Structural and thermodynamic limits of layer thickness in 2D halide perovskites
Abstract
In the fast-evolving field of halide perovskite semiconductors, the 2D perovskites (A') 2(A) n-1M nX 3n+1[where A = Cs +, CH 3NH 3 +, HC(NH 2) 2 +; A' = ammonium cation acting as spacer; M = Ge 2+, Sn 2+, Pb 2+; and X = Cl -, Br -, I -] have recently made a critical entry. The n value defines the thickness of the 2D layers, which controls the optical and electronic properties. The 2D perovskites have demonstrated preliminary optoelectronic device lifetime superior to their 3D counterparts. They have also attracted fundamental interest as solution-processed quantum wells with structural and physical properties tunable via chemical composition, notably by the nvalue defining the perovskite layer thickness. The higher members ( n > 5) have not been documented, and there are important scientific questions underlying fundamental limits for n. To develop and utilize these materials in technology, it is imperative to understand their thermodynamic stability, fundamental synthetic limitations, and the derived structure–function relationships. We report the effective synthesis of the highest iodide n-members yet, namely (CH 3(CH 2) 2NH 3) 2(CH 3NH 3) 5Pb 6I 19( n= 6) and (CH 3(CH 2) 2NH 3) 2(CH 3NH 3) 6Pb 7I 22(more »
- Authors:
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Sponsoring Org.:
- U.S. OFFICE OF NAVAL RESEARCH
- OSTI Identifier:
- 1576006
- Resource Type:
- Journal Article
- Journal Name:
- Proceedings of the National Academy of Sciences of the United States of America
- Additional Journal Information:
- Journal Volume: 116; Journal Issue: 1; Journal ID: ISSN 0027-8424
- Publisher:
- National Academy of Sciences
- Country of Publication:
- United States
- Language:
- ENGLISH
Citation Formats
Soe, Chan Myae Myae, Nagabhushana, G. P., Shivaramaiah, Radha, Tsai, Hsinhan, Nie, Wanyi, Blancon, Jean-Christophe, Melkonyan, Ferdinand, Cao, Duyen H., Traoré, Boubacar, Pedesseau, Laurent, Kepenekian, Mikaël, Katan, Claudine, Even, Jacky, Marks, Tobin J., Navrotsky, Alexandra, Mohite, Aditya D., Stoumpos, Constantinos C., and Kanatzidis, Mercouri G. Structural and thermodynamic limits of layer thickness in 2D halide perovskites. United States: N. p., 2018.
Web. doi:10.1073/pnas.1811006115.
Soe, Chan Myae Myae, Nagabhushana, G. P., Shivaramaiah, Radha, Tsai, Hsinhan, Nie, Wanyi, Blancon, Jean-Christophe, Melkonyan, Ferdinand, Cao, Duyen H., Traoré, Boubacar, Pedesseau, Laurent, Kepenekian, Mikaël, Katan, Claudine, Even, Jacky, Marks, Tobin J., Navrotsky, Alexandra, Mohite, Aditya D., Stoumpos, Constantinos C., & Kanatzidis, Mercouri G. Structural and thermodynamic limits of layer thickness in 2D halide perovskites. United States. https://doi.org/10.1073/pnas.1811006115
Soe, Chan Myae Myae, Nagabhushana, G. P., Shivaramaiah, Radha, Tsai, Hsinhan, Nie, Wanyi, Blancon, Jean-Christophe, Melkonyan, Ferdinand, Cao, Duyen H., Traoré, Boubacar, Pedesseau, Laurent, Kepenekian, Mikaël, Katan, Claudine, Even, Jacky, Marks, Tobin J., Navrotsky, Alexandra, Mohite, Aditya D., Stoumpos, Constantinos C., and Kanatzidis, Mercouri G. Tue .
"Structural and thermodynamic limits of layer thickness in 2D halide perovskites". United States. https://doi.org/10.1073/pnas.1811006115.
@article{osti_1576006,
title = {Structural and thermodynamic limits of layer thickness in 2D halide perovskites},
author = {Soe, Chan Myae Myae and Nagabhushana, G. P. and Shivaramaiah, Radha and Tsai, Hsinhan and Nie, Wanyi and Blancon, Jean-Christophe and Melkonyan, Ferdinand and Cao, Duyen H. and Traoré, Boubacar and Pedesseau, Laurent and Kepenekian, Mikaël and Katan, Claudine and Even, Jacky and Marks, Tobin J. and Navrotsky, Alexandra and Mohite, Aditya D. and Stoumpos, Constantinos C. and Kanatzidis, Mercouri G.},
abstractNote = {In the fast-evolving field of halide perovskite semiconductors, the 2D perovskites (A')2(A)n-1MnX3n+1[where A = Cs+, CH3NH3+, HC(NH2)2+; A' = ammonium cation acting as spacer; M = Ge2+, Sn2+, Pb2+; and X = Cl-, Br-, I-] have recently made a critical entry. The n value defines the thickness of the 2D layers, which controls the optical and electronic properties. The 2D perovskites have demonstrated preliminary optoelectronic device lifetime superior to their 3D counterparts. They have also attracted fundamental interest as solution-processed quantum wells with structural and physical properties tunable via chemical composition, notably by the nvalue defining the perovskite layer thickness. The higher members (n > 5) have not been documented, and there are important scientific questions underlying fundamental limits for n. To develop and utilize these materials in technology, it is imperative to understand their thermodynamic stability, fundamental synthetic limitations, and the derived structure–function relationships. We report the effective synthesis of the highest iodide n-members yet, namely (CH3(CH2)2NH3)2(CH3NH3)5Pb6I19(n= 6) and (CH3(CH2)2NH3)2(CH3NH3)6Pb7I22(n = 7), and confirm the crystal structure with single-crystal X-ray diffraction, and provide indirect evidence for “(CH3(CH2)2NH3)2(CH3NH3)8Pb9I28” (“n = 9”). Direct HCl solution calorimetric measurements show the compounds with n > 7 have unfavorable enthalpies of formation (ΔHf), suggesting the formation of higher homologs to be challenging. Finally, we report preliminary n-dependent solar cell efficiency in the range of 9–12.6% in these higher n-members, highlighting the strong promise of these materials for high-performance devices.},
doi = {10.1073/pnas.1811006115},
url = {https://www.osti.gov/biblio/1576006},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
issn = {0027-8424},
number = 1,
volume = 116,
place = {United States},
year = {2018},
month = {12}
}
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2D Homologous Perovskites as Light-Absorbing Materials for Solar Cell Applications
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Nanocrystals of Cesium Lead Halide Perovskites (CsPbX 3 , X = Cl, Br, and I): Novel Optoelectronic Materials Showing Bright Emission with Wide Color Gamut
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journal, January 2001
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Role of Organic Counterion in Lead- and Tin-Based Two-Dimensional Semiconducting Iodide Perovskites and Application in Planar Solar Cells
journal, October 2016
- Mao, Lingling; Tsai, Hsinhan; Nie, Wanyi
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Advances and Promises of Layered Halide Hybrid Perovskite Semiconductors
journal, October 2016
- Pedesseau, Laurent; Sapori, Daniel; Traore, Boubacar
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Exploiting dimensionality and defect mitigation to create tunable microwave dielectrics
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- Lee, Che-Hui; Orloff, Nathan D.; Birol, Turan
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Understanding Quantum Confinement of Charge Carriers in Layered 2D Hybrid Perovskites
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Exciton state in two-dimensional perovskite semiconductor (C10H21NH3)2PbI4
journal, March 1989
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High Members of the 2D Ruddlesden-Popper Halide Perovskites: Synthesis, Optical Properties, and Solar Cells of (CH 3 (CH 2 ) 3 NH 3 ) 2 (CH 3 NH 3 ) 4 Pb 5 I 16
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Effect of reduced dimensionality on the optical band gap of SrTiO 3
journal, March 2013
- Lee, Che-Hui; Podraza, Nikolas J.; Zhu, Ye
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High-efficiency solution-processed perovskite solar cells with millimeter-scale grains
journal, January 2015
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