Project: ADRENALINE - hAliDe peRovskites sEqueNtiAL deposItioN mEchanism (by ab initio rare events simulations).

Prace Call: 17th
ID: 2018184423, Leader: Simone Meloni
Affiliation: Sapienza University of Rome (IT), IT
Research Field: Chemical Sciences and Materials
Collaborators: Lorenzo Gontrani University of Rome Sapienza IT , Diego Di Girolamo Sapienza University of Rome IT , Sara Marchio Sapienza University of Rome (IT) IT
Resource Awarded: 78 Mil. core hours on Piz Daint

Abstract

The objective of the ADRENALINE project is to study the atomistic mechanism, energetics and kinetics of the sequential deposition method of (hybrid) lead halide perovskites for 3rd generation solar cells and optoelectronics applications. The project is based on ab initio rare event simulations of the key step of the process, the intercalation of the cation A+ (methylammonium, CH3NH3+, formamidinium, (NH2)2CH+, and Cesium cation, Cs+) and anion X- (I-, Br- and Cl-) and reorganization of the intermediate product into the final one. We intend to address several questions about these stages: • What are the intercalation site of cations and anions? How do they change from cation to cation and from anion/precursor to anion/precursor? • What is the driving force pushing cations and anions solvated in isopropyl alcohol (or other suitable solvents) to intercalate into the precursor structure? • What is the atomistic structure of the intermediate compound? • What is the mechanism and kinetics of formation of the intermediate compound from the intercalated ions? • What is the driving force pushing the intermediate compound to transform into the corresponding perovskite? • What is the mechanism and kinetics of the transformation of the intermediate compound into the corresponding perovskite? • Overall, what is the mechanism and energetics of the entire intercalation and reorganization step of the sequential deposition process? What is the rate limiting step? How do these quantities depend on the type of halide, and the associated precursor? How do they depend on the nature of the cation? The ADRENALINE project will have a significant impact on the fabrication of perovskite devices; the knowledge of the energetics and kinetics of the various stage of the intercalation and reorganization step of the overall formation reaction, the identification of the role of the solvent will allow improving the deposition mechanism, thus contributing to further enhance the efficiency and stability of lead halide perovskites solar cells.