Synthetic control over orientational degeneracy of spacer cations enhances solar cell efficiency in two-dimensional perovskites

Jun Hu, Iain W. H. Oswald, Samuel J. Stuard, Masrur Morshed Nahid, Ninghao Zhou, Olivia F. Williams, Zhenkun Guo, Liang Yan, Huamin Hu, Zheng Chen, Xun Xiao, Yun Lin, Zhibin Yang, Jinsong Huang, Andrew M. Moran, Harald Ade, James R. Neilson and Wei You ()
Additional contact information
Jun Hu: University of North Carolina at Chapel Hill
Iain W. H. Oswald: Colorado State University
Samuel J. Stuard: North Carolina State University
Masrur Morshed Nahid: North Carolina State University
Ninghao Zhou: University of North Carolina at Chapel Hill
Olivia F. Williams: University of North Carolina at Chapel Hill
Zhenkun Guo: University of North Carolina at Chapel Hill
Liang Yan: University of North Carolina at Chapel Hill
Huamin Hu: University of North Carolina at Chapel Hill
Zheng Chen: University of North Carolina at Chapel Hill
Xun Xiao: University of North Carolina at Chapel Hill
Yun Lin: University of North Carolina at Chapel Hill
Zhibin Yang: University of North Carolina at Chapel Hill
Jinsong Huang: University of North Carolina at Chapel Hill
Andrew M. Moran: University of North Carolina at Chapel Hill
Harald Ade: North Carolina State University
James R. Neilson: Colorado State University
Wei You: University of North Carolina at Chapel Hill

Nature Communications, 2019, vol. 10, issue 1, 1-11

Abstract: Abstract Two-dimensional perovskites have emerged as more intrinsically stable materials for solar cells. Chemical tuning of spacer organic cations has attracted great interest due to their additional functionalities. However, how the chemical nature of the organic cations affects the properties of two-dimensional perovskites and devices is rarely reported. Here we demonstrate that the selection of spacer cations (i.e., selective fluorination of phenethylammonium) affects the film properties of two-dimensional perovskites, leading to different device performance of two-dimensional perovskite solar cells (average n = 4). Structural analysis reveals that different packing arrangements and orientational disorder of the spacer cations result in orientational degeneracy and different formation energies, largely explaining the difference in film properties. This work provides key missing information on how spacer cations exert influence on desirable electronic properties and device performance of two-dimensional perovskites via the weak and cooperative interactions of these cations in the crystal lattice.

Date: 2019
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DOI: 10.1038/s41467-019-08980-x

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