Stabilizing Hybrid Perovskite Materials through Supramolecular Templating in Photovoltaics*

Hybrid organic-inorganic perovskites have emerged as one of the most promising semiconductor materials in photovoltaics, yet their instability under operating conditions interferes with their applications. To address this challenge, we rely on supramolecular tools by purposefully tailoring noncovalent interactions to template hybrid perovskite architectures through halogen bonding, π-based interactions, and host-guest complexation, which has been assessed by solid-state NMR spectroscopy. As a result, we have achieved perovskite solar cells with superior operational stabilities without compromising their photovoltaic performances, which provides a versatile strategy for advancing hybrid perovskite photovoltaics.