Two-Dimensional Halide Perovskites Incorporating Straight Chain Symmetric Diammonium Ions, (NH3CmH2mNH3)(CH3NH3)n-1PbnI3n+1 (m = 4–9; n = 1–4)
Abstract
We report that low-dimensional halide perovskites have recently attracted intense interest as alternatives to the three-dimensional (3D) perovskites because of their greater tunability and higher environmental stability. Herein, we present the new homologous 2D series (NH3CmH2mNH3)(CH3NH3)n-1PbnI3n+1 (m = 4–9; n = 1–4), where m represents the carbon-chain number and n equals layer-thickness number. Multilayer (n > 1) 2D perovskites incorporating diammonium cations were successfully synthesized by the solid-state grinding method for m = 4 and 6 and by the solution method for m = 7–9. Structural characterization by single-crystal X-ray diffraction for the m = 8 and m = 9 series (n = 1–4) reveals that these compounds adopt the Cc space group for even n members and Pc for odd n members. The optical bandgaps are 2.15 eV for two-layer (n = 2), 2.01 eV for three-layer (n = 3), and 1.90 eV for four-layer (n = 4). The materials exhibit excellent solution processability, and casting thin-films of the n = 3 members was successfully accomplished. The films show a clear tendency for the higher-m members to have preferred orientation on the glass substrate, with m = 8 exhibiting almost perfect vertical layer orientation and m = 9 displayingmore »
- Authors:
-
[1];
[1];
[3];
[3];
[4];
[5];
[5];
[6];
[1];
[1];
[1]
- Northwestern Univ., Evanston, IL (United States)
- Northwestern Univ., Evanston, IL (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Rice Univ., Houston, TX (United States)
- Univ Rennes, ENSCR, INSA Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes) (France)
- Univ Rennes, INSA Rennes, CNRS, Institut FOTON (France)
- Publication Date:
- Research Org.:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Laboratory Directed Research and Development (LDRD) Program
- OSTI Identifier:
- 1506004
- Report Number(s):
- LA-UR-19-20437
Journal ID: ISSN 0002-7863
- Grant/Contract Number:
- 89233218CNA000001; SC0012704; AC52-06NA25396; SC0001059; FOA-0001647-1544; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 140; Journal Issue: 38; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Li, Xiaotong, Hoffman, Justin, Ke, Weijun, Chen, Michelle, Tsai, Hsinhan, Nie, Wanyi, Mohite, Aditya D., Kepenekian, Mikaël, Katan, Claudine, Even, Jacky, Wasielewski, Michael R., Stoumpos, Constantinos C., and Kanatzidis, Mercouri G. Two-Dimensional Halide Perovskites Incorporating Straight Chain Symmetric Diammonium Ions, (NH3CmH2mNH3)(CH3NH3)n-1PbnI3n+1 (m = 4–9; n = 1–4). United States: N. p., 2018.
Web. doi:10.1021/jacs.8b07712.
Li, Xiaotong, Hoffman, Justin, Ke, Weijun, Chen, Michelle, Tsai, Hsinhan, Nie, Wanyi, Mohite, Aditya D., Kepenekian, Mikaël, Katan, Claudine, Even, Jacky, Wasielewski, Michael R., Stoumpos, Constantinos C., & Kanatzidis, Mercouri G. Two-Dimensional Halide Perovskites Incorporating Straight Chain Symmetric Diammonium Ions, (NH3CmH2mNH3)(CH3NH3)n-1PbnI3n+1 (m = 4–9; n = 1–4). United States. https://doi.org/10.1021/jacs.8b07712
Li, Xiaotong, Hoffman, Justin, Ke, Weijun, Chen, Michelle, Tsai, Hsinhan, Nie, Wanyi, Mohite, Aditya D., Kepenekian, Mikaël, Katan, Claudine, Even, Jacky, Wasielewski, Michael R., Stoumpos, Constantinos C., and Kanatzidis, Mercouri G. Fri .
"Two-Dimensional Halide Perovskites Incorporating Straight Chain Symmetric Diammonium Ions, (NH3CmH2mNH3)(CH3NH3)n-1PbnI3n+1 (m = 4–9; n = 1–4)". United States. https://doi.org/10.1021/jacs.8b07712. https://www.osti.gov/servlets/purl/1506004.
@article{osti_1506004,
title = {Two-Dimensional Halide Perovskites Incorporating Straight Chain Symmetric Diammonium Ions, (NH3CmH2mNH3)(CH3NH3)n-1PbnI3n+1 (m = 4–9; n = 1–4)},
author = {Li, Xiaotong and Hoffman, Justin and Ke, Weijun and Chen, Michelle and Tsai, Hsinhan and Nie, Wanyi and Mohite, Aditya D. and Kepenekian, Mikaël and Katan, Claudine and Even, Jacky and Wasielewski, Michael R. and Stoumpos, Constantinos C. and Kanatzidis, Mercouri G.},
abstractNote = {We report that low-dimensional halide perovskites have recently attracted intense interest as alternatives to the three-dimensional (3D) perovskites because of their greater tunability and higher environmental stability. Herein, we present the new homologous 2D series (NH3CmH2mNH3)(CH3NH3)n-1PbnI3n+1 (m = 4–9; n = 1–4), where m represents the carbon-chain number and n equals layer-thickness number. Multilayer (n > 1) 2D perovskites incorporating diammonium cations were successfully synthesized by the solid-state grinding method for m = 4 and 6 and by the solution method for m = 7–9. Structural characterization by single-crystal X-ray diffraction for the m = 8 and m = 9 series (n = 1–4) reveals that these compounds adopt the Cc space group for even n members and Pc for odd n members. The optical bandgaps are 2.15 eV for two-layer (n = 2), 2.01 eV for three-layer (n = 3), and 1.90 eV for four-layer (n = 4). The materials exhibit excellent solution processability, and casting thin-films of the n = 3 members was successfully accomplished. The films show a clear tendency for the higher-m members to have preferred orientation on the glass substrate, with m = 8 exhibiting almost perfect vertical layer orientation and m = 9 displaying both vertical and parallel layer orientation, as confirmed by grazing-incidence wide-angle X-ray scattering (GIWAXS) measurements. Lastly, the vertical layer orientation for the (NH3C8H16NH3)(CH3NH3)2Pb3I10 member results in the best thermal, light, and air stability within this series, thus showing excellent potential for solar cell applications.},
doi = {10.1021/jacs.8b07712},
journal = {Journal of the American Chemical Society},
number = 38,
volume = 140,
place = {United States},
year = {Fri Aug 31 00:00:00 EDT 2018},
month = {Fri Aug 31 00:00:00 EDT 2018}
}
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