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Title: Hybrid Dion–Jacobson 2D Lead Iodide Perovskites

Abstract

The three-dimensional hybrid organic–inorganic perovskites have shown huge potential for use in solar cells and other optoelectronic devices. Although these materials are under intense investigation, derivative materials with lower dimensionality are emerging, offering higher tunability of physical properties and new capabilities. Here, we present two new series of hybrid two-dimensional (2D) perovskites that adopt the Dion–Jacobson (DJ) structure type, which are the first complete homologous series reported in halide perovskite chemistry. Lead iodide DJ perovskites adopt a general formula A'A n–1PbnI 3n +1 (A' = 3-(aminomethyl)piperidinium (3AMP) or 4-(aminomethyl)piperidinium (4AMP), A = methylammonium (MA)). These materials have layered structures where the stacking of inorganic layers is unique as they lay exactly on top of another. With a slightly different position of the functional group in the templating cation 3AMP and 4AMP, the as-formed DJ perovskites show different optical properties, with the 3AMP series having smaller band gaps than the 4AMP series. Analysis on the crystal structures and density functional theory (DFT) calculations suggest that the origin of the systematic band gap shift is the strong but indirect influence of the organic cation on the inorganic framework. Fabrication of photovoltaic devices utilizing these materials as light absorbers reveals that (3AMP)(MA) 3Pbmore » 4I 13 has the best power conversion efficiency (PCE) of 7.32%, which is much higher than that of the corresponding (4AMP)(MA) 3Pb 4I 13.« less

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [3]
  1. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
  2. Univ. Rennes, Rennes (France); National Centre for Scientific Research (CNRS), Rennes (France)
  3. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry, and Argonne-Northwestern Solar Energy Research (ANSER) Center
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Argonne-Northwestern Solar Energy Research Center (ANSER)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1470389
Grant/Contract Number:  
SC0001059
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 140; Journal Issue: 10; Related Information: ANSER partners with Northwestern University (lead); Argonne National Laboratory; University of Chicago; University of Illinois, Urbana-Champaign; Yale University; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysis (homogeneous); catalysis (heterogeneous); solar (photovoltaic); solar (fuels); photosynthesis (natural and artificial); bio-inspired; hydrogen and fuel cells; electrodes - solar; defects; charge transport; spin dynamics; membrane; materials and chemistry by design; optics; synthesis (novel materials)

Citation Formats

Mao, Lingling, Ke, Weijun, Pedesseau, Laurent, Wu, Yilei, Katan, Claudine, Even, Jacky, Wasielewski, Michael R., Stoumpos, Constantinos C., and Kanatzidis, Mercouri G. Hybrid Dion–Jacobson 2D Lead Iodide Perovskites. United States: N. p., 2018. Web. doi:10.1021/jacs.8b00542.
Mao, Lingling, Ke, Weijun, Pedesseau, Laurent, Wu, Yilei, Katan, Claudine, Even, Jacky, Wasielewski, Michael R., Stoumpos, Constantinos C., & Kanatzidis, Mercouri G. Hybrid Dion–Jacobson 2D Lead Iodide Perovskites. United States. doi:10.1021/jacs.8b00542.
Mao, Lingling, Ke, Weijun, Pedesseau, Laurent, Wu, Yilei, Katan, Claudine, Even, Jacky, Wasielewski, Michael R., Stoumpos, Constantinos C., and Kanatzidis, Mercouri G. Wed . "Hybrid Dion–Jacobson 2D Lead Iodide Perovskites". United States. doi:10.1021/jacs.8b00542. https://www.osti.gov/servlets/purl/1470389.
@article{osti_1470389,
title = {Hybrid Dion–Jacobson 2D Lead Iodide Perovskites},
author = {Mao, Lingling and Ke, Weijun and Pedesseau, Laurent and Wu, Yilei and Katan, Claudine and Even, Jacky and Wasielewski, Michael R. and Stoumpos, Constantinos C. and Kanatzidis, Mercouri G.},
abstractNote = {The three-dimensional hybrid organic–inorganic perovskites have shown huge potential for use in solar cells and other optoelectronic devices. Although these materials are under intense investigation, derivative materials with lower dimensionality are emerging, offering higher tunability of physical properties and new capabilities. Here, we present two new series of hybrid two-dimensional (2D) perovskites that adopt the Dion–Jacobson (DJ) structure type, which are the first complete homologous series reported in halide perovskite chemistry. Lead iodide DJ perovskites adopt a general formula A'An–1PbnI3n+1 (A' = 3-(aminomethyl)piperidinium (3AMP) or 4-(aminomethyl)piperidinium (4AMP), A = methylammonium (MA)). These materials have layered structures where the stacking of inorganic layers is unique as they lay exactly on top of another. With a slightly different position of the functional group in the templating cation 3AMP and 4AMP, the as-formed DJ perovskites show different optical properties, with the 3AMP series having smaller band gaps than the 4AMP series. Analysis on the crystal structures and density functional theory (DFT) calculations suggest that the origin of the systematic band gap shift is the strong but indirect influence of the organic cation on the inorganic framework. Fabrication of photovoltaic devices utilizing these materials as light absorbers reveals that (3AMP)(MA)3Pb4I13 has the best power conversion efficiency (PCE) of 7.32%, which is much higher than that of the corresponding (4AMP)(MA)3Pb4I13.},
doi = {10.1021/jacs.8b00542},
journal = {Journal of the American Chemical Society},
number = 10,
volume = 140,
place = {United States},
year = {2018},
month = {2}
}

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