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Title: New Type of 2D Perovskites with Alternating Cations in the Interlayer Space, (C(NH 2 ) 3 )(CH 3 NH 3 ) n Pb n I 3n+1 : Structure, Properties, and Photovoltaic Performance

Abstract

We present the new homologous series (C(NH2)3)(CH3NH3)nPbnI3n+1 (n = 1, 2, 3) of layered 2D perovskites. Structural characterization by single-crystal X-ray diffraction reveals that these compounds adopt an unprecedented structure type, which is stabilized by the alternating ordering of the guanidinium and methylammonium cations in the interlayer space (ACI). Compared to the more common Ruddlesden–Popper (RP) 2D perovskites, the ACI perovskites have a different stacking motif and adopt a higher crystal symmetry. The higher symmetry of the ACI perovskites is expressed in their physical properties, which show a characteristic decrease of the bandgap with respect to their RP perovskite counterparts with the same perovskite layer thickness (n). The compounds show a monotonic decrease in the optical gap as n increases: Eg = 2.27 eV for n = 1 to Eg = 1.99 eV for n = 2 and Eg = 1.73 eV for n = 3, which show slightly narrower gaps compared to the corresponding RP perovskites. First-principles theoretical electronic structure calculations confirm the experimental optical gap trends suggesting that the ACI perovskites are direct bandgap semiconductors with wide valence and conduction bandwidths. To assess the potential of the ACI perovskites toward solar cell applications, we studied the (C(NH2)3)(CH3NH3)3Pb3I10 (nmore » = 3) compound. Compact thin films from the (C(NH2)3)(CH3NH3)3Pb3I10 compound with excellent surface coverage can be obtained from the antisolvent dripping method. Planar photovoltaic devices from optimized ACI perovskite films yield a power-conversion-efficiency of 7.26% with a high open-circuit voltage of ~1 V and a striking fill factor of ~80%.« less

Authors:
 [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2];  [3];  [3];  [1]; ORCiD logo [2]; ORCiD logo; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [1]; ORCiD logo [1]
  1. Department of Chemistry and Argonne-Northwestern Solar Energy Research Center, Northwestern University, Evanston, Illinois 60208, United States
  2. Institut des Sciences Chimiques de Rennes (ISCR), UMR 6226, CNRS, Ecole Nationale Supérieure de Chimie de Rennes, INSA, Université de Rennes 1 Rennes 35708, France
  3. Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States
  4. Fonctions Optiques pour les Technologies de l’Information (FOTON), UMR 6082, CNRS, INSA Rennes, Université de Rennes 1, Rennes 35708, France
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Energy Frontier Research Centers (EFRC) (United States). Argonne-Northwestern Solar Energy Research Center (ANSER)
Sponsoring Org.:
FOREIGN
OSTI Identifier:
1410126
Resource Type:
Journal Article
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 45; 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

Citation Formats

Soe, Chan Myae Myae, Stoumpos, Constantinos C., Kepenekian, Mikaël, Traoré, Boubacar, Tsai, Hsinhan, Nie, Wanyi, Wang, Binghao, Katan, Claudine, Seshadri, Ram, Mohite, Aditya D., Even, Jacky, Marks, Tobin J., and Kanatzidis, Mercouri G.. New Type of 2D Perovskites with Alternating Cations in the Interlayer Space, (C(NH 2 ) 3 )(CH 3 NH 3 ) n Pb n I 3n+1 : Structure, Properties, and Photovoltaic Performance. United States: N. p., 2017. Web. doi:10.1021/jacs.7b09096.
Soe, Chan Myae Myae, Stoumpos, Constantinos C., Kepenekian, Mikaël, Traoré, Boubacar, Tsai, Hsinhan, Nie, Wanyi, Wang, Binghao, Katan, Claudine, Seshadri, Ram, Mohite, Aditya D., Even, Jacky, Marks, Tobin J., & Kanatzidis, Mercouri G.. New Type of 2D Perovskites with Alternating Cations in the Interlayer Space, (C(NH 2 ) 3 )(CH 3 NH 3 ) n Pb n I 3n+1 : Structure, Properties, and Photovoltaic Performance. United States. doi:10.1021/jacs.7b09096.
Soe, Chan Myae Myae, Stoumpos, Constantinos C., Kepenekian, Mikaël, Traoré, Boubacar, Tsai, Hsinhan, Nie, Wanyi, Wang, Binghao, Katan, Claudine, Seshadri, Ram, Mohite, Aditya D., Even, Jacky, Marks, Tobin J., and Kanatzidis, Mercouri G.. Wed . "New Type of 2D Perovskites with Alternating Cations in the Interlayer Space, (C(NH 2 ) 3 )(CH 3 NH 3 ) n Pb n I 3n+1 : Structure, Properties, and Photovoltaic Performance". United States. doi:10.1021/jacs.7b09096.
@article{osti_1410126,
title = {New Type of 2D Perovskites with Alternating Cations in the Interlayer Space, (C(NH 2 ) 3 )(CH 3 NH 3 ) n Pb n I 3n+1 : Structure, Properties, and Photovoltaic Performance},
author = {Soe, Chan Myae Myae and Stoumpos, Constantinos C. and Kepenekian, Mikaël and Traoré, Boubacar and Tsai, Hsinhan and Nie, Wanyi and Wang, Binghao and Katan, Claudine and Seshadri, Ram and Mohite, Aditya D. and Even, Jacky and Marks, Tobin J. and Kanatzidis, Mercouri G.},
abstractNote = {We present the new homologous series (C(NH2)3)(CH3NH3)nPbnI3n+1 (n = 1, 2, 3) of layered 2D perovskites. Structural characterization by single-crystal X-ray diffraction reveals that these compounds adopt an unprecedented structure type, which is stabilized by the alternating ordering of the guanidinium and methylammonium cations in the interlayer space (ACI). Compared to the more common Ruddlesden–Popper (RP) 2D perovskites, the ACI perovskites have a different stacking motif and adopt a higher crystal symmetry. The higher symmetry of the ACI perovskites is expressed in their physical properties, which show a characteristic decrease of the bandgap with respect to their RP perovskite counterparts with the same perovskite layer thickness (n). The compounds show a monotonic decrease in the optical gap as n increases: Eg = 2.27 eV for n = 1 to Eg = 1.99 eV for n = 2 and Eg = 1.73 eV for n = 3, which show slightly narrower gaps compared to the corresponding RP perovskites. First-principles theoretical electronic structure calculations confirm the experimental optical gap trends suggesting that the ACI perovskites are direct bandgap semiconductors with wide valence and conduction bandwidths. To assess the potential of the ACI perovskites toward solar cell applications, we studied the (C(NH2)3)(CH3NH3)3Pb3I10 (n = 3) compound. Compact thin films from the (C(NH2)3)(CH3NH3)3Pb3I10 compound with excellent surface coverage can be obtained from the antisolvent dripping method. Planar photovoltaic devices from optimized ACI perovskite films yield a power-conversion-efficiency of 7.26% with a high open-circuit voltage of ~1 V and a striking fill factor of ~80%.},
doi = {10.1021/jacs.7b09096},
journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 45,
volume = 139,
place = {United States},
year = {2017},
month = {11}
}