoslot array functioning as a single-mode cavity. The small mode volume of the nanoslots enables high coupling strengths in the phonon-polariton system. We show theoretically that the nanoslot resonator mediates an effective interaction between phonon modes, leading to superthermal phonon bunching in thermal equilibrium between distinct modes. Our findings are well described by a multimodal Hopfield model. This work establishes a pathway for engineering phononic properties for light-harvesting and light-emitting technologies.

Date: 2025
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DOI: 10.1038/s41467-025-63810-7

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