TY - JOUR
T1 - Hybrid Dion-Jacobson 2D Lead Iodide Perovskites
AU - Mao, Lingling
AU - Ke, Weijun
AU - Pedesseau, Laurent
AU - Wu, Yilei
AU - Katan, Claudine
AU - Even, Jacky
AU - Wasielewski, Michael R.
AU - Stoumpos, Constantinos C.
AU - Kanatzidis, Mercouri G.
N1 - Funding Information:
This work was supported by the Department of Energy, Office of Science, Basic Energy Sciences, under Grant SC0012541 (synthesis and structural characterization of materials, M.G.K.). The device assembly and PL lifetime measurements were supported by the ANSER Center, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences under award DESC0001059 (W.K., M.R.W.). The work at FOTON was performed using HPC resources from GENCI-TGCC/ CINES (Grant 2017-0906724). Y.W. thanks the Fulbright Scholars Program for a Graduate Research Fellowship and gratefully acknowledges support of a Ryan Fellowship from the NU International Institute for Nanotechnology (IIN). This work made use of the IMSERC at Northwestern University, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205), the State of Illinois, and the International Institute for Nanotechnology (IIN). This work made use of the EPIC, Keck-II, and SPID facilities of Northwestern University’s NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205); the MRSEC program (NSF DMR-1121262) at the Materials Research Center; the International Institute for Nanotechnology (IIN); the Keck Foundation; and the State of Illinois, through the IIN.
Publisher Copyright:
© 2018 American Chemical Society.
PY - 2018/3/14
Y1 - 2018/3/14
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85043780833&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85043780833&partnerID=8YFLogxK
U2 - 10.1021/jacs.8b00542
DO - 10.1021/jacs.8b00542
M3 - Article
C2 - 29465246
AN - SCOPUS:85043780833
VL - 140
SP - 3775
EP - 3783
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
SN - 0002-7863
IS - 10
ER -