Abstract

Hybrid organic-inorganic perovskite materials have become one of the most promising semiconductors in optoelectronics, yet their instability under operating conditions obstructs their application.^[1] This has stimulated a range of strategies to address this challenge, including the development of low-dimensional or layered perovskite architectures comprising of organic spacer moieties templating hybrid perovskite slabs.^[2] We purposefully tailor supramolecular interactions with the organic components to template hybrid perovskite architectures,^[3–6] such as through halogen bonding^[4] or π-based interactions,^[5–6] as well as host-guest complexation,^[7] which has been uniquely assessed by solid-state NMR crystallography. As a result, we have achieved perovskite solar cells with superior operational stabilities without compromising their photovoltaic performances,^[3,5,7] which provides a versatile strategy for hybrid perovskite photovoltaics. Moreover, we have extended the functionality of the organic spacer layers by introducing electroactive components into layered hybrid perovskite frameworks^[8–9] and exploiting their mechanochromism,^[10] providing a new platform for advanced optoelectronic applications.

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