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Nanoscale size effects in α-FAPbI3 evinced by large-scale ab initio simulations

Author

Listed:
  • Virginia Carnevali

    (Swiss Federal Institute of Technology (EPFL))

  • Lorenzo Agosta

    (Swiss Federal Institute of Technology (EPFL))

  • Vladislav Slama

    (Swiss Federal Institute of Technology (EPFL))

  • Nikolaos Lempesis

    (Swiss Federal Institute of Technology (EPFL)
    University of Ioannina)

  • Andrea Vezzosi

    (Swiss Federal Institute of Technology (EPFL))

  • Ursula Rothlisberger

    (Swiss Federal Institute of Technology (EPFL))

Abstract

Formamidinium-lead-iodide (FAPbI3) has a rich phase diagram, and long-range correlation between the organic cations and lattice dipoles can influence phase transitions and optoelectronic properties. System size effects are crucial for an appropriate theoretical description of FAPbI3. We perform a systematic ab initio study on the structural and electronic properties of the photoactive phase of FAPbI3 as a function of system size. To ensure an accurate theoretical description, three criteria must be satisfied: the (correct) value of the band gap, the extent (or the absence of) structural distortions, and the zeroing out of the total dipole moment. The net dipole moment vanishes as the system size increases due to PbI6 octahedra distortions rather than due to FA+ rotations. Additionally, thermal band gap fluctuations are predominantly correlated with octahedral tilting. The optimal agreement between simulation results and experimental properties for FAPbI3 is only achieved by system sizes approaching the nanoscale.

Suggested Citation

  • Virginia Carnevali & Lorenzo Agosta & Vladislav Slama & Nikolaos Lempesis & Andrea Vezzosi & Ursula Rothlisberger, 2025. "Nanoscale size effects in α-FAPbI3 evinced by large-scale ab initio simulations," Nature Communications, Nature, vol. 16(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-61351-7
    DOI: 10.1038/s41467-025-61351-7
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    1. So Min Park & Mingyang Wei & Nikolaos Lempesis & Wenjin Yu & Tareq Hossain & Lorenzo Agosta & Virginia Carnevali & Harindi R. Atapattu & Peter Serles & Felix T. Eickemeyer & Heejong Shin & Maral Vafai, 2023. "Low-loss contacts on textured substrates for inverted perovskite solar cells," Nature, Nature, vol. 624(7991), pages 289-294, December.
    2. Adam D. Wright & Carla Verdi & Rebecca L. Milot & Giles E. Eperon & Miguel A. Pérez-Osorio & Henry J. Snaith & Feliciano Giustino & Michael B. Johnston & Laura M. Herz, 2016. "Electron–phonon coupling in hybrid lead halide perovskites," Nature Communications, Nature, vol. 7(1), pages 1-9, September.
    3. Marina R. Filip & Giles E. Eperon & Henry J. Snaith & Feliciano Giustino, 2014. "Steric engineering of metal-halide perovskites with tunable optical band gaps," Nature Communications, Nature, vol. 5(1), pages 1-9, December.
    4. Yuhang Liang & Feng Li & Xiangyuan Cui & Taoyuze Lv & Catherine Stampfl & Simon P. Ringer & Xudong Yang & Jun Huang & Rongkun Zheng, 2024. "Toward stabilization of formamidinium lead iodide perovskites by defect control and composition engineering," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
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