Chemical Behavior and Local Structure of the Ruddlesden–Popper and Dion–Jacobson Alloyed Pb/Sn Bromide 2D Perovskites

化学 卤化物 溴化物 带隙 结晶学 化学计量学 密度泛函理论 相(物质) 无机化学 物理化学 材料科学 计算化学 光电子学 有机化学
作者
Ping Fu,Michael A. Quintero,Eugenia S. Vasileiadou,Parth Raval,Claire Welton,Mikaël Képénékian,George Volonakis,Jacky Even,Yukun Liu,Christos D. Malliakas,Yi Yang,Craig C. Laing,Vinayak P. Dravid,G. N. Manjunatha Reddy,Can Li,Edward H. Sargent,Mercouri G. Kanatzidis
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:145 (29): 15997-16014 被引量:13
标识
DOI:10.1021/jacs.3c03997
摘要

The alloyed lead/tin (Pb/Sn) halide perovskites have gained significant attention in the development of tandem solar cells and other optoelectronic devices due to their widely tunable absorption edge. To gain a better understanding of the intriguing properties of Pb/Sn perovskites, such as their anomalous bandgap's dependence on stoichiometry, it is important to deepen the understanding of their chemical behavior and local structure. Herein, we investigate a series of two-dimensional Ruddlesden-Popper (RP) and Dion-Jacobson (DJ) phase alloyed Pb/Sn bromide perovskites using butylammonium (BA) and 3-(aminomethyl)pyridinium (3AMPY) as the spacer cations: (BA)2(MA)n-1PbxSnn-xBr3n+1 (n = 1-3) and (3AMPY)(MA)n-1PbxSnn-xBr3n+1 (n = 1-3) through a solution-based approach. Our results show that the ratio and site preference of Pb/Sn atoms are influenced by the layer thickness (n) and spacer cations (A'), as determined by single-crystal X-ray diffraction. Solid-state 1H, 119Sn, and 207Pb NMR spectroscopy analysis shows that the Pb atoms prefer the outer layers in n = 3 members: (BA)2(MA)PbxSnn-xBr10 and (3AMPY)(MA)PbxSnn-xBr10. Layered 2D DJ alloyed Pb/Sn bromide perovskites (3AMPY)(MA)n-1PbxSnn-xBr3n+1 (n = 1-3) demonstrate much narrower optical band gaps, lower energy PL emission peaks, and longer carrier lifetimes compared to those of RP analogs. Density functional theory calculations suggest that Pb-rich alloys (Pb:Sn ∼4:1) for n = 1 compounds are thermodynamically favored over 50:50 (Pb:Sn ∼1:1) compositions. From grazing-incidence wide-angle X-ray scattering (GIWAXS), we see that films in the RP phase orient parallel to the substrate, whereas for DJ cases, random orientations are observed relative to the substrate.
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