Proceedings of Perovskite Thin Film Photovoltaics (ABXPV16)
Publication date: 14th December 2015
While a massive effort is currently being made to develop competitive perovskite solar cells, the fundamental properties of these materials remain relatively unexplored. In this contribution we exclusively focus on the computational study such fundamental properties with no intention of contributing to the amelioration of perovskite solar cells efficiency. We focus here on traditional lead-iodide perovskites X-Pb-I3 where X is an organic cation. Several candidates are considered in our studies for example methylamonium, hyroxylamonium or guanidinium.
We present our recent computational studies related to the dipole organization within the perovskites structures and the impact that these domains have on the optoelectronic properties of the material. The organization of the dipoles in domains presenting a preferential orientation was studied using monte-carlo simulations. These simulations clearly demonstrate how large domains can form at low temperature. The stability of these domains was then assessed via molecular dynamics simulations using a dedicated force field. The relationship between domain orientation and opto-electronic properties of the perovskites was then studied using electronic structure calculations. Using a combination of ab-initio and semi-empirical techniques, we explore how localized electronic states can be created at the interface between domains. These states can potentially act as localized channels that keep the electrons and holes spacially separated thus increasing their lifetime. Finally the charge mobility of these materials was evaluated to understand how the domains formation can affect the charge propagation within these structures.
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