globalchange  > 气候变化与战略
DOI: 10.1073/pnas.1811006115
论文题名:
Structural and thermodynamic limits of layer thickness in 2D halide perovskites
作者: Myae Soe C.M.; Nagabhushana G.P.; Shivaramaiah R.; Tsai H.; Nie W.; Blancon J.-C.; Melkonyan F.; Cao D.H.; Traoré B.; Pedesseau L.; Kepenekian M.; Katan C.; Even J.; Marks T.J.; Navrotsky A.; Mohite A.D.; Stoumpos C.C.; Kanatzidis M.G.
刊名: Proceedings of the National Academy of Sciences of the United States of America
ISSN: 0027-8424
出版年: 2019
卷: 116, 期:1
起始页码: 58
结束页码: 66
语种: 英语
英文关键词: Formation enthalpy ; Homologous series ; Layered compounds ; Perovskites ; Photovoltaics ; Ruddlesden–Popper halide
Scopus关键词: halide ; perovskite ; Article ; calorimetry ; crystal structure ; priority journal ; structure activity relation ; structure analysis ; synthesis ; thermodynamics ; thermostability ; thickness ; X ray diffraction
英文摘要: 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 n value 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. © 2019 National Academy of Sciences. All Rights Reserved.
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资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/163579
Appears in Collections:气候变化与战略

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作者单位: Myae Soe, C.M., Argonne–Northwestern Solar Energy Research Center, Northwestern University, Evanston, IL 60208, United States, Peter A. Rock Thermochemistry Laboratory, University of California, Davis, CA 95616, United States; Nagabhushana, G.P., Peter A. Rock Thermochemistry Laboratory, University of California, Davis, CA 95616, United States, Nanomaterials in the Environment, Agriculture, and Technology Organized Research Unit, University of California, Davis, CA 95616, United States; Shivaramaiah, R., Peter A. Rock Thermochemistry Laboratory, University of California, Davis, CA 95616, United States, Nanomaterials in the Environment, Agriculture, and Technology Organized Research Unit, University of California, Davis, CA 95616, United States; Tsai, H., Material Synthesis and Integrated Devices, MPA-11, Los Alamos National Laboratory, Los Alamos, NM 87545, United States; Nie, W., Material Synthesis and Integrated Devices, MPA-11, Los Alamos National Laboratory, Los Alamos, NM 87545, United States; Blancon, J.-C., Material Synthesis and Integrated Devices, MPA-11, Los Alamos National Laboratory, Los Alamos, NM 87545, United States; Melkonyan, F., Department of Chemistry, Northwestern University, Evanston, IL 60208, United States, Argonne–Northwestern Solar Energy Research Center, Northwestern University, Evanston, IL 60208, United States; Cao, D.H., Department of Chemistry, Northwestern University, Evanston, IL 60208, United States, Argonne–Northwestern Solar Energy Research Center, Northwestern University, Evanston, IL 60208, United States; Traoré, B., Univ Rennes, ENSCR, INSA Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes), UMR 6226, Rennes, F-35000, France; Pedesseau, L., Univ Rennes, INSA Rennes, CNRS, Institut FOTON – UMR 6082, Rennes, F-35000, France; Kepenekian, M., Univ Rennes, ENSCR, INSA Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes), UMR 6226, Rennes, F-35000, France; Katan, C., Univ Rennes, ENSCR, INSA Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes), UMR 6226, Rennes, F-35000, France; Even, J., Univ Rennes, INSA Rennes, CNRS, Institut FOTON – UMR 6082, Rennes, F-35000, France; Marks, T.J., Department of Chemistry, Northwestern University, Evanston, IL 60208, United States, Argonne–Northwestern Solar Energy Research Center, Northwestern University, Evanston, IL 60208, United States; Navrotsky, A., Peter A. Rock Thermochemistry Laboratory, University of California, Davis, CA 95616, United States, Nanomaterials in the Environment, Agriculture, and Technology Organized Research Unit, University of California, Davis, CA 95616, United States; Mohite, A.D., Material Synthesis and Integrated Devices, MPA-11, Los Alamos National Laboratory, Los Alamos, NM 87545, United States, Department of Chemical and Biomolecular Engineering, Rice University, Houston, TX 77005, United States; Stoumpos, C.C., Department of Chemistry, Northwestern University, Evanston, IL 60208, United States, Argonne–Northwestern Solar Energy Research Center, Northwestern University, Evanston, IL 60208, United States, Department of Materials Science and Technology, University of Crete, Heraklion, GR-70013, Greece; Kanatzidis, M.G., Department of Chemistry, Northwestern University, Evanston, IL 60208, United States, Argonne–Northwestern Solar Energy Research Center, Northwestern University, Evanston, IL 60208, United States

Recommended Citation:
Myae Soe C.M.,Nagabhushana G.P.,Shivaramaiah R.,et al. Structural and thermodynamic limits of layer thickness in 2D halide perovskites[J]. Proceedings of the National Academy of Sciences of the United States of America,2019-01-01,116(1)
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