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DOI	10.1073/pnas.1811006115
	Structural and thermodynamic limits of layer thickness in 2D halide perovskites
	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.
发表日期	2019
ISSN	0027-8424
起始页码	58
结束页码	66
卷号	116 期号:1
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.
英文关键词	Formation enthalpy; Homologous series; Layered compounds; Perovskites; Photovoltaics; Ruddlesden–Popper halide
语种	英语
scopus关键词	halide; perovskite; Article; calorimetry; crystal structure; priority journal; structure activity relation; structure analysis; synthesis; thermodynamics; thermostability; thickness; X ray diffraction
来源期刊	Proceedings of the National Academy of Sciences of the United States of America
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/160388
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...
推荐引用方式 GB/T 7714	Myae Soe C.M.,Nagabhushana G.P.,Shivaramaiah R.,et al. Structural and thermodynamic limits of layer thickness in 2D halide perovskites[J],2019,116(1).
APA	Myae Soe C.M..,Nagabhushana G.P..,Shivaramaiah R..,Tsai H..,Nie W..,...&Kanatzidis M.G..(2019).Structural and thermodynamic limits of layer thickness in 2D halide perovskites.Proceedings of the National Academy of Sciences of the United States of America,116(1).
MLA	Myae Soe C.M.,et al."Structural and thermodynamic limits of layer thickness in 2D halide perovskites".Proceedings of the National Academy of Sciences of the United States of America 116.1(2019).