Abstract

Hybrid perovskites have emerged as one of the leading materials in photovoltaics due to their remarkable optoelectronic properties and solar-to-electric power conversion efficiencies [1-2]. However, their limited stabilities under ambient and operating conditions remain challenging [1-2]. On the contrary, layered hybrid perovskites based on the assemblies of organic and inorganic components feature superior operational stabilities [3-8]. To this end, supramolecular chemistry provides a powerful tool for controlling hybrid materials by tailoring noncovalent interactions. We demonstrate the utility of this approach through designing molecular modulators based on fine-tuning various noncovalent interactions [8-11], such as metal coordination [10], hydrogen [5,10] or halogen bonding [9], and π-interactions [8], among others [11]. Furthermore, their structure-directing (i.e. templating) role has been uniquely assessed by solid-state NMR spectroscopy and DFT calculations [5-7,9-11]. As a result, we obtain perovskite solar cells that exhibit superior performances and enhanced operational stabilities [8-11]. Moreover, the underlying molecular design has been extended into creating layered perovskite architectures that enable further control through templating effects [3-7]. This has been investigated by using a combination of techniques to unravel the design principles and exemplify the utility of supramolecular chemistry in advancing photovoltaics.

[1] J. V. Milić et al. Chimia 2019, 73, 317; [2] M. Graetzel et al. Substantia 2019, 3, 27; [3] Y. Li et al. Nano Lett. 2019, 19, 150; [4] J. V. Milić et al. Adv. Energy Mater. 2019, 1900284; [5] L. Hong, et al. Angew. Chem. Int. Ed. 2020, 59, 4691; [6] F. Jahanbakhshi et al. J. Mater. Chem. A 2020 , 8, 17732; [7] M. C. Gélvez-Rueda et al. Adv. Funct. Mater. 2020, 2003428; [8] Y. Liu et al. Sci. Adv. 2019, 5, eaaw2543; [9] M. A. Ruiz-Preciado et al. J. Am. Chem. Soc. 2020, 142, 1645 [10] D. Bi et al. Nat. Commun. 2018, 9, 4482 [11] T-Z. Su et al. J. Am. Chem. Soc. 2020, in press.