“…Despite the rapid progress in research on single crystals of 3D HOIPs, , the amount of studies related to single crystals of 2D HOIPs remains comparatively limited, with the notable exception of 2D HOIPs containing phenethylammonium- and alkylammonium-based cations. − However, recent reports have shown that extended aromatic systems can improve the efficiency and/or stability in thin-film devices . For example, carefully designed organic cations based on carbazole, − pyrene, oligothiophene, − or benzothienobenzothiophene have resulted in perovskite thin films with specific optoelectronic properties, such as improved charge carrier mobility ,, and lifetime. , Moreover, our research group − and others have demonstrated the self-assembly of organic charge–transfer complexes into the organic layers of perovskite films by intercalating an acceptor chromophore into an organic layer containing electron donating organic cations, resulting in long-lived charge carriers and a reduced exciton binding energy . 2D HOIP single-crystal research with tailored aromatic moieties can therefore catalyze studies to ultimately maximize the figures of merit of various optoelectronic devices.…”