Carbazole-based hole-transport materials for efficient Perovskite solar cells. A computational study

In this study, DFT calculations carried out using Carbazole-based HTMs substituted with dimethoxy phenylamine units (DMPA) in positions 2,3,6,7 and 9 are coupled with the experimental results drawn from the literature. The most important challenge for us is to establish a link between the optoelectronic and structural properties of molecules and their performance as HTMs. In this work, we find that the important structural effect is generated by the pyridinic nucleus. The substituents linked to the nitrogen atom of carbazole do not contribute to HOMO or LUMO in most of the studied HTMs. Hence, apart from the illustrated performances, parameters as the contribution of such substituents to being attached to the perovskite, or to the cohesion of the HTM's molecules contributing to the perovskite stability all prove decisive. The 2,7 substitution favors more stabilization of LUMOs when compared to 3,6 substitution, which leads to a narrow gap for 2,7 homologous. This makes these 2,7-substituted molecules good candidates as light absorbent in Organic Solar cells. The differences in the solar cell performances using these HTMs is mostly linked to the effect of these groups on their intermolecular interactions on one hand, and on the interfacial contact between HTMs and perovskite on the other hand.