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

Hu, Jun; Oswald, Iain W.  H.; Stuard, Samuel J.; Nahid, Masrur Morshed; Zhou, Ninghao; Williams, Olivia F.; Guo, Zhenkun; Yan, Liang; Hu, Huamin; Chen, Zheng; Xiao, Xun; Lin, Yun; Yang, Zhibin; Huang, Jinsong; Moran, Andrew M.; Ade, Harald; Neilson, James R.; You, Wei

doi:10.1038/s41467-019-08980-x

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

Journal Article · Wed Mar 20 00:00:00 UTC 2019 · Nature Communications

DOI: https://doi.org/10.1038/s41467-019-08980-x · OSTI ID:1612398

Hu, Jun ^[1]; Oswald, Iain W. H. ^[2];

^[3]; Nahid, Masrur Morshed ^[3]; Zhou, Ninghao ^[4]; Williams, Olivia F. ^[4]; Guo, Zhenkun ^[4];

^[4]; Hu, Huamin ^[4]; Chen, Zheng ^[4]; Xiao, Xun ^[5];

^[5]; Yang, Zhibin ^[5];

^[5]; Moran, Andrew M. ^[4]; Ade, Harald ^[3]; Neilson, James R. ^[2];

^[6]

Univ. of North Carolina, Chapel Hill, NC (United States). Dept. of Chemistry; DOE/OSTI
Colorado State Univ., Fort Collins, CO (United States). Dept. of Chemistry
North Carolina State Univ., Raleigh, NC (United States). Dept. of Physics
Univ. of North Carolina, Chapel Hill, NC (United States). Dept. of Chemistry
Univ. of North Carolina, Chapel Hill, NC (United States). Dept. of Applied Physical Sciences
Univ. of North Carolina, Chapel Hill, NC (United States). Dept. of Chemistry; Univ. of North Carolina, Chapel Hill, NC (United States). Dept. of Applied Physical Sciences

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.

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Research Organization:: Colorado State Univ., Fort Collins, CO (United States); Univ. of California, Oakland, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-05CH11231; SC0016083

OSTI ID:: 1612398

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 10; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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General Post-annealing Method Enables High-Efficiency Two-Dimensional Perovskite Solar Cells Yan, Liang; Hu, Jun; Guo, Zhenkun ACS Applied Materials & Interfaces, Vol. 10, Issue 39 https://doi.org/10.1021/acsami.8b10230	journal	September 2018
Charge-Carrier Dynamics and Crystalline Texture of Layered Ruddlesden–Popper Hybrid Lead Iodide Perovskite Thin Films Venkatesan, Naveen R.; Labram, John G.; Chabinyc, Michael L. ACS Energy Letters, Vol. 3, Issue 2 https://doi.org/10.1021/acsenergylett.7b01245	journal	January 2018
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Ligand-Stabilized Reduced-Dimensionality Perovskites Quan, Li Na; Yuan, Mingjian; Comin, Riccardo Journal of the American Chemical Society, Vol. 138, Issue 8 https://doi.org/10.1021/jacs.5b11740	journal	February 2016
Observation of Internal Photoinduced Electron and Hole Separation in Hybrid Two-Dimentional Perovskite Films Liu, Junxue; Leng, Jing; Wu, Kaifeng Journal of the American Chemical Society, Vol. 139, Issue 4 https://doi.org/10.1021/jacs.6b12581	journal	January 2017
Exploration of Crystallization Kinetics in Quasi Two-Dimensional Perovskite and High Performance Solar Cells Zhou, Ning; Shen, Yiheng; Li, Liang Journal of the American Chemical Society, Vol. 140, Issue 1 https://doi.org/10.1021/jacs.7b11157	journal	December 2017
Enhanced Out-of-Plane Conductivity and Photovoltaic Performance in n = 1 Layered Perovskites through Organic Cation Design Passarelli, James V.; Fairfield, Daniel J.; Sather, Nicholas A. Journal of the American Chemical Society, Vol. 140, Issue 23 https://doi.org/10.1021/jacs.8b03659	journal	May 2018
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CCDC 1893383: Experimental Crystal Structure Determination Jun, Hu,; H., Oswald, Iain W.; J., Stuard, Samuel https://doi.org/10.5517/ccdc.csd.cc21k6wq The current record is supplemented by this dataset	dataset	January 2019
CCDC 1893384: Experimental Crystal Structure Determination Jun, Hu,; H., Oswald, Iain W.; J., Stuard, Samuel https://doi.org/10.5517/ccdc.csd.cc21k6xr The current record is supplemented by this dataset	dataset	January 2019
CCDC 1893385: Experimental Crystal Structure Determination Jun, Hu,; H., Oswald, Iain W.; J., Stuard, Samuel https://doi.org/10.5517/ccdc.csd.cc21k6ys The current record is supplemented by this dataset	dataset	January 2019