New Type of 2D Perovskites with Alternating Cations in the Interlayer Space, (C(NH2)3)(CH3NH3)nPbnI3n+1: Structure, Properties, and Photovoltaic Performance
Abstract
In this study, 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 studiedmore »
- Authors:
-
- Northwestern Univ., Evanston, IL (United States)
- Université de Rennes (France)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Univ. of California, Santa Barbara, CA (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Light Energy Activated Redox Processes (LEAP); Univ. of California, Santa Barbara, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF)
- OSTI Identifier:
- 1599738
- Grant/Contract Number:
- SC0012541; SC0001059; AC52-06NA25396; AC02-06CH11357; ECCS-1542205; DMR-1121262
- Resource Type:
- Accepted Manuscript
- 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:
- 14 SOLAR ENERGY; 36 MATERIALS SCIENCE; 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(NH2)3)(CH3NH3)nPbnI3n+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(NH2)3)(CH3NH3)nPbnI3n+1: Structure, Properties, and Photovoltaic Performance. United States. https://doi.org/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. Thu .
"New Type of 2D Perovskites with Alternating Cations in the Interlayer Space, (C(NH2)3)(CH3NH3)nPbnI3n+1: Structure, Properties, and Photovoltaic Performance". United States. https://doi.org/10.1021/jacs.7b09096. https://www.osti.gov/servlets/purl/1599738.
@article{osti_1599738,
title = {New Type of 2D Perovskites with Alternating Cations in the Interlayer Space, (C(NH2)3)(CH3NH3)nPbnI3n+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 = {In this study, 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},
number = 45,
volume = 139,
place = {United States},
year = {Thu Nov 02 00:00:00 EDT 2017},
month = {Thu Nov 02 00:00:00 EDT 2017}
}
Web of Science
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Unveiling the Importance of Precursor Preparation for Highly Efficient and Stable Phenethylammonium‐Based Perovskite Solar Cells
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Design principles for electronic charge transport in solution-processed vertically stacked 2D perovskite quantum wells
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Dimensional tailoring of hybrid perovskites for photovoltaics
journal, November 2018
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A simple method for phase control in two-dimensional perovskite solar cells
journal, January 2018
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- Journal of Materials Chemistry A, Vol. 6, Issue 39
Emission enhancement and bandgap retention of a two-dimensional mixed cation lead halide perovskite under high pressure
journal, January 2019
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Low-dimensional emissive states in non-stoichiometric methylammonium lead halide perovskites
journal, January 2019
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Factors determining the vertical orientation of two-dimensional perovskites
journal, January 2019
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Hydrophobic perovskites based on an alkylamine compound for high efficiency solar cells with improved environmental stability
journal, January 2019
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Guanidinium induced phase separated perovskite layer for efficient and highly stable solar cells
journal, January 2019
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Octahedral connectivity and its role in determining the phase stabilities and electronic structures of low-dimensional, perovskite-related iodoplumbates
journal, November 2018
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Structural and thermodynamic limits of layer thickness in 2D halide perovskites
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- Proceedings of the National Academy of Sciences, Vol. 116, Issue 1
DFT study of electronic structure and optical properties of layered two-dimensional CH 3 NH 3 PbX 3 (X=Cl, Br, I)
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Efficient and accurate calculation of band gaps of halide perovskites with the Tran-Blaha modified Becke-Johnson potential
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First representatives of (210)-oriented perovskite variants−Synthesis, crystal structures and properties of the new 2D hybrid perovskites A[HC(NH2)2]PbI4; A=[C(NH2)3], [HSC(NH2)2]
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Low‐Dimensional Dion–Jacobson‐Phase Lead‐Free Perovskites for High‐Performance Photovoltaics with Improved Stability
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Unveiling the Importance of Precursor Preparation for Highly Efficient and Stable Phenethylammonium‐Based Perovskite Solar Cells
journal, April 2020
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Octahedral connectivity and its role in determining the phase stabilities and electronic structures of low-dimensional, perovskite-related iodoplumbates
text, January 2018
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Hybrid Halide Perovskites: Discussions on Terminology and Materials
journal, October 2019
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Highly Emissive Self-Trapped Excitons in Fully Inorganic Zero-Dimensional Tin Halides
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Band-edge Exciton Fine Structure and Exciton Recombination Dynamics in Single crystals of Layered Hybrid Perovskites
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Highly Emissive Self-Trapped Excitons in Fully Inorganic Zero-Dimensional Tin Halides
journal, July 2018
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Incorporating Large A Cations into Lead Iodide Perovskite Cages: Relaxed Goldschmidt Tolerance Factor and Impact on Exciton–Phonon Interaction
journal, July 2019
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Guanidinium-Formamidinium Lead Iodide: A Layered Perovskite-Related Compound with Red Luminescence at Room Temperature
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Two-Dimensional Dion–Jacobson Hybrid Lead Iodide Perovskites with Aromatic Diammonium Cations
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Design principles for electronic charge transport in solution-processed vertically stacked 2D perovskite quantum wells
journal, May 2018
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Structural and thermodynamic limits of layer thickness in 2D halide perovskites
journal, December 2018
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Phase-Transition-Induced Carrier Mass Enhancement in 2D Ruddlesden-Popper Perovskites
text, January 2019
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