Hybrid organic-inorganic perovskites have emerged as one of the most promising materials in photovoltaics. However, their instability under operating conditions hampers their practical application. This stimulates the development of hybrid materials with enhanced stabilities during operation. For this purpose, supramolecular chemistry provides a powerful toolbox for controlling the properties of hybrid materials by purposefully tailoring the noncovalent interactions of the organic components. We have demonstrated the role of supramolecular engineering in templating hybrid perovskite structures through halogen bonding and π-based interactions, as well as host-guest complexation, which has been uniquely assessed by solid-state NMR spectroscopy and NMR crystallography. As a result, we have obtained perovskite solar cells that exhibit superior performances and operational stabilities, highlighting the important role of supramolecular templating in advancing hybrid perovskite photovoltaics.
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