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Room-temperature epitaxy of α-CH3NH3PbI3 halide perovskite by pulsed laser deposition

Nature Synthesis volume 4, pages 432–443 (2025)Cite this article

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Abstract

Epitaxial growth on lattice-(mis)matched substrates has advanced the understanding of semiconductors and enabled high-end technologies such as III-V-based light-emitting diodes. However, for metal halide perovskites, there is a knowledge gap in thin film heteroepitaxial growth, hindering progress towards new applications. Here we demonstrate the epitaxial growth of cubic (α)-CH3NH3PbI3 films on lattice-matched KCl substrates by pulsed laser deposition at room temperature. Epitaxial stabilization of α-CH3NH3PbI3 is confirmed via reciprocal space mapping, X-ray diffraction pole figures, electron backscatter diffraction and photoluminescence. A bandgap of 1.66 eV stable for over 300 days and Urbach energies of 12.3 meV for 15-nm-thick films are demonstrated. The impact of strain on α-phase stabilization is corroborated by first-principles density functional theory calculations, which also predict substantial bandgap tunability. This work demonstrates the potential of pulsed laser deposition for vapour-phase heteroepitaxial growth of metal halide perovskites, inspiring studies to unlock novel functionalities.

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Fig. 1: Heteroepitaxy of halide perovskite thin films by PLD, a case of CH3NH3PbI3 on KCl.
Fig. 2: Structural insights from XRD.
Fig. 3: Structural insights from RSMs and PFs from XRD, SEM and electron backscattering diffraction.
Fig. 4: Epitaxial growth on lattice-mismatched substrates.
Fig. 5: Epitaxial strain-dependent bandgap calculations of CH3NH3PbI3 phases using first-principles DFT.
Fig. 6: Influence of thickness on PL and Urbach energy.
Fig. 7: Charge-carrier transport and recombination for 15-nm-thick and 70-nm thick α-CH3NH3PbI3 films on KCl.

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Source data are provided with this paper. Supplementary data are available in the Supplementary Information.

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Acknowledgements

We acknowledge the technical support from the TSST part of Demcon, Dominic Post and the MESA+ staff, M. A. Smithers, M. J. Goodwin and M. Tsvetanova for performing the SEM, FIB and TEM measurements, respectively. This work is financed by the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation Program (CREATE, grant agreement no. 852722) received by M.M.-M. N.O. and E.C.G. acknowledge the Dutch Research Council (NWO), Gatan (EDAX), Amsterdam Scientific Instruments (ASI) and CL Solutions for financing the project ‘Achieving Semiconductor Stability From The Ground Up’ (project number 19459), which enabled the EBSD characterization. N.F.-C. and S.E.R.-L. acknowledge the financial support from ANID FONDECYT Regular grant number 1220986. N.F.C. acknowledges partial financial support from the project InTec, code ‘FRO2395’, from the Ministry of Education of Chile. Powered@NLHPC: This research was partially supported by the supercomputing infrastructure of the National Laboratory for High Performance Computing (NLHPC) (CCSS210001). M.L. acknowledges the support of the Czech Science Foundation (project no. 23-06598S) and the use of the CzechNanoLab research infrastructure supported by the MEYS (project no. LM2023051). T.B.H. and L.M.H. acknowledge financial support from the Engineering and Physical Sciences Research Council (EPSRC). J.R.S.L. thanks Oxford Photovoltaics for additional support as part of an EPSRC Industrial CASE studentship.

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Authors and Affiliations

  1. MESA+ Institute for Nanotechnology, University of Twente, Enschede, the Netherlands

    Junia S. Solomon, Tatiana Soto-Montero, Yorick A. Birkhölzer, Daniel M. Cunha, Wiria Soltanpoor, Gertjan Koster, Guus Rijnders, Linn Leppert & Monica Morales-Masis

  2. Institute of Physics, Academy of Sciences of the Czech Republic, Prague, Czech Republic

    Martin Ledinský

  3. Center for Nanophotonics, AMOLF, Science Park, Amsterdam, the Netherlands

    Nikolai Orlov & Erik C. Garnett

  4. Van der Waals-Zeeman Institute, Institute of Physics, University of Amsterdam, Amsterdam, the Netherlands

    Erik C. Garnett

  5. Doctorado en Fisicoquímica Molecular, Facultad de Ciencias Exactas, Universidad Andres Bello, Santiago, Chile

    Nicolás Forero-Correa

  6. Departamento de Ciencias Físicas, Universidad de La Frontera, Temuco, Chile

    Nicolás Forero-Correa

  7. Departamento de Física y Astronomía, Universidad Andres Bello, Santiago, Chile

    Sebastian E. Reyes-Lillo

  8. Clarendon Laboratory, Department of Physics, University of Oxford, Oxford, UK

    Thomas B. Haward, Joshua R. S. Lilly & Laura M. Herz

  9. Institute for Advanced Study, Technical University of Munich, Garching, Germany

    Laura M. Herz

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  1. Junia S. Solomon
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Contributions

J.S.S. and M.M.-M. conceived the idea. J.S.S. and T.S.-M. performed the initial optimization of the deposition. J.S.S. prepared the thin films by PLD and performed the XRD, PL and AFM measurements and analysis. Y.A.B. and D.M.C. supported RSMs, XRD PF measurements and analysis. G.K. and G.R. provided advisory support for the discussion of results from RSM and XRD PF measurements and analysis. N.O. and E.C.G. performed the EBSD and synchrotron XRD measurements and analysis. M.L. guided PL and Urbach energy analysis. T.B.H., J.R.S.L. and L.M.H. performed the time-resolved spectroscopic measurements and analysis. N.F.-C., S.E.R.-L. and L.L. performed the theoretical calculations. J.S.S., T.S.-M., Y.A.B., D.M.C., W.S., S.E.R.-L., L.L. and M.M.-M. performed the investigation. J.S.S., T.S.-M., Y.A.B., N.O., M.L., S.E.R.-L., L.L. and M.M.-M. worked on the visualization of the results. M.M.-M. supervised the overall work. J.S.S. and M.M.-M. wrote the paper with input from all the authors. All the coauthors analysed and discussed the results.

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Correspondence to Junia S. Solomon or Monica Morales-Masis.

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Supplementary Figs. 1–13 and Tables 1–3.

Supplementary Video 1

Scotch tape experiment to demonstrate the strong interactions between the substrate and the adlayer.

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Statistical source data.

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Statistical source data.

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Statistical source data.

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DFT data.

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Statistical source data.

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Solomon, J.S., Soto-Montero, T., Birkhölzer, Y.A. et al. Room-temperature epitaxy of α-CH3NH3PbI3 halide perovskite by pulsed laser deposition. Nat. Synth 4, 432–443 (2025). https://doi.org/10.1038/s44160-024-00717-z

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