Structural and Optical Properties of Solvated PbI2 in γ-Butyrolactone: Insight into the Solution Chemistry of Lead Halide Perovskite Precursors

We employ a fine-tuned theoretical framework, combining ab initio molecular dynamics (AIMD), density functional theory (DFT), and time-dependent (TD) DFT methods, to investigate the interactions and optical properties of the iodoplumbates within the low coordinative γ-butyrolactone (GBL) solvent environment, widely employed in the perovskite synthesis. We uncover the extent of GBL coordination to PbI₂ investigating its relation to the solvated PbI₂ optical properties. The employed approach has been further validated by comparison with the experimental UV-vis absorption spectrum of PbI₂ in GBL solvent. A comparison with other solvents, commonly employed in the perovskite synthesis, such as N,N-dimethylformamide (DMF) and dimethyl sulfoxide (DMSO) is also reported. The methodology developed in this work can be reasonably extended to the investigation of similar systems.