Dimensionality engineering has proved to be a reliable strategy for addressing the issue of perovskite stability. In this study, a series of previously unreported low-dimensional organic-inorganic hybrid perovskite single crystals were designed and grown by following a simple hydrothermal approach involving solution processing. The as-prepared terpyridine-derived perovskite single crystals displayed tunable structures and electronic dimensionality, which was closely associated with the crystal growth conditions. The performed DFT calculations suggested that the fluctuating conduction band edge demonstrates obvious charge delocalization associated with the π-conjugation effect, a feature promoting efficient charge transport by means of coupling structural dimensionality and electronic dimensionality. This study has provided new ideas for the design of new materials to be used in fields involving photovoltaic devices.
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