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Title: Two-Dimensional Dion–Jacobson Hybrid Lead Iodide Perovskites with Aromatic Diammonium Cations

Abstract

Two-dimensional (2D) halide perovskites have extraordinary optoelectronic properties and structural tunability. Among them, the Dion–Jacobson phases with the inorganic layers stacking exactly on top of each other are less explored. Herein, we present the new series of 2D Dion– Jacobson halide perovskites, which adopt the general formula of A'An–1PbnI3n+1 (A' = 4-(aminomethyl)pyridinium (4AMPY), A = methylammonium (MA), n = 1–4). By modifying the position of the CH2NH3+ group from 4AMPY to 3AMPY (3AMPY = 3-(aminomethyl)pyridinium), the stacking of the inorganic layers changes from exactly eclipsed to slightly offset. Here, the perovskite octahedra tilts are also different between the two series, with the 3AMPY series exhibiting smaller bandgaps than the 4AMPY series. Compared to the aliphatic cation of the same size (AMP = (aminomethyl)- piperidinium), the aromatic spacers increase the rigidity of the cation, reduce the interlayer spacing, and decrease the dielectric mismatch between inorganic layer and the organic spacer, showing the indirect but powerful influence of the organic cations on the structure and consequently on the optical properties of the perovskite materials. All A'An–1PbnI3n+1 compounds exhibit strong photoluminescence (PL) at room temperature. Preliminary solar cell devices based on the n = 4 perovskites as absorbers of both series exhibit promisingmore » performances, with a champion power conversion efficiency (PCE) of 9.20% for (3AMPY)(MA)3Pb4I13-based devices, which is higher than the (4AMPY)(MA)3Pb4I13 and the corresponding aliphatic analogue (3AMP)(MA)3Pb4I13-based ones.« less

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [1]
  1. Northwestern Univ., Evanston, IL (United States)
  2. Univ. Rennes, Rennes (France)
  3. Argonne National Lab. (ANL), Lemont, IL (United States)
  4. Univ. of Crete, Heraklion (Greece)
  5. Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
US Department of the Navy, Office of Naval Research (ONR); USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1559034
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 141; Journal Issue: 32; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; halide perovskites; natural quantum-wells; photoluminescence; dielectric constant; exciton binding energy; solar cell devices

Citation Formats

Li, Xiaotong, Ke, Weijun, Traoré, Boubacar, Guo, Peijun, Hadar, Ido, Kepenekian, Mikaël, Even, Jacky, Katan, Claudine, Stoumpos, Constantinos C., Schaller, Richard D., and Kanatzidis, Mercouri G. Two-Dimensional Dion–Jacobson Hybrid Lead Iodide Perovskites with Aromatic Diammonium Cations. United States: N. p., 2019. Web. doi:10.1021/jacs.9b06398.
Li, Xiaotong, Ke, Weijun, Traoré, Boubacar, Guo, Peijun, Hadar, Ido, Kepenekian, Mikaël, Even, Jacky, Katan, Claudine, Stoumpos, Constantinos C., Schaller, Richard D., & Kanatzidis, Mercouri G. Two-Dimensional Dion–Jacobson Hybrid Lead Iodide Perovskites with Aromatic Diammonium Cations. United States. https://doi.org/10.1021/jacs.9b06398
Li, Xiaotong, Ke, Weijun, Traoré, Boubacar, Guo, Peijun, Hadar, Ido, Kepenekian, Mikaël, Even, Jacky, Katan, Claudine, Stoumpos, Constantinos C., Schaller, Richard D., and Kanatzidis, Mercouri G. Wed . "Two-Dimensional Dion–Jacobson Hybrid Lead Iodide Perovskites with Aromatic Diammonium Cations". United States. https://doi.org/10.1021/jacs.9b06398. https://www.osti.gov/servlets/purl/1559034.
@article{osti_1559034,
title = {Two-Dimensional Dion–Jacobson Hybrid Lead Iodide Perovskites with Aromatic Diammonium Cations},
author = {Li, Xiaotong and Ke, Weijun and Traoré, Boubacar and Guo, Peijun and Hadar, Ido and Kepenekian, Mikaël and Even, Jacky and Katan, Claudine and Stoumpos, Constantinos C. and Schaller, Richard D. and Kanatzidis, Mercouri G.},
abstractNote = {Two-dimensional (2D) halide perovskites have extraordinary optoelectronic properties and structural tunability. Among them, the Dion–Jacobson phases with the inorganic layers stacking exactly on top of each other are less explored. Herein, we present the new series of 2D Dion– Jacobson halide perovskites, which adopt the general formula of A'An–1PbnI3n+1 (A' = 4-(aminomethyl)pyridinium (4AMPY), A = methylammonium (MA), n = 1–4). By modifying the position of the CH2NH3+ group from 4AMPY to 3AMPY (3AMPY = 3-(aminomethyl)pyridinium), the stacking of the inorganic layers changes from exactly eclipsed to slightly offset. Here, the perovskite octahedra tilts are also different between the two series, with the 3AMPY series exhibiting smaller bandgaps than the 4AMPY series. Compared to the aliphatic cation of the same size (AMP = (aminomethyl)- piperidinium), the aromatic spacers increase the rigidity of the cation, reduce the interlayer spacing, and decrease the dielectric mismatch between inorganic layer and the organic spacer, showing the indirect but powerful influence of the organic cations on the structure and consequently on the optical properties of the perovskite materials. All A'An–1PbnI3n+1 compounds exhibit strong photoluminescence (PL) at room temperature. Preliminary solar cell devices based on the n = 4 perovskites as absorbers of both series exhibit promising performances, with a champion power conversion efficiency (PCE) of 9.20% for (3AMPY)(MA)3Pb4I13-based devices, which is higher than the (4AMPY)(MA)3Pb4I13 and the corresponding aliphatic analogue (3AMP)(MA)3Pb4I13-based ones.},
doi = {10.1021/jacs.9b06398},
journal = {Journal of the American Chemical Society},
number = 32,
volume = 141,
place = {United States},
year = {Wed Jul 17 00:00:00 EDT 2019},
month = {Wed Jul 17 00:00:00 EDT 2019}
}

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Cited by: 169 works
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Figures / Tables:

Table 1 Table 1: Crystal and Refinement Data for (xAMPY)(MA)n-1PbnI3n+1 (x = 3 or 4, n = 1−4).

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