• Accepted Paper

Bridging surface dynamics and phase transitions in CsPbI3 perovskite with machine-learning force fields and dispersion interactions

Iryna Knysh, Anton Charkin-Gorbulin, Claudio Quarti, David Beljonne, Igor Poltavsky, and Alexandre Tkatchenko

Phys. Rev. Materials - Accepted 15 October, 2026

DOI: https://doi.org/10.1103/qcvb-y84n

Abstract

In the rapidly evolving field of machine learning (ML) for atomistic simulations of materials and molecules, achieving transferability across different systems remains a key challenge. In this contribution, we demonstrate a case of transfer learning in which an ML model trained exclusively on surface slab data of the cubic (α) phase of CsPbI3 perovskite can reproduce the key features of the dynamic behavior for different phases of the bulk material. Using an equivariant message-passing network (MACE) architecture, we construct an efficient ML force-field trained on the dataset obtained from the molecular dynamics simulations of a CsPbI3 slab. The resulting model yields stable and reliable trajectories for both slab and bulk, reproducing the experimentally observed phase transitions of CsPbI3. We demonstrate that pairwise dispersion methods (TS/D3) mispredict the correct phase of CsPbI3 bulk at ambient conditions, while more advanced approaches (MBD-NL/rVV10) recover both the experimentally observed phase sequence with increasing temperature (orthorhombic–tetragonal–cubic) and the corresponding phase-transition temperatures. Through a local analysis of the rotational driving forces acting on PbI6 octahedra, we show that this discrepancy can be traced to the strong sensitivity of Cs and I atomic forces to the treatment of van der Waals (vdW) dispersion. Overall, our results demonstrate that surface–slab datasets augmented with an accurate treatment of vdW dispersion provide a robust foundation for constructing transferable machine-learning force fields that consistently describe both surface and bulk behavior across multiple length scales.

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