Energetics of Solvent-Based Deposition of FullereneDerivative on the Inorganic–Organic Hybrid Lead Halide PerovskiteSurface

The elementary processes that govern particle deposition on substrates during solution processing of thin films are not well understood due to the complex interactions between solute–solvent, solute–substrate, and solvent–substrate. This study presents a fundamental step-by-step systematic analysis of the deposition of a rather complex molecule, the [6,6]-phenyl-C61-butyric acid methyl ester (PCBM), with seemingly infinite orientational configurations, on the (110) surface of methylammonium lead iodide (CH3NH3PbI3) perovskite in a solvated environment. We employed the adaptive biasing force (ABF) method in conjunction with classical molecular dynamics (MD) simulations to determine the potential of mean force (PMF) and corresponding configurations of deposited PCBM in the presence of chlorobenzene (CB) and vacuum. Our calculations underscore the impact of solvent on the energetics of deposition and the resulting configurations of deposited PCBM. In the presence of solvent, the most energetically favorable ...