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Exciton diffusion beyond 2 μm enabled by maximum symmetry in two-dimensional perovskites

Nature Synthesis (2026)Cite this article

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Abstract

High crystallographic symmetry is a key feature of many inorganic semiconductors and underpins their remarkable physical properties. By contrast, hybrid (organic and inorganic) crystals such as two-dimensional metal halide perovskites exhibit much lower crystal symmetry due to in-plane or out-of-plane octahedral distortions. Although they exhibit efficient photoinduced emission at room temperature, limited control over charge carrier transport remains a major challenge for optoelectronic applications. Here, inspired by three-dimensional cubic (α-phase) FAPbI3 (FA, formamidinium), we developed FA-based layered two-dimensional perovskites using tailored cage cations, spacers and crystallization protocols. The compounds achieve near-maximal predicted symmetry, adopting a tetragonal P4/mmm space group without octahedral distortion. Among reported two-dimensional perovskites, these materials present short interlayer distances (4 Å) and lower optical bandgaps (1.7–1.8 eV). The absence of octahedral distortions results in an exciton diffusion length of 2.5 µm and a diffusivity of 4.4 cm2 s−1, both of which are an order of magnitude larger than those of previously reported two-dimensional perovskites and are on par with monolayer transition metal dichalcogenides.

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Fig. 1: Hot extraction method and structure of 2D FA DJ perovskites.
Fig. 2: Undistorted structure and optical properties of 2D FA DJ perovskites.
Fig. 3: Static structural properties of 2D FA DJ perovskites.
Fig. 4: Structure dynamics of 2D FA DJ perovskites.
Fig. 5: 2D FA DJ perovskite photodetectors.

Data availability

Crystallographic data for the structures reported in this Article have been deposited at the Cambridge Crystallographic Data Centre, under deposition numbers CCDC 2433611 (n = 2, RT), 2433612 (n = 2, 100 K), 2433613 (n = 3, RT), 2433615 (n = 3, 100 K), 2433614 (n = 4, RT) and 2433610 (n = 4, 100 K). All the data supporting the findings of this study are available in the Article and its Supplementary Information. The raw NMR data (.fid files) supporting this study are available via Figshare at https://doi.org/10.6084/m9.figshare.31427666 (ref. 107).

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Acknowledgements

This material is based upon work supported by the US National Science Foundation Science and Technology Center (STC) for Integration of Modern Optoelectronic Materials on Demand (IMOD) under cooperative agreement no. DMR-2019444. J.H. acknowledges the financial support from the China Scholarships Council (grant no. 202107990007). M.Z. acknowledges funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement no. 899546. G.V. acknowledges funding from the Agence Nationale pour la Recherche through the CPJ programme and the SURFIN project (ANR-23-CE09-0001). Access to the HPC resources of TGCC was obtained under the Allocation Grant No. 2025 - A0190907682 and A0180911434 made by GENCI. The authors acknowledge computational resources from the EuroHPC Joint Undertaking and supercomputer LUMI (https://lumi-supercomputer.eu/), hosted by CSC (Finland) and the LUMI consortium through a EuroHPC Access call. M.Y.S. was supported by the donors of ACS Petroleum Research Fund under grant no. 65743-ND6. C.W. and G.N.M.R. thank EU H2020 (grant no. 795091) and INFRANALYTICS FR-2054 CNRS. J.E. acknowledges financial support from the Institut Universitaire de France. S.J.H. acknowledges support from NSF grant no. HRD-2112550 (Phase II CREST Center IDEALS). S.S. and B.Z. acknowledge support from NSF/EPSCoR RII Track-1: EQUATE under award no. OIA-2044049. Y.G. acknowledges support from NSF under award no. DMR-2339721.

Author information

Author notes

  1. These authors contributed equally: Jin Hou, Jared Fletcher.

Authors and Affiliations

  1. Department of Materials Science and NanoEngineering, Rice University, Houston, TX, USA

    Jin Hou, Isaac Metcalf & Aditya D. Mohite

  2. Department of Chemistry, Northwestern University, Evanston, IL, USA

    Jared Fletcher, Stefan Zeiske, Isaiah W. Gilley, Donghoon Shin, Bin Chen & Mercouri G. Kanatzidis

  3. Photonics Initiative, Advanced Science Research Center, City University of New York, New York, NY, USA

    Siedah J. Hall & Matthew Y. Sfeir

  4. Department of Physics, The Graduate Center, City University of New York, New York, NY, USA

    Siedah J. Hall & Matthew Y. Sfeir

  5. Department of Chemical and Biomolecular Engineering, Rice University, Houston, TX, USA

    Hao Zhang, Faiz Mandani & Aditya D. Mohite

  6. Applied Physics Graduate Program, Smalley-Curl Institute, Rice University, Houston, TX, USA

    Hao Zhang

  7. University of Rennes, INSA Rennes, CNRS, Institut FOTON - UMR 6082, Rennes, France

    Marios Zacharias & Jacky Even

  8. University of Rennes, ENSCR, CNRS, Institut des Sciences Chimiques de Rennes - UMR 6226, Rennes, France

    George Volonakis & Claudine Katan

  9. University of Lille, CNRS, Centrale Lille Institute, Univ. Artois, UMR 8181 − UCCS− Unité de Catalyse et Chimie du Solide, Lille, France

    Claire Welton & G. N. Manjunatha Reddy

  10. Department of Chemistry, University of Nebraska-Lincoln, Lincoln, NE, USA

    Shuo Sun, Bo Zhang & Yinsheng Guo

Authors
  1. Jin Hou
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  2. Jared Fletcher
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  3. Siedah J. Hall
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  4. Hao Zhang
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  5. Marios Zacharias
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  6. George Volonakis
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  7. Claire Welton
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  8. Stefan Zeiske
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  9. Isaiah W. Gilley
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  10. Donghoon Shin
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  11. Faiz Mandani
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  12. Isaac Metcalf
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  13. Shuo Sun
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  14. Bo Zhang
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  15. Yinsheng Guo
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  16. Bin Chen
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  17. G. N. Manjunatha Reddy
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  18. Claudine Katan
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  19. Jacky Even
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  20. Matthew Y. Sfeir
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  21. Mercouri G. Kanatzidis
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  22. Aditya D. Mohite
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Contributions

A.D.M. conceived the idea. J.H. developed the synthetic method and conducted the experiments. J.F. performed the single-crystal XRD and refinement of the crystal structure under the guidance of M.G.K. J.H. performed 1D XRD measurements with the help of F.M. and I.M. H.Z. and J.H. performed optical characterizations. S.J.H. performed real-space diffusion measurements, corresponding diffusion length calculations and analysis under the supervision of M.Y.S. C.W. and G.N.M.R. performed ssNMR measurements and analysis. S.S. and B.Z. performed low-frequency Raman spectroscopy measurements under the guidance of Y.G. M.Z., G.V. and I.W.G. performed the calculations and analysed the computational results. D.S. performed atomic force microscopy thickness measurements. S.Z. performed photoreactor measurement and analysed the results with guidance from B.C. J.H., J.F., H.Z. performed data analysis with guidance from C.K., M.G.K., J.E. and A.D.M. J.H. wrote the manuscript with input from all authors. All authors read the manuscript and agree to its contents, and all data are reported in the main text and Supplementary Information.

Corresponding authors

Correspondence to Mercouri G. Kanatzidis or Aditya D. Mohite.

Ethics declarations

Competing interests

A.D.M. and J.H. have filed a PCT patent application (PCT/US25/23930) on a method for fabricating FA DJ 2D perovskites in the USA. The other authors declare no competing interests.

Peer review

Peer review information

Nature Synthesis thanks Jonghee Yang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. Primary Handling Editor: Alexandra Groves, in collaboration with the Nature Synthesis team.

Additional information

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Supplementary information

Supplementary Information (download PDF )

Supplementary Discussions 1.1–1.9, Figs. 1–47, Tables 1–7 and References.

Supplementary Data 1

Crystallographic data of DJ n = 2 at 100 K (CCDC number 2433612).

Supplementary Data 2

Crystallographic data of DJ n = 2 at RT (CCDC number 2433611).

Supplementary Data 3

Crystallographic data of DJ n = 3 at 100 K (CCDC number 2433615).

Supplementary Data 4

Crystallographic data of DJ n = 3 at RT (CCDC number 2433613).

Supplementary Data 5

Crystallographic data of DJ n = 4 at 100 K (CCDC number 2433610).

Supplementary Data 6

Crystallographic data of DJ n = 4 at RT (CCDC number 2433614).

Source data

Source Data Fig. 1 (download XLSX )

Statistical source data.

Source Data Fig. 2 (download XLSX )

Statistical source data.

Source Data Fig. 3 (download XLSX )

Statistical source data.

Source Data Fig. 4 (download XLSX )

Statistical source data.

Source Data Fig. 5 (download XLSX )

Statistical source data.

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Hou, J., Fletcher, J., Hall, S.J. et al. Exciton diffusion beyond 2 μm enabled by maximum symmetry in two-dimensional perovskites. Nat. Synth (2026). https://doi.org/10.1038/s44160-026-01041-4

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