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

Virginia Carnevali¹, Lorenzo Agosta¹, Vladislav Slama¹

¹Laboratory of Computational Chemistry and Biochemistry, Institute of Chemical Sciences and Engineering, Swiss Federal Institute of Technology (EPFL), Lausanne, Switzerland.

Nature Communications

|July 24, 2025

Summary

System size significantly impacts formamidinium-lead-iodide (FAPbI3) properties. Accurate theoretical descriptions require nanoscale simulations to capture essential structural and electronic behaviors for optoelectronic applications.

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Area of Science:

Materials Science
Solid-State Physics
Computational Chemistry

Background:

Formamidinium-lead-iodide (FAPbI3) exhibits a complex phase diagram.
Organic cations and lattice dipoles influence FAPbI3's phase transitions and optoelectronic properties.

Purpose of the Study:

Investigate system size effects on FAPbI3's structural and electronic properties.
Determine the minimum system size for accurate theoretical modeling of FAPbI3.

Main Methods:

Systematic ab initio study of FAPbI3's photoactive phase.
Analysis of structural distortions, band gap, and dipole moment as a function of system size.

Main Results:

Net dipole moment vanishes with increasing system size due to PbI6 octahedra distortions.
Thermal band gap fluctuations correlate with octahedral tilting.
Accurate agreement with experimental properties is achieved at nanoscale system sizes.

Conclusions:

System size effects are critical for theoretical descriptions of FAPbI3.
Nanoscale simulations are necessary for reliable predictions of FAPbI3's properties.
Understanding these effects is key for optimizing FAPbI3-based optoelectronic devices.