Evolution of the Electronic and Excitonic Properties in 2D Ruddlesden–Popper Perovskites Induced by Bifunctional Ligands
Ball, Melissa L.
Rand, Barry P
AffiliationDepartment of Chemistry and Biochemistry, The University of Arizona
KeywordsGeneral Materials Science
Renewable Energy, Sustainability and the Environment
bifunctional organic ligands
exciton binding energy
MetadataShow full item record
CitationX. Zhong, X. Ni, A. Kaplan, X. Zhao, M. Ivancevic, M. L. Ball, Z. Xu, H. Li, B. P. Rand, Y.-L. Loo, J.-L. Brédas, A. Kahn, Evolution of the Electronic and Excitonic Properties in 2D Ruddlesden–Popper Perovskites Induced by Bifunctional Ligands. Adv. Energy Mater. 2024, 2304345. https://doi.org/10.1002/aenm.202304345
JournalAdvanced Energy Materials
Rights© 2024 Wiley-VCH GmbH.
Collection InformationThis item from the UA Faculty Publications collection is made available by the University of Arizona with support from the University of Arizona Libraries. If you have questions, please contact us at email@example.com.
Abstract2D Ruddlesden–Popper metal-halide perovskites exhibit structural diversity due to a variety of choices of organic ligands. Incorporating bifunctional ligands in such materials is particularly intriguing since it can result in novel electronic properties and functions. However, an in-depth understanding of the effects of bifunctional ligands on perovskite structures and, consequently, their electronic and excitonic properties, is still lacking. Here, n = 1 2D perovskites built with organic ligands containing ─CN, ─OH, ─COOH, ─phenyl (Ph), and ─CH3 functional groups are investigated using ultraviolet and inverse photoemission spectroscopies, density functional theory calculations, and tight-binding model analyses. The experimentally determined electronic gaps of the ─CN, ─COOH, ─Ph, and ─CH3 based perovskites exhibit a strong correlation with the in-plane Pb─I─Pb bond angle, while the ─OH based perovskite deviates from the linear trend. Based on the band structure calculations, this anomaly is attributed to the out-of-plane dispersion, caused predominantly by significant interlayer electronic coupling that is present in ─OH based perovskites. These results highlight the complex and diverse impacts of organic ligands on electronic properties, especially in terms of the involvement of strong interlayer electronic coupling. The impact of the bifunctional ligands on the evolution of the exciton binding energy is also addressed.
Note12 month embargo; first published 11 January 2024
VersionFinal accepted manuscript
SponsorsOffice of Naval Research