Coupling Evaporation, Chemical Reactions, and Crystallization: A Population-Balance Framework Applied to Two-Step Perovskite Crystallization
Abstract
A limited understanding of how evaporation couples to crystallization pathways hampers control over the formation of solution-processed perovskite photoactive layers. Identifying these mechanisms-and learning how to select and tune them-is essential for achieving the desired crystal morphology and, ultimately, improving solar-cell performance and stability. To investigate crystallization pathways in evaporating thin films, we develop a simple and general zero-dimensional population-balance model that couples evaporation, chemical reactions, and crystallization. We use the model to explore a range of parameters for a solvent-solute system that follows a two-step crystallization pathway: solvent evaporation first induces formation of a crystalline precursor, which subsequently recrystallizes into the final phase. The model predicts the evolution of the film composition during drying and provides quantitative LaMer curves. Based on these results, we introduce a vocabulary of "supply limitations" and "rate limitations" that enables the interpretation of crystallization kinetics in terms of the governing process conditions.
Related
- Polymer interface-driven perovskite crystallization in electrospun fibers
- Mitigating vertical crystallization inhomogeneity in blade-coated Sn–Pb perovskites for flexible all-perovskite tandem modules
- Interface-regulated vapour crystallization for ultrapure perovskite LEDs.
- Thermodynamic regularization based computational framework for strain-induced crystallization
- A physics-driven machine learning framework for predicting XRD patterns, magnetization, and magnetocaloric response in rare-earth-doped double perovskite oxides
BibTeX
@misc{segadlo2026coupling,
title = {{Coupling Evaporation, Chemical Reactions, and Crystallization: A Population-Balance Framework Applied to Two-Step Perovskite Crystallization}},
author = {K. Segadlo and O. J. J. Ronsin and J. Harting},
howpublished = {arXiv},
year = {2026},
month = oct,
doi = {10.48550/arxiv.2610.26591},
eprint = {2610.26591},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2610.26591},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - Coupling Evaporation, Chemical Reactions, and Crystallization: A Population-Balance Framework Applied to Two-Step Perovskite Crystallization
AU - K. Segadlo
AU - O. J. J. Ronsin
AU - J. Harting
PY - 2026
DA - 2026/10/19
PB - arXiv
DO - 10.48550/arxiv.2610.26591
UR - https://arxiv.org/abs/2610.26591
AB - A limited understanding of how evaporation couples to crystallization pathways hampers control over the formation of solution-processed perovskite photoactive layers. Identifying these mechanisms-and learning how to select and tune them-is essential for achieving the desired crystal morphology and, ultimately, improving solar-cell performance and stability. To investigate crystallization pathways in evaporating thin films, we develop a simple and general zero-dimensional population-balance model that couples evaporation, chemical reactions, and crystallization. We use the model to explore a range of parameters for a solvent-solute system that follows a two-step crystallization pathway: solvent evaporation first induces formation of a crystalline precursor, which subsequently recrystallizes into the final phase. The model predicts the evolution of the film composition during drying and provides quantitative LaMer curves. Based on these results, we introduce a vocabulary of "supply limitations" and "rate limitations" that enables the interpretation of crystallization kinetics in terms of the governing process conditions.
ER -