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Two-dimensional (2D) perovskites show better resistance and optoelectronic characteristics than three-dimensional compounds. However, the high exciton energy and insufficient interfacial charge flow significantly reduce perovskite device performance. In this regard, a strategy to obtain high-performance 2D perovskite solar cells employing synergistic impact of coadditives (NH4SCN and HCl) to enable the proper alignment of perovskite films through the substrate, which eventually increases crystallinity and charge transport of 2D perovskites and reduces defect states, is presented. This coadditive method successfully generates homogeneous 2D perovskite films with consistent crystal structures and higher film quality. The champion 2D perovskite device exhibited a photovoltaic performance of 16.45% with an improved J sc. These results suggest that developing additive engineering might result in remarkably stable and efficient 2D perovskite materials.

Perovskite solar cells have been intensively studied recently due to their superb optoelectronic properties and rapidly increasing power conversion efficiency. However, perovskite solar cells with the AMX3 structure as the light‐absorbing layer have a big stability problem. Multiple alternatives have been developed to ensure their stability, such as dimensional engineering (2D and 2D/3D), which consists of the incorporation of large organic cations into the perovskite structure. Research in dimensional engineering has been prevalent in the Ruddlesden–Popper phases. The presence of this large cation slows the decomposition and improves the stability of perovskites. Thus, new 2D perovskites are being studied based on Dion–Jacobson (DJ) phases, consisting of the addition of diammonium cations and leading to the formation of 2D and 2D/3D perovskites with better stability due to their hydrogen bonding on both sides. Moreover, 2D DJ perovskites offer the advantage of decreasing the gap between layers with higher contacts, which improves not only their optoelectronic properties, but also their charge transport properties. This article begins with an overview of the crystal structure and optoelectronic characteristics of 2D perovskites. Then, the progress achieved currently in using DJ‐phase perovskites in photovoltaic is assessed. Finally, the possible research routes for producing low‐dimensional perovskites are highlighted.

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