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    The Role of Fluorine-Functionalized Organic Spacers for Defect Passivation and Low-Dimensional Phase Formation in 3D MAPI Perovskite Solar Cells
    (WILEY-V C H VERLAG GMBH, 2025) Semerci, A; Urieta-Mora, J; Driessen, S; Buyruk, A; Hooijer, R; Molina-Ontoria, A; Alkan, B; Akın, S; Fanetti, M; Balakrishnan, H; Hartschuh, A; Tao, SX; Martin, N; Müller-Buschbaum, P; Emin, S; Ameri, T
    Widespread application of organic-inorganic halide perovskites (OIHP) still faces a major obstacle in mitigating moisture-induced degradation. Integrating organic spacers, as defect passivation facilitators along with low-dimensional phase (LDP) formation is an effective approach to enhance the efficiency and robustness of 3D methyl ammonium lead iodide (MAPI) in photovoltaics (PV). Here, the formamidinium cation (FA+) employing 3,5-difluorobenzene-1-carboximidamidium iodide (2F), 4-(trifluoromethyl)benzene-1-carboximidamidium iodide (3F), and 2,3,4,5,6-pentafluorobenzene-1-carboximidamidium iodide (5F) organic spacers as passivation layer in 3D/LDP OIHP solar cells is utilized. Fluorine atom position and quantity in organic spacers change the optoelectronic characteristics of the perovskites, enhancing hydrophobicity, facilitating LDP formation, and augmenting dipole moments, thereby facilitating charge separation processes. PV performance analysis reveals that 3F-treated 3D/LDP devices achieve the highest efficiency of 19.22%. Experimental results and density functional theory (DFT) studies attribute the higher performance of 3F-modified devices to effective LDP formation, enhanced passivation of defect states at perovskite surfaces and grain boundaries, the highest dipole moment and lowest band gap among the evaluated spacers. The stability tests show that, after 1000 h, 3F- and 5F-modified 3D/LDP OIHP devices retain over 85% of their initial efficiency. This research opens novel avenues for designing appropriate organic spacers to attenuate defects in 3D/LDP PV devices.